text:
It's Called "Leadership"
The more their campaigns go on, the more the clear differences between Mr. Obama and Mrs. Clinton appear. They are not so much policy differences as they are personal differences. And, in a word, I believe those differences can all be chalked up to the "L" word"…."Leadership". In exit poll after exit poll, an overwhelming majority of Democratic voters have said they would be "comfortable" with EITHER Mr. Orbama OR Mrs. Clinton as President. So what attributes of Mr. Obama's character are now fueling his growing popularity, and what attributes are now sinking Mrs. Clinton's?
The more their campaigns go on, the more the clear differences between Mr. Obama and Mrs. Clinton appear. They are not so much policy differences as they are personal differences. And, in a word, I believe those differences can all be chalked up to the "L" word"…."Leadership".
In exit poll after exit poll, an overwhelming majority of Democratic voters have said they would be "comfortable" with EITHER Mr. Orbama OR Mrs. Clinton as President. So what attributes of Mr. Obama's character are now fueling his growing popularity, and what attributes are now sinking Mrs. Clinton's?
I believe the principle answer to that question lies in their fundamentally differing leadership skills and abilities.
Leadership is that mix of sometimes innate, sometimes learned abilities that inspire others to action. Wikipedia defines leadership as simply, "The ability to affect human behavior so as to accomplish a mission designated by the leader." About.com calls it the, "Art of motivating a group of people to act towards achieving a common goal". It's a mix of wisdom gained from experience, charisma, psychology and an (often innate) ability to clearly articulate what the goals are and then help make people think it was their idea to work together in achieving them.
In many ways, and as at least one definition of it shown above attests, it's an art form, not a science.
Clearly, Mr. Obama has it (or more of it) than Mrs. Clinton. This is probably why he is regularly packing upwards of 20,000 people into large sports arenas to hear him speak and why she (and Mr. McCain) are speaking to audiences of a simply a few hundred or a thousand or so. For example, while he was in Ohio last week to deliver his "victory speech" after his win in the Wisconsin primaries, Mr. McCain had an audience of maybe a hundred people in the room (the exact number was probably a lot less) who had even bothered to turn up to listen to him. That fact, alone, speaks volumes.
People now accuse Mr. Obama of taking on almost a "rock-star-like" quality. To the contrary, I believe what they are now seeing are simply his many leadership qualities at work…his innate (or learned) ability to inspire an audience to a higher calling with his words and his actions.
That is, while Mrs. Clinton doggedly insists on yammering on and on about the "specifics" of her "10 point plan" for this or that social ill, he is choosing to inspire the country to a higher calling by saying in essence, "Follow me and we'll take our country in a new direction and the specifics will take care of themselves."
These, my friends, are ALSO outward signs of Mr. Obama's keen leadership qualities at work.
What's more, during last week's debate in Texas, Senator Obama said, "Senator Clinton of late has said: Let's get real. The implication is that the people who've been voting for me or involved in my campaign are somehow delusional…" said Obama. "You know, the thinking is that somehow, they're being duped, and eventually they're going to see the reality of things. Well, I think they perceive reality of what's going on in Washington very clearly. What they see is that if we don't bring the country together, stop the endless bickering, actually focus on solutions and reduce the special interests that have dominated Washington, then we will not get anything done. And the… reason that this campaign has done so well is because people understand that it is not just a matter of putting forward policy positions. Senator Clinton and I share a lot of policy positions. But if we can't inspire the American people to get involved in their government and if we can't inspire them to go beyond the racial divisions and the religious divisions and the regional divisions that have plagued our politics for so long, then we will continue to see the kind of gridlock and nonperformance in Washington that is resulting in families suffering in very real ways. I'm running for president to start doing something about that suffering, and so are the people who are behind my campaign."
Note Mr. Obama's liberal use of the words "we" and "inspire" in those comments. Once again, it's a call for people ("we") to take action and using his inspirational leadership skills and abilities ("follow me") to do it.
Both Mr. McCain and Mrs. Clinton like to drone on and on about their "experience" with the Washington insiders. But, George Will, in a recent editorial comment aptly noted that …"The President who came to office with the most glittering array of experiences had served 10 years in the House of Representatives, then became minister to Russia, then served 10 years in the Senate, then four years as secretary of state (during a war that enlarged the nation by 33 percent), then was minister to Britain. Then, in 1856, James Buchanan was elected president and in just one term secured a strong claim to the rank as America's worst President."
In his editorial, Mr. Will went on to note that, "this also meant that a gentleman by the name of Abraham Lincoln, himself an "inexperienced" former one-term Congressman, clearly had an easy act to follow." However, the REAL difference between the Presidential successes of these two men was in their vastly differing leadership skills and abilities. Lincoln had them in spades. So did FDR, Kennedy and Reagan. Buchanan obviously did not.
What's more, Mr. Will noted that, "Mrs. Clinton is now 60 years old. She left Yale Law School at age 25. Evidently she considers everything she has done since school, from her years at Little Rock's Rose law firm to her good fortune with cattle futures, as presidentially relevant "experience.""
Mr. Obama, himself, has also pointed out that Mr. Rumsfeld and Mr. Cheney were well "experienced" in the ways of Washington and the military, and just look where all of THAT experience has now gotten us!
It has often been said that a President's specific job is NOT so much to "run the country", as it is to "lead the nation". What that simply means is that a candidate's leadership skills and abilities ought to be at the very top of all of our lists of "must haves" when we pick our Presidents.
The bottom line here is that experience alone does not (necessarily) equate to one's leadership ability. Conversely, leadership attributes do not solely depend on one's "experience". And while it is true that so-called "referent leadership"…. the kind that inspires people to follow you because you convey a sense that you "know the ropes"…is important, it is seldom the main element in a leader's overall success. Other qualities, such as the ability to articulate and inspire your followers while truly listening to them, freely admitting your mistakes (and then quickly learning from them) become far more important than what you may (or may not) already have in your head on "day one".
By any measure, leadership in the Office of President of the United States has been conspicuous by its absence for at least the last decade. And, because such leadership has been absent from that office for so very long, I firmly believe the American people had all but given up hope of ever seeing it again.
But, clearly, they are now seeing it revived in the candidacy of one Mr. Barack Obama.


DANA POINT – The biting wind and post-rain air temperature drop made for some frigid conditions at the Dana Hills pool deck, but in the 82-degree pool, the Dolphins girls water polo team played just as hot as their water on Tuesday.
The No. 2 seed Dana Hills scored seven goals in the second quarter and got seven goals in the game from senior Lauren Bellavia to cruise by Warren of Downey, 18-4, in a CIF-SS Division 4 first-round game at Dana Hills High School.
Dana Hills will hit the road for the second round at Woodbridge in Irvine on Thursday, Feb. 7. Woodbridge, the fourth-place team in the Pacific Coast League, beat Beaumont on the road, 4-3, in the first round.
Dana Hills battled through the South Coast League and upset El Toro in the league tournament semifinals last week to claim second-place. The Dolphins battled with Division 1 and 2 teams all season to earn the No. 2 seed in Division 4.
Dana Hills was ready from the jump and powered out to a 7-0 lead. The Dolphins led 10-1 at halftime and 15-1 after three quarters.
Bellavia scored the game's first and last goals and put in three in the third quarter for a game-high seven goals. Senior Elisa Lopez-Sanchez and sophomore Kat Besanceney each potted three goals, senior Julia Reznicek added two goals and sophomores Paige Riester, Lucy Kao and Jill Duarte each scored a goal.


Giving a clear, concise introduction to land law, this book looks at the way in which the law regulates our relationship with the land on which we walk, work, and live. Land law is about the connections between people and land, and also the relationships between people, jostling for space and allocating resources. As people change, so do the ways they use and think about land: land law today looks very different from how it did fifty years ago, and in another generation's time it will have changed again. Elizabeth Cooke introduces the building blocks of land law, namely property rights in land, and explains how they have evolved by a mixture of design and accident. The book examines ownership rights, non-ownership rights, both legal and equitable, and provides analysis of how these different rights can apply to a single piece of land, and how they are managed and enforced. Throughout the book the role of registration is central, and the implications of the Land Registration Act 2002 for English land law are fully explored. The second edition has been updated to incorporate important developments in the law relating to the family home, and in the interaction of land law with the law of human rights. It also benefits from the author's own contribution to the Law Commission's report on easements, covenants, and profits à prendre. Written in an accessible style, this book is an essential read for all those coming to the subject for the first time.


Goodwill's mission is to help people achieve their full potential through the dignity and power of work!
Click here for a complete listing of donation locations and hours of operation.
Click here for a complete listing of store locations and hours of operation.
Your donations of gently used goods are sold in our retail stores. More than 90 cents of every dollar Palmetto Goodwill generates in stores funds programs and services for people with disabilities and other barriers to employment in our community.
All sales are final. No refunds, exchanges or store credit will be made.
What types of donations will Goodwill not accept?
Please click here for a complete list of what types of donations Palmetto Goodwill can and cannot accept.
Does Goodwill accept computer donations?
Yes, Goodwill does accept donations of computers and computer equipment at all of our donation locations. Click here for more information.
Can I make a monetary donation to Goodwill?
Yes, Palmetto Goodwill does accept monetary gifts as well as donated goods. Click here to make a financial contribution.
Does Goodwill do home pickups?
Palmetto Goodwill does a limited amount of home pickups dependent on the size of the donation and location. Please contact us to see if we can arrange a pickup for your donations. All of Goodwill's retail stores feature a Goodwill Donation Drive-Through Center to make donating easy and convenient.
Does Goodwill accept vehicle donations?
Yes. We accept vehicle donations, regardless of the condition or type of vehicle. Click here for more information on how to donate your vehicle to Goodwill.
How do I enroll in one of your employment training programs?
Please visit one of our Job Link Centers to learn more about our training programs and to register for programs you are eligible for.
You are responsible for determining the fair market value of your donations to report on your taxes. Click here for a guide on how to estimate your donation's value.
Yes, Palmetto Goodwill greatly appreciates your donation of time! Click here to learn more about volunteering at Goodwill.
What employment opportunities are currently available at Palmetto Goodwill?
Palmetto Goodwill is always on the lookout for energetic employees who believe that making a difference matters. To view all job openings click here.
How do I apply for a job at Palmetto Goodwill?
Each job posting listed has a button that allows you to apply using our online application form. You will also have an opportunity to include a resume if you have one.
What if I do not have a resume? Can I fill out an employment application?
Yes, you can simply fill out an online application form.
I'd like to be able to include a cover letter with my resume, addressed to the appropriate individual. How can I find out the name of the appropriate individual?
All resumes are received in a central database and sorted by job applied for. It is not necessary to address a cover letter to a specific individual. If you would like to include a cover letter, you can paste it in the resume text field after the text of your resume or in the cover letter box provided.
What if a position I am interested in is not listed on the careers page? Can I submit a resume anyway?
No. Applications are only accepted for open positions that appear on the Jobs page of the website.
Once you have submitted your application, you will receive a confirmation email. If your skills and qualifications match what we are looking for you will be contacted by a hiring manager.
I applied for a job and have not heard back. Should I follow up?
No. Due to the large volume of applications we receive, we are unable to respond to each one. If your skills and qualifications match what we are looking for you will be contacted by a hiring manager for next steps in the hiring process. We encourage you to check back frequently as new job postings are constantly posted on the Jobs page.
I want to apply for multiple jobs at Palmetto Goodwill. Do I need to fill out an application for each one?
Yes. If you are applying for more than one position or want to apply at multiple stores, you need to submit an application for each open position.
How do I become a member of the Goodwill Rewards Card program?
Visit any one of the retail stores managed by Palmetto Goodwill to complete a registration form and you will receive your card and key tag instantly.
What are the benefits to being a member of the program?
As a Goodwill Rewards Card Member, you earn one point for each dollar spent on merchandise purchased at a Goodwill store managed by Goodwill Industries of Lower South Carolina. After you earn 250 points, and for every 250 points earned thereafter, you receive a 25% discount off of your next Goodwill purchase. Also, as a Goodwill Rewards Card member, you are eligible for exclusive promotions and special offers throughout the year.
Will my Goodwill Rewards Card be accepted at the Outlet Store?
Yes, you can use your Goodwill Rewards Card to accumulate and redeem points at the Outlet Store. Because of the extreme discounts offered at the Outlet Store, you will receive one point for every two dollars spent on merchandise at the Outlet store.
What if I do not have my Rewards card with me when I shop?
It is important to use your Goodwill Rewards card every time you shop at Goodwill. If you don't have your card with you, your cashier can look up your account before beginning your transaction. Unfortunately, there is no way to add points after the purchase has been made.


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Confront your inadequacies and push your personal boundaries: It's the surest way to grow, improve and expand the scope of your influence.
The most valuable "currency" of any organization is the initiative and creativity of its members. Every leader has the solemn moral responsibility to develop these to the maximum in all his people. This is the leader's highest priority.
Grow a leader-grow the organization. A company cannot grow without until its leaders grow within.
Nothing is more powerful for your future than being a gatherer of good ideas and information. That's called doing your homework.
It all comes down to this: If you want one year of happiness, grow grain, if you want 10 years of happiness, grow trees, if you want 100 years of happiness, grow people.
In order to be happy, human beings must feel they are continuing to grow. Clearly, we must adopt the concept of continuous improvement as a daily principle.
Keep learning; don't be arrogant by assuming that yo know it all, that you have a monopoly on the truth; always assume that you can learn something from someone else.
We only learn our limits by going beyond them. I propose that we all commit ourselves to the process of Constant and Never ending Improvement.
Leaders don't rise to the pinnacle of success without developing the right set of attitudes and habits; they make every day a masterpiece.
Coaching isn't an addition to a leader's job, it's an integral part of it.
If you are going to help people reach their potential, they need to be recognized and rewarded. Everyone needs that.
Seek advice, but make sure it's from someone who has successfully handled mistakes or adversities.
Leaders never outgrow the need to change.


Last month, the Senate voted to confirm D.C. Circuit Court nominee Neomi Rao, who will now be the first Indian American woman to sit on a federal appeals court.
Critics have repeatedly shed light on the dearth of people of color among Trump's judicial nominees, especially when compared to those of President Obama. Trump has nominated not a single African American or Latino to federal appeals courts amongst a sea of white men. Despite this, two other conservative Asian American federal appeals court nominees in addition to Rao face imminent confirmations–and lifetime appointments–to the U.S. judiciary: Michael Park and Kenneth Lee, to the Second and Ninth Circuits, respectively, have also received hearings before the Senate Judiciary Committee.
Don't be fooled: these appeals court nominees are a danger to civil rights and justice for the Asian American and Pacific Islander (AAPI) community; they are pawns in Trump's larger scheme to uphold white supremacy under the guise of promoting racial diversity in the top ranks of government.


fb772792efd1 Initial commit. Last MatPLC CVS with some makefile inclusion removed in order to compile fine out of MatPLC.
c7219a37cc39 Add conversion functions option.
2c3c4dc34979 Support for semantic verification of calls to standard functions.
01068ccb73b2 Fix make on system without mercurial installed.
89eb85bab58f Make generation of #line directives optional.
6482d83fadee Add print version command line option.
8bfcc8e62bd6 Fix C code generation when forward references (-p command line option) is on.
3127ddda2be2 Improve usability command line under windows.
c62a4078f269 Allow use of ENO keyword in structured variable field selector.


Yeah, yeah, I know. I'm the world's worst blogger. Whatever, sue me. If you're reading this, you probably came from a Russian website anyway so what's the chance you really know what I'm talking about anyway?
Here are your Random Friday Saturday Facts.
1. I've been reading a zillion responses to the New York Times article on How Yoga Can Wreck Your Body. I was going to write a response of my own, but I think there are people far wiser and more experienced who have better things to say than I. YogaDork has a Complete and Exhaustive Guide to the existing responses. These are some of my favorites.
2. Today I slept in until 11am, made myself an omelet, stayed in my PJs, and have watched 6 episodes of Grey's Anatomy.
3. I know I've already posted about my home yoga practice, but I still find it really hard to stay motivated to practice on my own.
4. I love sushi. Especially tuna nigiri and spider rolls.
5. I miss the farmer's market.
6. I still have two Christmas presents to send and one left to open.
7. I took down our Christmas decorations yesterday.
8. I told myself that the last time I donated my hair that it would be the last time. My hair is so long right now, that I'll probably just finish growing it out and donate it...again.
9. I'm contemplating going on a bike ride tomorrow, but I don't know that I have the gear--or desire--to ride my bike in the cold weather. But I need to get out and do SOMETHING.
10. I am a die hard, dedicated, loyal, tried-and-true, would-help-bury-a-dead-body kind of friend. But sometimes I feel like my friends wouldn't do the same thing for me.


Parents love to observe their children have enjoyable while enjoying video games might these be indoor or outside. Introduce children to new, thrilling ways of studying with the help of fun on-line video games, movies, experiments, puzzles, coloring sheets, and extra! The best way to get your baby to embrace studying is to make it enjoyable. As of late, kids are practically born with the power to use a smartphone and have an instantaneous understanding of technology from a younger age, and ninety one p.c of kids play video games.
Starfall has been educating children to read with phonics for well over a decade. Toddlers can be trained about different themes within the academic video games of Pocoyo by the hand of their favorite characters. Up to eight players can participate in multiplayer periods that embody modifying each other's architecture, taking part in minigames like hide-and-search and tag, chatting and using emotes, and dancing.
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text:
require_relative 'helper'

class TestFakerNameID < Test::Unit::TestCase
  include DeterministicHelper

  assert_methods_are_deterministic(
    FFaker::NameID,
    :name, :name_with_prefix, :first_name, :first_name_female, :first_name_male,
    :last_name, :prefix, :female_prefix, :male_prefix
  )

  def setup
    @tester = FFaker::NameID
  end

  def test_name
    assert_match(/\A[a-zA-Z\s]+\z/, @tester.name)
  end

  def test_name_with_prefix
    prefix, name, last_name = @tester.name_with_prefix.split(/\s+/)
    assert_include(@tester::PREFIXES, prefix)
    refute_empty(name)
    refute_empty(last_name)
  end

  def test_female_name_with_prefix
    prefix, name, last_name = @tester.female_name_with_prefix.split(/\s+/)
    assert_include(@tester::FEMALE_PREFIXES, prefix)
    assert_include(@tester::FIRST_NAMES_FEMALE, name)
    refute_empty(last_name)
  end

  def test_male_name_with_prefix
    prefix, name, last_name = @tester.male_name_with_prefix.split(/\s+/)
    assert_include(@tester::MALE_PREFIXES, prefix)
    assert_include(@tester::FIRST_NAMES_MALE, name)
    refute_empty(last_name)
  end

  def test_first_name
    assert_include(@tester::FIRST_NAMES, @tester.first_name)
  end

  def test_first_name_female
    assert_include @tester::FIRST_NAMES_FEMALE, @tester.first_name_female
  end

  def test_first_name_male
    assert_include @tester::FIRST_NAMES_MALE, @tester.first_name_male
  end

  def test_last_name
    assert_include(@tester::LAST_NAMES, @tester.last_name)
  end

  def test_prefix
    assert_include(@tester::PREFIXES, @tester.prefix)
  end

  def test_female_prefix
    assert_include(@tester::FEMALE_PREFIXES, @tester.female_prefix)
  end

  def test_male_prefix
    assert_include(@tester::MALE_PREFIXES, @tester.male_prefix)
  end
end

redpajama_set_name: RedPajamaGithub


text:
Turkey to ease restrictions if coronavirus cases decrease
The government is planning to ease restrictions imposed on businesses in line with the COVID-19 pandemic should the number of coronavirus cases decrease to a certain limit, President Recep Tayyip Erdoğan said late Feb. 1.
"We are planning to start easing the coronavirus measures that have been implemented on businesses if the number of coronavirus cases goes down to a certain limit," Erdoğan said in a press conference after attending a cabinet meeting where the coronavirus measures were discussed.
The government imposed weeknight curfews and full lockdowns on weekends in December 2020 due to a surge in the number of daily coronavirus cases, restricting the operation of restaurants and cafes to takeaways and delivery services.
While business owners are expecting to reopen their business as soon as possible, it has not been made clear as to when businesses can start operating again.
With the rising daily number of cases, which was once 5,000 and nowadays around 6,000 to 7,000, experts are speculating that the new U.K. variant of COVID-19 may be the reason for it.
"The number has risen. It is either because of the mutation of the virus or people taking coronavirus measures too lightly. I think, the number of mutated virus cases is more than reported," said Zafer Kurugöl, an academic from Ege University.
The new variant of coronavirus that emerged in the United Kingdom in December 2020 raised alarms worldwide, with experts saying that the new strain is stronger and fast-spreading than the current strain.
So far, the new strain of coronavirus has been detected in some 128 people from 17 provinces in Turkey.
Turkey's Health Ministry has decided to send coronavirus mutation detection kits to hospitals in order to check the spread of the new variant of coronavirus across the country, according to daily Hürriyet.
A second test will be conducted on anyone who tests COVID-19 positive using the new kits in order to determine the new variant of the coronavirus.
"With these new kits, we will be able to track the new coronavirus variant," Kurugöl said on Feb. 2.
Due to the new coronavirus kits, it will be easier to detect and track the U.K. variant of the virus at the end of the first half of February, Kurugöl added.
Turkey began a mass COVID-19 vaccination campaign on Jan. 14, starting with health care workers along with top officials to encourage public to get vaccinated.
Until now, nearly 2.3 million have been inoculated, according to the official website of the Health Ministry.
Elon Musk, White House discuss electric vehicles
Memphis releases deadly police beating video
Rome archaeologists search for start of Appian Way
Unlicensed foreign realtors selling houses through social media
Over 800,000 cubic meters of bottom mud removed from Lake Van
Child abuse victim 'starts new life'
Three e-scooter companies withdraw from market in Istanbul
Hospital staff attacking doctor sentenced to 11 years
Türkiye marks International Holocaust Remembrance Day
3 more arrested in ex-nationalist head's murder
Türkiye to increase gold production to reduce imports: Erdoğan
Tesla head Elon Musk met with senior White House officials on Jan. 27 to discuss the Biden administration's push to grow the electric vehicle market, Press Secretary Karine Jean-Pierre said.
Foreigners residing for a long time in the southern province of Antalya have started to work illegally as real estate agents to sell or rent properties with a 10 percent commission through social media groups amid the increasing demand of Ukrainians and Russians to reside in the city.
Vine wins Tour Down Under
Australia's Jay Vine claimed his first World Tour victory in the Tour Down Under yesterday, with Britain's Simon Yates winning a thrilling uphill battle to take the race's final stage.

redpajama_set_name: RedPajamaCommonCrawl


Welcome to Dream Land Havanese, home of AKC Havanese since 1998. We strive to provide healthy, loving, AKC Havanese puppies as lifelong companions. Parent dogs are OFA health tested for the breed..
We offer regular play days and training at our home or at a training facility in the winter. Contact me for the next play day, everyone is welcome.
Please visit our Puppy Gallery page for photos of this litter. Male and female available.
Welcome to Dream Land Miniature Horses, home of AMHA top 10 World and Supreme halter horses since 1990.
We are offering for sale several mares one from our surpreme halter mare Scott Creek Silver Contessa a many time high point halter mare.


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Aves > Accipitriformes > Accipitridae > Gypaetus
Gypaetus barbatus (Linnaeus, 1758) – Bearded Vulture
This is also known as the Lammergeier.
This species is listed as Near Threatened in the IUCN Red List of Threatened Species (https://www.iucnredlist.org/)
Gypaetus barbatus – Bearded Vulture
This species is uncommon. It inhabits remote mountainous terrains (600m-1,700m) in Asian countries including India (mainly in the Himalaya), Iraq, Iran, Nepal, Bhutan, East Russia, and in African countries including Ethiopia, Kenya, Uganda, Morocco, and Eritrea. This species has gone extinct in Montenegro, Serbia, Jordan, and Syria, and possibly extinct in Albania and North Macedonia. It mostly forages on carrions and a good amount of bones. In India, the breeding season for this species is December-June (BirdLife International 2017).
According to the IUCN Red List assessment, the population of this species is declining, with the current population estimate of 1,300-6,700 individuals. The threats to its persistence come from overgrazing, breeding habitat disturbance and ingestion of highly toxic Diclofenac (an NSAID) used in livestock (BirdLife International 2017).
BirdLife International 2017. Gypaetus barbatus (amended version of 2017 assessment). The IUCN Red List of Threatened Species 2017: e.T22695174A118590506.
https://dx.doi.org/10.2305/IUCN.UK.2017-3.RLTS.T22695174A118590506.en. Accessed on 15 February 2020.
Bhavanarayeni, R., and A. Bayani. 2023. Gypaetus barbatus (Linnaeus, 1758) – Bearded Vulture. Satose, V., A. Bayani, V. Ramachandran, P. Roy, and K. Kunte (Chief Editors). Birds of India, v. 2.17. Indian Foundation for Butterflies.
http://www.birdsofindia.org/sp/1069/Gypaetus-barbatus


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Research ArticleNANOPARTICLES
Molecular ligand modulation of palladium nanocatalysts for highly efficient and robust heterogeneous oxidation of cyclohexenone to phenol
Teng Xue1,*,
Zhaoyang Lin2,*,
Chin-Yi Chiu1,
View ORCID ProfileYongjia Li1,
View ORCID ProfileLingyan Ruan1,
Gongming Wang2,
Zipeng Zhao1,
Chain Lee2,
Xiangfeng Duan2,3,† and
View ORCID ProfileYu Huang1,3,†
1Department of Materials Science and Engineering, University of California Los Angeles, Los Angeles, CA 90095, USA.
2Department of Chemistry and Biochemistry, University of California Los Angeles, Los Angeles, CA 90095, USA.
3California NanoSystems Institute, University of California Los Angeles, Los Angeles, CA 90095, USA.
↵†Corresponding author. Email: xduan{at}chem.ucla.edu (X.D.); yhuang{at}seas.ucla.edu (Y.H.)
Teng Xue
Zhaoyang Lin
Chin-Yi Chiu
Yongjia Li
ORCID record for Yongjia Li
Lingyan Ruan
ORCID record for Lingyan Ruan
Gongming Wang
Zipeng Zhao
Chain Lee
Xiangfeng Duan
For correspondence: xduan@chem.ucla.edu yhuang@seas.ucla.edu
Yu Huang
ORCID record for Yu Huang
Metallic nanoparticles are emerging as an exciting class of heterogeneous catalysts with the potential advantages of exceptional activity, stability, recyclability, and easier separation than homogeneous catalysts. The traditional colloid nanoparticle syntheses usually involve strong surface binding ligands that could passivate the surface active sites and result in poor catalytic activity. The subsequent removal of surface ligands could reactivate the surface but often leads to metal ion leaching and/or severe Ostwald ripening with diminished catalytic activity or poor stability. Molecular ligand engineering represents a powerful strategy for the design of homogeneous molecular catalysts but is insufficiently explored for nanoparticle catalysts to date. We report a systematic investigation on molecular ligand modulation of palladium (Pd) nanoparticle catalysts. Our studies show that β-functional groups of butyric acid ligand on Pd nanoparticles can significantly modulate the catalytic reaction process to modify the catalytic activity and stability for important aerobic reactions. With a β-hydroxybutyric acid ligand, the Pd nanoparticle catalysts exhibit exceptional catalytic activity and stability with an unsaturated turnover number (TON) >3000 for dehydrogenative oxidation of cyclohexenone to phenol, greatly exceeding that of homogeneous Pd(II) catalysts (TON, ~30). This study presents a systematic investigation of molecular ligand modulation of nanoparticle catalysts and could open up a new pathway toward the design and construction of highly efficient and robust heterogeneous catalysts through molecular ligand engineering.
palladium nanoparticle
nanocatalyst
turn-over number
Heterogeneous nanoparticle catalysts are a topic of increasing interest due to their long-term stability, recyclability, and easier separation from the reaction mixture (1–4). Molecular ligands play an essential role in the design of homogeneous molecular catalysts, where the molecular ligands can be used to tune the catalytic activity, selectivity, versatility, and stability. On the other hand, the impact of molecular ligands on nanoparticle catalysts is far less understood. To date, most efforts have been limited to exploring the roles of molecular ligands in controlling the size and the facet of nanoparticles during nanoparticle synthetic steps (5–9). A few examples have suggested that a local ligand-induced microenvironment could enhance the catalytic activity by bringing the catalyst and the substrate into close proximity (10) or facilitate asymmetric reactions due to ligand chirality (11). Systematic ligand engineering studies are rarely reported toward nanoparticle catalysts simultaneously with enhanced catalytic activity and stability, especially for industry-relevant reactions. Here, we report a systematic study of heterogeneous Pd nanoparticle catalysts for aerobic oxidation reactions, especially phenol production.
Aerobic oxidation reactions have attracted significant industrial attention because of their mild and green conditions. Homogenous Pd catalysts have proved successful in driving these reactions. However, the inevitable deligation processes during the aerobic oxidation cycles can lead to the formation of inactive Pd black and deactivate the catalysts (Fig. 1) (12–14). Phenols are recognized as the key structure motif and core building block for a wide range of industrial chemicals (15). The selective functionalization of phenols is generally challenging. Electrophilic substitution represents the most common method for the synthesis of a variety of para- and ortho-substituted phenols but is not applicable for meta-substituted phenols. Dehydrogenation of cyclohexanones followed by tautomerization can result in meta-substituted phenols but is often limited by relatively low turnover, harsh reaction conditions, poor functional group tolerance, and the requirement of additional sacrificial agents (16–20). The Stahl group has recently developed a homogeneous Pd(II)-catalyzed aerobic oxidation method to enable a high-yield transformation of cyclohexenone to phenol under relatively mild reaction conditions using only oxygen as the oxidant (21). However, like other aerobic oxidation reactions, the deligation from homogeneous Pd catalysts results in catalytically inactive large Pd particles (>100 nm), leading to untimely deactivation of catalytic activity and a relatively low turnover number (TON; ~30) (22, 23). Studies have shown that heterogeneous Pd/C catalysts can catalyze dehydrogenation reactions; however, the reactions require a high catalyst/reactant ratio, an addition of hydrogen acceptors, a long reaction time, and an elevated temperature (24–26). Heterogeneous Pd nanoparticles on different supports have also been explored for oxidative dehydrogenation of cyclohexenones but typically with extremely low yield (<1.5%) (21).
Fig. 1 Reaction pathway of Pd-catalyzed aerobic dehydrogenative oxidation of cyclohexenone to phenol.
Ln represents the various β-substituted butyric acid ligands. HX represents the acids added to the reaction.
Here, we report a rational design and systematic investigation of the ligand effect on Pd nanoparticle catalysts for aerobic oxidation, especially oxidation of cyclohexenone to phenol, using variable β-substituted butyric acid as the capping ligands. Our studies show that β-hydroxybutyric acid (HB) can function as a particularly unique molecular ligand for Pd nanoparticles with excellent catalytic activity and stability and can be used to catalyze the dehydrogenative oxidation of cyclohexenone to phenol with an unsaturated TON >3000, greatly exceeding that of the homogeneous Pd(II) catalysts (TON, ~30). Further kinetic studies also demonstrated that β-functional groups of butyric acids can actively participate in the catalytic cycle to mediate the nanocatalyst activity and stability.
It has been recently shown that the homogeneous catalyst Pd(TFA)2 could catalyze aerobic dehydrogenative oxidation of cyclohexenone to phenol with a moderate yield (21). Acids are released during the cyclohexenone-to-phenol transformation processes and then reenter the catalytic cycle to regenerate catalytic active Pd(II) species. The substitution of homogeneous Pd catalysts with ultrafine Pd nanostructures can also catalyze the reaction but requires additional acid activation. Our initial studies on commercial Pd/C showed nearly no activity without acid (yield, <1%), consistent with previous studies (21). The addition of weak acetic acid (HOAc) could slightly increase the yield (6%), whereas the introduction of a strong acid, trifluoroacetic acid (TFA), could boost the yield to 67%. However, the carbon black–supported Pd nanoparticles undergo a severe Ostwald ripening process during the reaction to form large inactive particles with essentially no recyclability (yield, <1% for the recycled Pd/C catalysts).
The severe ripening issue of the commercial Pd/C could be attributed to the fact that Pd nanoparticles do not have a proper ligand environment to protect them from leaching off Pd(II) ions during the catalytic cycles. The use of ligands with a strong binding functional group could ensure nanoparticle stability but often severely compromises the catalytic activity because of the passivation of the catalytic active sites by the strong binding ligands (27). Therefore, it is a considerable challenge to design a proper surface ligand that can maintain nanoparticle stability without sacrificing the catalytic activity. To this end, we propose using butyric acid with variable β-substitution as the secondary binding site to engineer the particle stability. Instead of engineering the primary binding functional group that could fundamentally change the nanoparticle size/morphology or directly passivate the catalytic active sites, the β-functional groups can function as secondary binding sites to capture/retain the leached Pd(II) ions near the nanoparticle surface and regulate their participation in the catalytic cycle without significantly altering the binding conditions to the nanoparticle surfaces (28). The Pd nanoparticles were synthesized with a diameter of 10 nm using HB as the capping agent, following a process that we recently developed for the synthesis of Pt nanoparticles (29). The particle synthesis was conducted in aqueous solutions containing Na2PdCl4, ascorbic acid, and NaBH4. Fourier transform infrared (FTIR) studies confirm that the carboxylic group strongly binds to the Pd surfaces, whereas the β-hydroxy group only weakly interacts with the Pd surfaces (see fig. S1).
The resulting nanoparticles were supported on carbon black and used as the catalysts [3-hydroxybutyric acid–ligated Pd nanoparticles (HB-Pd/C)] for aerobic oxidation of cyclohexenone to phenol, which is compared with the catalytic behavior of the homogeneous catalyst Pd(TFA)2. Under the reaction conditions of various substrate/catalyst ratios, the TON normalized by the total amount of Pd catalyst has been determined. TON is an important measure of catalyst stability. Under low turnover conditions, namely, low substrate/catalyst ratio (100:3), the TON of the heterogeneous nanoparticle catalyst HB-Pd/C is 31, about 1.5 times higher than that of the homogeneous Pd(TFA)2 catalyst (20) after a 24-hour reaction (Table 1). HB-Pd/C also showed a maximum turnover frequency (TOF) of around 4.33 hour−1, higher than that of Pd(TFA)2 (around 2.34 hour−1). The maximum TOF is a characterization of the intrinsic catalytic activity under a given reaction condition, regardless of the reaction rate decrease toward the end of the reaction caused by the depletion of a substrate concentration. It is important to note that calculations of both the TON and the TOF are based on the total number of Pd atoms, although there are only <10% Pd surface atoms that may function as the potential active sites for the 10-nm-size Pd nanoparticles. In contrast, in the case of Pd(TFA)2 homogeneous catalysts, all Pd atoms could serve as catalytic centers. Therefore, HB-Pd/C is at least 20 times more active than Pd(TFA)2 if we only consider the surface Pd atoms. Additionally, the homogeneous catalysts suffer from the competing deligation process that leads to the formation of large inactive Pd black and thus prematurely deactivate the catalytic activity with relatively low TONs. This competition reaction can be greatly accelerated under conditions of a high substrate/catalyst ratio (30, 31), which inevitably limit the potential applications of homogeneous catalysts under industrial-favored high turnover conditions. For example, with an increased substrate/catalyst ratio of 1000:3, the reaction with the homogeneous Pd(TFA)2 catalysts quickly saturates with a maximum yield of 8.4% and a TON of 28, indicating the deactivation of the catalyst at a low TON. The loss of catalytic activity of Pd(TFA)2 is due to the formation and precipitation of large inactive Pd black particles in the reaction process (see fig. S2). In contrast, with a proper ligand environment, HB-Pd/C could drive the reaction to near completion with a yield of 95.4% and a TON of 314 (Table 1). It is important to note that the TON is unsaturated, indicating that the reaction rate is not limited by the intrinsic stability of the catalysts but only by the amount of available substrate. Further increasing the substrate/catalyst ratio to 10,000:3, the reaction with HB-Pd/C exhibits a linear time course with an unsaturated TON >3000 toward the end of the reaction (Table 1). These studies clearly demonstrate that the exceptional catalytic activity and stability of HB-Pd/C are largely retained throughout the reaction process (Fig. 2). However, we see little cyclohexanone oxidation under the same condition of cyclohexenone oxidation with either commercial Pd/C catalysts (yield, <1%) or HB-Pd/C catalysts (yield, <3%). These results are consistent with those of previous studies (23), and might be due to the change of redox potential of the Pd(0)/Pd(II) couple when interacting with different substrates.
Table 1 The TON of heterogeneous catalyst HB-Pd/C and homogeneous catalyst Pd(TFA)2 under different reaction conditions.
Under a low turnover condition, the substrate/catalyst ratio is 100:3; under a high turnover condition, the substrate/catalyst ratio is 1000:3; and under an ultrahigh turnover condition, the substrate/catalyst ratio is 10,000:3.
Fig. 2 Comparison of TON of heterogeneous nanoparticle catalysts with homogeneous molecular catalysts.
TON of time-dependent reaction catalyzed by HB-Pd/C (red line) and Pd(TFA)2 (black line) with different substrate/catalyst ratios of (A) 100:3, (B) 1000:3, and (C) 10,000:3.
To further understand the function of ligand β-functional groups, we synthesized nanoparticles using a series of butyric acid ligands with different β-functional groups and supported on carbon black for subsequent catalytic studies [HB-Pd/C, AB-Pd/C (3-aminobutyric acid–ligated Pd nanoparticles), and CB-Pd/C (3-chlorobutyric acid–ligated Pd nanoparticles)]. In general, all three types of Pd nanoparticles show a similar average size of 10 nm (Fig. 3, A to C). The similarity in particle size with different β-substituted ligands confirms that the carboxylic group is the primary binding site and dominates the binding affinity with Pd(0) at the particle surfaces, whereas β-functional groups (hydroxy, amino, and chloro) do not significantly alter the binding conditions to the nanoparticle surface.
Fig. 3 TEM morphology and size distribution of HB-Pd/C, AB-Pd/C, CB-Pd/C, and commercial Pd/C.
TEM morphology of (A) as-synthesized HB-Pd/C, (B) as-synthesized AB-Pd/C, (C) as-synthesized CB-Pd/C, (D) commercial Pd/C, (E) HB-Pd/C after 24-hour reaction, (F) AB-Pd/C after 24-hour reaction, (G) CB-Pd/C after 24-hour reaction, and (H) commercial Pd/C after 24-hour reaction. Scale bars, 40 nm. Inset histograms represent the size distribution of the corresponding samples.
We then investigated the catalytic behavior of various carbon-supported Pd nanoparticles for aerobic dehydrogenative oxidation of cyclohexenones under TFA-acidified conditions for 24 hours. The size of the Pd nanoparticles before and after catalyzing the reaction was also evaluated using a transmission electron microscope (TEM). The catalytic studies show that the HB-Pd/C–catalyzed reaction exhibits a rather high yield up to 93% (Table 2, entry 1), much higher than the commercial Pd/C. The reactions also demonstrate good heterogeneity by hot filtration test (see fig. S3), consistent with the recent finding that 3-methylcyclohexenone dehydrogenative oxidation is dominated by heterogeneous Pd nanoparticles (23). TEM studies show that the size of Pd nanoparticles does not exhibit any obvious change after the 24-hour reaction (Fig. 3, A and E). This is in stark contrast to commercial Pd/C catalysts that showed a severe ripening process and an increase in the particle size (Fig. 3, D and H) and diminished catalytic activity in the reharvested material (Table 2, entry 4). With the size of the HB-Pd/C largely maintained during the catalytic cycle, the reharvested HB-Pd/C displays a highly similar catalytic activity with a yield of 83% (Table 2, entry 1). The small decrease in the reaction yield may be partly attributed to the incomplete reharvest of all catalyst nanoparticles and also probably the inevitable equilibrium amount of Pd(II) species in the reaction solution (in equilibrium with ligated Pd nanoparticles) that cannot be reharvested. HB-Pd/C can also catalyze the reaction in other polar solvents such as N-methylpyrrolidone with a high yield (81%); however, the yield in nonpolar solvents such as hexane is low (17%), consistent with the results of homogeneous catalysts (21). The AB-Pd/C-catalyzed reaction shows a lower yield of 74% that greatly reduces to 24% in reactions with the recycled AB-Pd/C (Table 2, entry 2). The severe decrease of catalytic activity in the reharvested catalyst may be attributed to obvious Ostwald ripening of AB-Pd nanoparticles during the catalytic cycle, with the average size increasing from 10 to 24 nm after the first cycle of reaction (Fig. 3, B and F). The CB-Pd/C–catalyzed reaction exhibits an even lower initial yield of 57% in its first cycle, which is, however, largely retained (48%) in the reharvested catalysts (Table 2, entry 3). The average size of the CB-Pd/C nanoparticles is largely unchanged after catalyzing the reactions (Fig. 3, C and G).
Table 2 The yield of various heterogeneous catalysts mediated for 3-methylcyclohexenone dehydrogenative oxidation.
The reactions were carried out in 10 ml of dimethyl sulfoxide (DMSO) solutions containing 1 mmol of 3-methylcyclohexenone, 0.03 mmol of Pd-equivalent catalysts, and 1.2 mmol of TFA under 1 atm of oxygen at 100°C for 24 hours.
We have further investigated the reaction kinetics by monitoring the product yield as a function of reaction time, based on which we can determine the maximum TOF of each catalyst normalized by the total number of Pd atoms in the catalyst. The maximum TOF of the fresh HB-Pd/C is around 4.33 hour−1, higher than that of commercial Pd/C (2.85 hour−1), AB-Pd/C (2.03 hour−1), and CB-Pd/C (1.48 hour−1). The reharvested AB-Pd/C lost nearly 70% of its activity with a maximum TOF of 0.57 hour−1 (Fig. 4B), and commercial Pd/C essentially lost all its activity (Fig. 4D). The loss of the catalytic activity in these two catalysts can be largely attributed to the seriously ripened nanoparticle size during the first cycle of catalytic reaction (see Fig. 3, F and H). In the case of HB-Pd/C and CB-Pd/C catalysts, because the nanoparticle size is largely unchanged during the first cycle of reaction, the recycled catalysts show much less change in catalytic activity (Fig. 3, E and G). Overall, the HB-Pd/C shows the highest initial catalytic activity, together with excellent recyclability (with the recycled catalytic activity twice that of CB-Pd/C and six times that of AB-Pd/C catalysts).
Fig. 4 Time-dependent reaction profiles of 3-methylcyclohexenone dehydrogenative oxidation.
The black and red lines represent the reaction profiles catalyzed by the fresh and reharvested catalysts: (A) HB-Pd/C, (B) AB-Pd/C, (C) CB-Pd/C, and (D) commercial Pd/C.
Our studies clearly demonstrate that different β-substitutions in the butyric acid ligands can greatly modulate the Ostwald ripening process and the catalytic activity and recyclability of the Pd nanoparticle catalysts, suggesting that the β-functional groups may play an important role in the catalytic cycle. Pd(0) sites on the particle surface have to be activated to Pd(II) by oxygen and acid to enter the catalytic cycle and enable the subsequent chemical transformation (Fig. 1). However, the Pd(II) ions may be easily leached off from the particle surfaces and lead to serious Ostwald ripening effects. The introduction of β-functional groups on butyric acid ligands could offer secondary binding sites to capture and anchor the Pd(II) ions on the particle surface and therefore prevent them from leaching into solution, thereby contributing to Ostwald ripening. In general, the stronger binding affinity of the β-functional groups, the tighter the Pd(II) ions are anchored on the surface, and the less the Ostwald ripening effect. However, too strong a binding ligand could also severely undermine the catalytic activity by competing with the substrate binding. Therefore, a proper binding strength of surface ligands to Pd(II) is essential for ensuring the optimized catalytic activity and stability.
Predicted by hard-soft acid base theory (HSABT) (32), the binding strength to Pd(II) follows a sequence of Cl > N > O. Thus, Cl is expected to have the strongest binding affinity to prevent Pd(II) from leaching off from the surface, and thus, CB-Pd/C exhibits minimum size change and the best recyclability during the catalytic reactions. X-ray photoelectron spectroscopy (XPS) studies show that there is significantly more proportion of Pd(II) in the nanoparticles after the catalytic reaction than the as-synthesized material (see fig. S4), indicating that a large portion of Pd is activated to Pd(II) and anchored on the nanoparticle surface. On the other hand, the tight binding of 3-chlorobutyric acid to Pd(II) can also partly passivate the catalytic activity with a compromised yield and TOF.
AB-Pd/C shows the most obvious Ostwald ripening during the catalytic reactions, which appears contradictory to a trend predicted by HSABT. To understand this fact, zeta potential measurements were performed. Zeta potentials of Pd nanoparticles with different ligands were measured before and after dispersion of the particles into a reaction solution, namely, DMSO solution containing TFA (Table 3). All particles show a positive shift of zeta potential after dispersing into the TFA/DMSO solution and washing process, which can be attributed to the partial protonation of the carboxyl group of all the three ligands by TFA. It is noted that the zeta potential of HB-Pd and CB-Pd remains negative after this process, whereas the AB-Pd zeta potential shifts from negative to positive, which can be attributed to the additional protonation of an amine group to form positively charged NH3+. The protonation of AB greatly weakens its binding strength to Pd(II). Moreover, with a positive charge, the activated Pd(II) species could more likely be pushed away from the AB-Pd surface because of electrostatic repulsion from the positively charged NH3+, in contrast to an electrostatic attraction force in HB-Pd and CB-Pd. This process could greatly accelerate the Ostwald ripening of AB-Pd nanoparticles and result in reduced catalytic activity and poor recyclability, as we have seen in our experiments.
Table 3 Zeta potential measurements on Pd nanoparticles before and after dispersing into a TFA/DMSO reaction solution.
HB has a weaker binding strength to Pd(II) than CB but stronger than AB in the TFA solution. The ligation of HB prevents the activated Pd(II) from leaching into the solution and the Ostwald ripening thereof. The competition reaction of HB binding to Pd(II) is not significant compared to substrate binding because of its moderate binding strength, so that the activated Pd(II) could readily enter the catalytic cycle without passivation. The proper binding strength of HB is crucial for HB-Pd/C as a catalyst to simultaneously ensure little Ostwald ripening, outstanding stability, and excellent catalytic activity.
To further support the explanation using HSABT, we have further used 3-bromobutyric acid (BB) as a ligand to synthesized carbon-supported Pd nanoparticles (BB-Pd/C) and investigated their catalytic behavior (fig. S5). The synthesized Pd nanoparticles (BB-Pd/C) show a size similar to those obtained with the other ligands (10 nm; fig. S5A), indicating that the carboxyl group is still the dominating functional group in terms of particle formation. The catalytic reaction gave an even lower catalytic activity than CB-Pd/C (yield, 11%; fig. S5C) but with very good reharvestability (>95%; fig. S5C). This could attribute to a stronger binding affinity of a Br group (than Cl) to the Pd(II) due to the fact that Br is a softer base, which inhibits not only the Pd(II) leaching but also the catalysis. TEM studies also demonstrate that the particle sizes do not show any obvious change before and after the reaction (fig. S5B), which also support the explanation above.
In summary, by systematically engineering the ligands on the surface of Pd nanoparticle catalysts, we have created a highly active and stable heterogeneous catalyst for efficient aerobic reactions that greatly exceeds the activity of a homogeneous catalyst, especially under industry-favored high turnover conditions. The Pd nanoparticle heterogeneous catalysts could maintain undiminished activity, which is in contrast to homogeneous catalysts that typically suffer from deligation and decomposition to form large unreactive species that prevent the continuity of the reaction under high turnover conditions. Our systematic studies revealed that β-functional groups play a significant role for the high efficiency and robust characteristics of Pd nanoparticle catalysts by mediating catalytic cycles. Overall, our studies demonstrate a new strategy to design and develop heterogeneous catalysts for highly efficient chemical transformations. It can affect diverse areas, including synthetic methodology and green chemistry.
Preparation of carbon-supported Pd nanoparticles capped with β-substituted butyric acid
The preparation of different β-substituted butyric acid–capped Pd nanoparticles followed the same process. In a typical synthesis, 625 μl of Na2PdCl4 stock solution (20 mM), 50 μl of ligand solution (20 mM), and 3.80 ml of H2O were premixed in a glass vial by vigorous stirring. The NaBH4 solution (50 mM) and ascorbic acid solution (50 mM) were freshly prepared each time before use. Ascorbic acid solution (0.05 ml) was first introduced into the reaction vial, followed by the injection of 20 μl of NaBH4 solution. The final solution volume was 5 ml. The nanoparticles were allowed to grow for 20 min before being centrifuged and washed with water. The nanoparticles were then redispersed in 5 ml of water. The solution was then mixed with carbon black solution (isopropanol/water ratio of 3:2) for 10 min. The resulting mixture was centrifuged, washed with water and ethanol, and dried.
Aerobic dehydrogenative oxidation reaction conditions, recyclability, and time-dependent reaction kinetics
Typical aerobic dehydrogenative oxidation reactions were carried out in 10 ml of DMSO solutions containing 1 mmol of 3-methylcyclohexenone, 0.03 mmol of Pd-equivalent catalysts, and 1.2 mmol of TFA, under 1 atm of oxygen at 100°C for 24 hours. The reaction yield was determined via gas chromatography–mass spectrometry (GC-MS). The catalysts were centrifuged, washed with DMSO, and redispersed for recyclability tests. Time-dependent reaction courses were done by taking aliquots at each time interval and sampled by GC-MS.
fig. S1. FTIR spectrum of HB-Pd/C and HB.
fig. S2. TEM image of large particle formation after homogeneous Pd(TFA)2-catalyzed reaction.
fig. S3. Hot filtration test of HB-Pd/C–catalyzed aerobic oxidation reaction.
fig. S4. XPS spectra of CB-Pd/C before and after reaction in Pd 3d region.
fig. S5. TEM morphology and size distribution of BB-Pd/C and catalytic behavior.
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, Palladium-catalyzed aerobic dehydrogenation of substituted cyclohexanones to phenols. Science 333, 209–213 (2011).
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, Intramolecular Pd(II)-catalyzed aerobic oxidative amination of alkenes: Synthesis of six-membered N-Heterocycles. Org. Lett. 14, 1234–1237 (2012).
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, Aerobic dehydrogenation of cyclohexanone to phenol catalyzed by Pd(TFA)2/2-dimethylaminopyridine: Evidence for the role of Pd nanoparticles. J. Am. Chem. Soc. 135, 8213–8221 (2013).
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, Straightforward heterogeneous palladium catalyzed synthesis of aryl ethers and aryl amines via a solvent free aerobic and non-aerobic dehydrogenative arylation. Green Chem. 15, 347–352 (2013).
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, Straightforward solvent-free heterogeneous palladium-catalyzed synthesis of arylamines from nonaromatic substrates by dehydrogenative alkylation. ACS Sustain. Chem. Eng. 1, 1463–1473 (2013).
Q. Jiang,
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, Reaction-activated palladium catalyst for dehydrogenation of substituted cyclohexanones to phenols and H2 without oxidants and hydrogen acceptors. Chem. Sci. 6, 4674–4680 (2015).
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, Synthesis, characterization, and catalytic applications of a palladium-nanoparticle-cored dendrimer. Nano Lett. 3, 1757–1760 (2003).
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, 3-Mercaptobutyric acid as an effective capping agent for highly luminescent CdTe quantum dots: New insight into the selection of mercapto acids. J. Phys. Chem. C 116, 12346–12352 (2012).
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, Tailoring molecular specificity toward a crystal facet: A lesson from biorecognition toward Pt{111}. Nano Lett. 13, 840–846 (2013).
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, Green, catalytic oxidation of alcohols in water. Science 287, 1636–1639 (2000).
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, Green, catalytic oxidations of alcohols. Acc. Chem. Res. 35, 774–781 (2002).
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Acknowledgments: Funding: Y.H. acknowledges the support from the Office of Naval Research through award N00014-15-1-2146 (nanocatalyst synthesis). X.D. acknowledges the support from the U.S. Department of Energy, Office of Basic Energy Sciences, Division of Materials Sciences and Engineering through award DE-SC0008055 (nanocatalyst characterization and catalytic studies). Author contributions: X.D. and Y.H. designed the experiments and supervised the research. T.X. and Z.L. carried out the experiments and performed the data analysis. All other authors contributed to material characterization and product analysis. All authors discussed the results and commented on the manuscript. Competing interests: The authors declare that there are no competing interests. Data and materials availability: All data needed to evaluate the conclusions in the paper are present in the paper and/or the Supplementary Materials. Additional data related to this paper may be requested from the authors by emailing X.D. at xduan{at}chem.ucla.edu and Y.H. at yhuang{at}seas.ucla.edu.
You are going to email the following Molecular ligand modulation of palladium nanocatalysts for highly efficient and robust heterogeneous oxidation of cyclohexenone to phenol
By Teng Xue, Zhaoyang Lin, Chin-Yi Chiu, Yongjia Li, Lingyan Ruan, Gongming Wang, Zipeng Zhao, Chain Lee, Xiangfeng Duan, Yu Huang
Molecular ligand modulation of Pd nanoparticle catalysts achieves exceptional activity and stability.


An Australian university that aims to be carbon neutral by the end of 2030 has recently received an investment worth $9.1 million (£4.5m) to be more energy efficient, a news report has been able to find.
The University of Melbourne will use the funding provided by the Clean Energy Finance Corporation (CEFC) to support a variety of projects that aim to help it reduce its energy bills and improve efficiency.
They include implementation of innovative efficient and renewable energy technologies such as solar panels, voltage optimisation and micro-turbines.
Paul McCartney, Executive Director at the CEFC said: "Australia's 39 universities make a major contribution to the national economy and to the Australian community. Yet they face the ongoing challenges of public budget restraint, intensifying global competition and the need to use cutting edge technologies to meet increasing student expectations.
Beside the aforementioned energy measures, implementing a very effective energy management system will also likely contribute to achieving significant savings and that's exactly where the HeatSave programmable wireless thermostatic valves can really come in handy.


InterForm400 is an IBM i software solution enabling formatting, distribution and archiving of your reports.
Cost savings, improved corporate ID, flexibility and independence. These are some of the key words that characterizes the InterForm400 solution.
Due to making pre-printed stationary redundant and due to the optimized distribution process of documents, either via distributed print or sending the documents via e-mail.
Flexibility as InterForm400 enables you to design your own business documents and mapping the spool data according to your designed forms.
Independence is offered as you do not have to rely on the ERP vendor's assistance when wanting to change the look of your documents and even additional data can be retrieved into your documents.


It's now possible to buy my pictures online by using Paypal. Your paid picture(s) will be send (by email), or a link will be provided to you (download link) within 24 hours from your valid payment.
The pictures are in Full/Half Size (see Dimensions tag for each picture before buying) - All pictures are send in High Resolution JPG format and without any watermarks. RAW files are NOT for sale!


We provide the mobile Internet industry with data and strategy consulting services to increase advertising revenue, deepen understanding of changes in consumer behavior, and enhance competitiveness.
Our mobile Internet solutions help the mobile Internet industry to optimize brand strategy, increase sales of mobile Internet ads and enhance competitiveness. Our services target smartphones/tablet-based mobile Internet enterprises, including those specialized in instant messaging, news, online video, SNS, utility tools, internet industry apps etc. and others that intend to conduct marketing via the mobile Internet or acquire digital advertising revenue. We also provide countermeasures to help our clients respond to challenges in the fast-changing market space.
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On the Tuesday, February 26th, 2013 broadcast at 9AM Pacific/12PM Eastern our special guest is health economist diva, member in good standing ('see Jane Think') of The Walking Gallery Jane Sarasohn-Kahn, aka @healthythinker. Jane is an in demand voice on Health 2.0, Health Data Palooza, other patient empowerment venues including health tech forums. She also publishes the popular blog 'health populi'.
Her clients include all stakeholders in health, including providers, payors and plans; companies in biopharma, medical devices, financial services, technology and consumer goods; non-profits and NGOs. Jane's lens on health was best described by Dr. Regina Benjamin, U.S. Surgeon General, who says that health is where we live, work, play and pray.
Jane will update us on her plans for HiMSS and what she has in her sights for the annual event in New Orleans.
Join us for a fun and informative chat with Jane!


text:
Infamous Singer and Songwriter, Bob Dylan Set to Perform at the Legendary Buffalo Chip
**Buffalo Chip, SD (June 22, 2010) **- Bob Dylan, America's quintessential singer, songwriter, activist and poet will be gracing the renowned stage of the Legendary Buffalo Chip for a once-in-a-lifetime performance on Tuesday, August 10. A musical luminary of unmatched proportions, Dylan will be offering those in attendance a unique glimpse into his remarkable repertoire of musical contributions that have spanned nearly 50 years.
A trendsetter by every definition of the word, Dylan's slangy yet profound lyrics successfully changed the face of American music, culture and politics. Raised in the small town of Hibbing, MN, Dylan quickly made a name for himself in the early 1960's. His deeply resonant and topical songs combined with his cool detachment and playful poetic nature have challenged, intrigued, and influenced listeners for five decades. During a time of political, social and cultural upheaval, Dylan proved that music can be the catalyst for true societal change.
With his guitar, keyboard, and harmonica in tow, Dylan has explored and revolutionized a myriad of musical genres including folk, blues, country, gospel, rock and roll, and rockabilly. Backed by an impressive and changing line-up of musicians, he has toured steadily since the late 1980's on what has been dubbed the "Never Ending Tour". Dylan's Seminole works include his mega-hit albums "Blonde on Blonde", "John Wesley Harding", and "Blood on the Tracks". He has also received numerous awards over the course of his legendary career including a Grammy, Golden Globe and Academy Awards. In addition to being inducted into the Rock and Roll Hall of Fame and Songwriters Hall of Fame, in 2008 the Pulitzer Prize jury awarded him a special citation for his profound impact on popular music and American culture.
"Having Bob Dylan play at the Chip is a dream come true," explains Legendary Buffalo Chip owner, Rod Woodruff. "His musical contributions are unmatched. He is truly a legend and we're thrilled to be able to offer our guests the best of the best when it comes to entertainment."
Playing host to the largest and most prestigious motorcycle music festival of its kind, the Legendary Buffalo Chip's 2010 Sturgis Rally Week musical lineup is guaranteed to provide visitors with the ultimate Sturgis experience. To celebrate Sturgis Rally Week's 70th Anniversary, Sturgis' premier entertainment venue and motorcycle travel destination has not only rounded up an enormous selection of legendary musical acts but offers its guests an array of accommodations, created to suit any travelers' needs. The Chip boasts a cozy selection of campgrounds and RV areas as well as travel trailer and cabin rentals.
Also set to perform at the Chip's infamous outdoor amphitheatre are ZZ Top, Kid Rock, Motley Crue, Ozzy Osbourne, The Doobie Brothers, and The Scorpions. Visit www.buffalochip.com to make your reservations for Sturgis Rally Week 2010- you simply can't miss this!


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text:
Q: VBA MySQL Several queries in one Execute I'm programming a tool which grabs data from local systems and then sends data to MySQL database. Now, it's running on Access DB, but it's very time-consuming to merge data from few local databases (it's running on some computers).
I decided to move to MySQL, connection works as well executing single queries.
But doing that in this way is not time-acceptable (for my data batch - 1,5 second to add data to accdb and almost 80 seconds to add the same to MySQL).
I'm aware that remote MySQL database will never be so fast as local Access DB (MySQL DB is on shared hosting, it's my private project).
I talked to my friend who is PHP & MySQL dev and he told me that running queries at batch would shorten the execution (e.g. execute 100 queries in one time instead of 100 single executions).
I modified my script to do so, but if I try to execute multiple queries I have Syntax Error (when I paste the same query into phpMyAdmin immediate window it works, so this is not syntax).
I read that ADODB Connection (which I use) cannot execute multiple queries - but if there any alternative?
I could write little console .NET application which reads .sql files and then executes a batch query, but first I want to be sure if it's really necessary.
My connection is declared
Set cn = CreateObject("ADODB.Connection")
cn.Open "Driver={MySQL ODBC 5.3 Unicode Driver};Server=SERVER;Database=DB_NAME;Uid=DB_USER;Pwd=DB_PWD;Option=3"

strQuery = "CREATE TABLE Z AS (SELECT * FROM tblOffers WHERE 1=2); CREATE TABLE ZZ AS (SELECT * FROM tblOffers WHERE 1=2);"
cn.Execute (strQuery)

These queries are just for testing - I'm not creating new tables in my project, but upsering data (insert or update if duplicate).
My single query looks like this:
INSERT INTO tblOffers (`TITLE`, `LINK`, `IMG`, `PRICE`, `DATE`, `PLATFORM`, `OFF_ID`, `LOCATION_ID`)
SELECT * FROM (
SELECT "Zgrywus PC", "https://www","zgrywus-pc-znin.jpg",10,'2017-07-08',"PC","6hZH9","0929865") As Tmp
ON DUPLICATE KEY
UPDATE `TITLE` = "Zgrywus PC",
`LINK` = "https://www",
`IMG` = "zgrywus-pc-znin.jpg",
`PRICE` = 10,
`DATE` = '2017-07-08',
`PLATFORM` = "PC",
`OFF_ID` = "6hZH9",
`LOCATION_ID` = "0929865";

EDIT: @joanolo, here's full code snippet:
Sub ExportDataToAccess()

    Dim cn As Object
    Dim strQuery As String, strClrQuery As String
    Set cn = CreateObject("ADODB.Connection")

    cn.Open "Driver={MySQL ODBC 5.3 Unicode Driver};Server=SERVER;Database=DB;Uid=UN;Pwd=PWD;Option=3"
    strQuery = "CREATE TABLE Z AS (SELECT * FROM tblOffers WHERE 1=2); CREATE TABLE ZZ AS (SELECT * FROM tblOffers WHERE 1=2);"
    Debug.Print strQuery
    cn.Execute (strQuery)

    cn.Close
    Set cn = Nothing

End Sub

And produced error is:
Screen
EDIT2, 10-07-2017
I decided to run multiple row INSERT - it works - so my problem is resolved, but if anyone would have any solve for issue of this topic, please share.

A: @Krukosz - I had the same question today, I solved it on another way. Well you can execute each command in a ForEach- oder other Loop, separated/splitted by the 'virtual' Dash-Comma ';' you use in 'normal' SQL-Statements not in VBA. It's cool that you can use vars over more Execute's.
Here is an example code, and @start will be 1082 in the end of this example. But it seems to remember vars only for a few minutes. If you wait 5 minutes and try the last row again, the value of @start will be 'Null'.
Set rst = dbc.Execute("SET @start = 898")
Set rst = dbc.Execute("SET @start = @start+184 ")
Set rst = dbc.Execute("SELECT @start,'test'")
..
.

redpajama_set_name: RedPajamaStackExchange


text:
Joy Lean Covington
January 6, 1930 - December 14, 2017
Joy Lean Covington, age 87, a 63-year resident of Wynne, Arkansas, died on Thursday, December 14, 2017, in Springdale, Arkansas. She was born on January 6, 1930, near Sumpter, Arkansas, the daughter of Howard Freddie Jones and Obelia Beasley Jones. Joy grew up and worked in Warren, Arkansas, and in 1950, she married her husband, Dr. Leslie Hughes "Doc" Covington, Sr. After living in Little Rock, in 1952, they moved to Wynne for his work with the Soil Conservation Service, and she worked at Manning Drug Store. Starting in 1960, remaining in Wynne, she supported her husband's return to college at the University of Tennessee College of Dentistry, where he graduated in 1964. For most of the 38 years Dr. Covington practiced Dentistry in Wynne, Joy was the Office Manager for his practice, and was instrumental in serving their patients. She was a long-time member of the Wynne Baptist Church where she was active with her Sunday School class and supported youth group activities during her sons' teenage years. She attended and enjoyed all her sons' athletic games and other school activities, believing that football keeps boys busy, tired and out of trouble. She loved great food, Sunday lunch at Kelly's with her friends, nice restaurants in Memphis and Little Rock, Razorback football and basketball games, musical theatre, and group trips with her husband and friends. Joy was a strong advocate for college education and most proud that she and Dr. Covington were able to fully fund their four sons' college education. She was known for her hospitality, especially to her sons' friends, and hosted a great Christmas Eve party every year for the entire crew. Two of her favorite sayings sum up her life: "Smile and the world will smile back at you", "You have a choice in life to be happy or sad, happy is a lot more fun!" She was preceded in death by her husband, her parents, sister, Retha Marlene Williams, brother, Kenneth Alton "Buster" Jones, and niece, Ruth Ann Racely. Joy is survived by her four sons, Dr. Kenneth Hughes (Laura Victoria) Covington of Eureka Springs, Arkansas, Leslie Jones (Shona Joy) Covington of Cherokee Village, Arkansas, Josie Lee (Heather Hunnicutt) Covington II of McLean, Virginia, and Leslie Hughes (Laura Lea) Covington, Jr. of Fayetteville, Arkansas; seven grandchildren, Joseph Griggs (Kimberly) Covington of Fayetteville, Arkansas, Kenneth Cash (Meredith Ann) Covington of Kirkwood, Missouri, Joy Victoria Covington, Katherine Joy Covington, Kendall Faith Covington, Abigail Elizabeth Covington, Ella Claire Covington and Leslie Hughes Covington, III; five great grandchildren, EmMarie Victoria Covington, Joseph Malachi Covington, Vivian Kay Covington, Henry Cash Covington and Norah Ann Covington; nieces and nephews, Joe "Butch" Williams, Joan Jennings, Frances Jean Caldwell, and Jim Williams, and other nephews and nieces. Joy's life will be celebrated during a service on Wednesday, December 20, 2016 at 1:00 p.m. at Cogbill Cemetery in Wynne, Arkansas. Kernodle Funeral Home is in charge of the arrangements, (870)-238-2323, www.kernodlefh.com In lieu of flowers, donations in Joy's honor can be made to the Yellowjacket Foundation--Dr. Leslie and Joy Covington Scholarship Fund, which will provide college scholarships to graduates of Wynne High School. Donations can be mailed to Sharon H. Lawson, Treasurer, Yellowjacket Foundation, 2003 Airpark Rd, Wynne, AR, 72396.
Joy Lean Covington, age 87, a 63-year resident of Wynne, Arkansas, died on Thursday, December 14, 2017, in Springdale, Arkansas. She was born on January 6, 1930, near Sumpter, Arkansas, the daughter of Howard Freddie Jones and Obelia Beasley... View Obituary & Service Information
The family of Joy Lean Covington created this Life Tributes page to make it easy to share your memories.
Joy Lean Covington, age 87, a 63-year resident of Wynne, Arkansas,...
Send flowers to the Covington family.


It wasn't right after having a baby but more around the two year mark, I noticed that there were things that changed about my body that I didn't quite expect and that I couldn't really change. I started shying away from being in photographs and would mostly be behind the camera, taking photos with my phone or camera of my crazy toddler. But when I look back on the memories I have with him, I know I am there, but I'm not part of the picture. Someday, when he's looking back at photos of his life, I want him to see me holding his hand gently, giving him compulsive cheek kisses every five seconds because I just can't help it, and showing him how to love and live in this world.
So, mamas out there, even if you don't feel like it for one reason or another, I want you to get in front of the camera. You are an important part of your child's story and ten and twenty years from now, I want you to be able to remember how you held his tiny hands in yours and kissed all of his fingers just because you couldn't help it. I want you to keep and treasure these moments that we all know go by too fast. Trust me, I know it's hard to bring yourself to be in front of the camera, but it will be so worth it.
The simple secret to capturing a beautiful maternity season: stop focusing on the belly.


"Be imitators of me, as I am of Christ. I commend you because you remember me in everything and maintain the traditions even as I have delivered them to you. But I want you to understand that the head of every man is Christ, the head of a woman is her husband, and the head of Christ is God.
St. Paul writes that he wishes the Corinthians to "maintain the traditions even as I have delivered them to you." He did not make this up just for their culture. Rather, he is passing on a tradition of women covering their heads and men not doing so. This tradition was from the Apostles and it was maintained until the 1960s when so many liturgical traditions were discarded.
The 1917 Code of Canon law required women to cover their heads and forbade men from covering their heads. The 1983 Code of Canon law omitted the passage about women covering their heads, but maintained that men should not.
St. Thomas Aquinas explains this statement from 1 Corinthians 11.10 simply by saying that it is because Angels are present at the Holy Sacrifice of the Mass, men must show reverence as well as women. Women show reverence by covering their heads, and men show reverence by not covering their heads.
Women still cover their heads when they have an audience with the pope.
What do you think of chapel veils? Join the conversation in the comments!
Susanna, after earning her MA in Theology at Franciscan University of Steubenville, lives in St. Paul, MN with her husband and four children. She spends her time going to beautiful liturgies, cooking, reading literature, home schooling her children, and writing all about it at her blog Living With Lady Philosophy.


text:
Temperature problems result in olive recall because of botulism danger
By News Desk on October 10, 2019
UNFI is recalling cases of "Arla Apetina Marinated Feta & Olives in Oil, Pitted" distributed in seven states because the product may have been exposed to conditions that allow the bacteria that causes botulism poisoning to grow.
A total of 75 cases of this product were distributed to 69 retail customers serviced by UNFI distribution centers in Greenwood, IN. and Sarasota, Fla. between Jan. 1, 2019 and Aug. 30 in Indiana, Kentucky, Illinois, Michigan, Florida, Ohio, and Missouri.
"The product requires refrigeration to ensure food safety and we have learned that some product distributed to retail customers from two UNFI distribution centers may have been exposed to temperatures above refrigeration during storage and/or distribution by UNFI'S customers," according to the company's recall notice.
"Extended exposure to above-refrigerated temperatures may allow the growth of bacteria such as Clostridium Botulinum to reach unsafe levels, which if consumed can cause life-threatening illness or death."
The company's recall notice, posted by the Food and Drug Administration, did not include the names of any of the retail stores that received the recalled olives. The recall notice states that 69 retailers received the product.
Consumers can determine whether they have the recalled product by checking the 3.1-pound plastic packages for UPC number 9393605697.
"Retailers who have purchased the Arla Apetina Marinated Feta & Olives in Oil, Pitted product from these two distribution centers should remove any remaining product from the supply chain and discard the product in a manner that would prevent its consumption or distribution and contact their UNFI account managers for a full refund," according to the recall notice.
Consumers with questions may contact the company at 800-451-2525.
About botulism poisoning
Anyone who has eaten any of the recalled products and developed signs of botulism poisoning should immediately seek medical attention, according to information from the CDC. Untreated, botulism can paralyze the muscles needed for breathing, resulting in sudden death.
"In foodborne botulism, symptoms generally begin 18 to 36 hours after eating contaminated food. However, symptoms can begin as soon as 6 hours after or up to 10 days later," according to the CDC website.
The symptoms of botulism may include some or all of the following: double vision, blurred vision, drooping eyelids, slurred speech, difficulty swallowing, difficulty breathing, a thick-feeling tongue, dry mouth, and muscle weakness.
People with botulism may not show all of these symptoms at once.
These symptoms all result from muscle paralysis caused by the toxin. If untreated, the disease may progress and symptoms may worsen to cause paralysis of certain muscles, including those used in breathing and those in the arms, legs, and the body from the neck to the pelvis area.
Tags: botulism, Clostridium botulinum, FDA, olives, UNFI