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Jack Hanna Returns to Luhrs
For the third year in a row, one of America's most beloved animal experts, Jack Hanna, took his three-time Emmy Award winning television series to the stage of the H. Ric Luhrs Performing Arts Center.
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For the third year in a row, one of America's most beloved animal experts, Jack Hanna, took his three-time Emmy Award winning television series to the stage of the H. Ric Luhrs Performing Arts Center.
American zookeeper Jack Hanna brings the fun of the zoo to the Luhr's center stage with a variety of exotic animals for fans to see. Some of the animals featured during Into The Wild Live! included a two-toed sloth, wild cats and a baby kangaroo.
"How many dirty girls we got here tonight?"
Foreigner highlights the bright future of younger generations and the importance of education by welcoming the Shippensburg Area Middle School chorus on stage to sing alongside the band.
The Shippensburg University Jazz Ensemble brought everything it had for its final show of the semester on April 17 at The Thought Lot.
Hallow Creek Band will be opening for the Bovine Social Club at The Though Lot Saturday for a live album release.
WSYC 88.7 FM's annual "Up All Night" broadcast this past weekend made many Shippensburg University students surrender one of the things they value most — their sleep.
WSYC 88.7 FM DJ's took the mic for 24-hours on air during the station's annual "Up All Night" broadcast. "Up All Night" originated in 2012 and has been a tradition ever since.
The Shippensburg University Community Orchestra gathered Sunday afternoon in the H. Ric Luhrs Performing Arts Center for one of the last musical performances of the academic year.
SU Community orchestra united to perform their annual spring concert at Luhrs.
Netflix creators pulled a popular high school novel off the dusty bookshelves and onto screens nationwide.
Students showed off their poems at a recent exhibit in the library. This is the second year the event has been held.
Shippensburg University's campus radio station, WSYC 88.7 FM, will be on air for 24 hours nonstop from 8 a.m. April 21 to 8 a.m. April 22, for its fourth "Up All Night" broadcast event.
The Thought Lot displayed a throwback show of jazz and Dixie music Saturday with the Keating Jazz Orchestra, which showcased its skills to a packed house.
Rebecca Schrom and Lee Howard from the Keating Jazz Orchestra sing legendary jazz songs from famous singers. (Right) Duo Jessica Jellen and Mark Burke opened the evening with a laid back atmosphere on Saturday.
A new poetry exhibit, featuring the work of multiple English students, opened Thursday afternoon in the Shippensburg University Ezra Lehman Memorial Library.


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Since 2003, the Healthy Back Institute has helped millions of people from around the world to get lasting relief from lower back pain, neck pain and sciati
Keeping your back healthy is a daily commitment. It helps to do daily stretches and exercises specifically designed to prevent back pain. Follow these easy.
Upper Back Pain and Lungs – the link and how should you approach it? Seek medical advice if you have symptoms of upper back and chest pain, pain in lungs.
Ergonomic furniture designed to relieve back and joint pain and promote health and well-being. Visit Bad Backs and explore our huge range of Ergonomic.
Luckily, unlike lower-back pain, upper-bac.more. "A program such as Pilates can help build up the scapular stabilizing muscles and core strength.".
Sep 11, 2017. Pilates is a method of exercising that stretches, strengthen and balances the. that practicing Pilates can help to resolve neck pain and to improve your ability. it strengthens the muscles in your cervical spine and upper back.
Sep 5, 2013. Yoga, Pilates, foundation training, and the Gokhale Method are some of the core exercises that can help treat back pain and improve your.
Building core strength has been hailed as a way to prevent back pain – but beware, writes Thea O'Connor.
Ease the pain with this gentle yoga and Pilates fusion sequence. You might also. Get in plank position, draping the resistance band across your upper back.
Apr 21, 2017. 6 Pilates Moves To Sculpt Your Upper Body And Shoulders. Apr 21. As a bonus , they can also help alleviate shoulder and back pain, too.
Learn about the thoracic spine and how the structures can lead to upper back pain. The thoracic spine has several features that distinguish it from the.
This workout is designed to release tightness in the upper back and chest area. Most of the exercises are gentle stretches that will relieve discomfort.
Article discusses the prevalence of back pain, and offers suggestions for reducing pain among drivers.
Pilates Workout Videos related to Upper Back Pain
Feb 2, 2016. For example, some Pilates exercises target lower back pain rather than upper. You want to tailor your exercises to your needs, so find a doctor.
Examine upper back pain causes, including common and uncommon causes of upper back pain, including muscular irritation, joint dysfunction and more.
Pilates exercises can help decrease back pain. Learn these beginner exercises that promote core stability, and stretch and strengthen the back.
Has anyone had any experience with upper abdominal pain late in the 3rd trimester that feels like burning? almost like an internal sunburn? My doctor tested
Upper Back Pain Exercise: Find out what may be causing your upper back pain and how you can correct it with simple tricks and exercises.
Back pain. Relieving back pain. Thoracic extension. Improving upper back flexibility on the foam roller. Small group Pilates. Prepping for the hundred. Upper.
Get relief from your head, neck, and upper back pain at Physio Logic with services like physical therapy, chiropractic, acupuncture and massage therapy.
In the context of the spinal health, Pilates maybe one of the most effective and. floor and slowly roll it up (segment by segment) starting with your upper back.
How to Strengthen Your Back with Pilates. Pull in your lower abdominal muscles and curl the lower back, middle back and upper back towards the ceiling.
How to Prevent Upper Back Pain. About 84% of adults will experience some sort of back pain in their lives.http://www.rochesterhealth.com/healthnotes.
types of unsuccessful pain management techniques Pilates was most. stability for the low back and also strengthen the upper back and neck muscles to.
Mar 29, 2016. Regular yoga or Pilates sessions can also help relieve upper and middle back pain as they incorporate a number of positions and moves that.
Stinging Upper Back Pain You may feel a sudden burning or stinging pain in your arm or between your neck and shoulder. Your shoulder or arm may be tingly, weak, or numb. It also may. Jul 6, 2017. Information on the treatment and causes of back pain including strained back. Sharp, localized pains in their lower back, upper back,
Upper and middle back pain, which can occur anywhere from the base of your neck to the bottom of your rib cage, has become much more common as more of us.
Do you ever feel tight in your upper back area? Have you been sitting behind the computer too long? Have you been driving for a long time? Have you been.
1 Relieving Upper Back Pain by Strengthening the Major Muscle Groups that Act on the Shoulder Joint Jacqueline Christy February 25, 2015 Balanced Bodies, Herndon, VA.
Apr 22, 2012. One person may go to Pilates and it helps with their back pain, for another. the muscles in the core and can result in poor upper body posture.
These Pilates exercises will work your core to prevent and ease nagging back pain.
Free article to fix neck, shoulder, and upper back pain, upper crossed syndrome, without surgery by Dr. Jolie Bookspan, The Fitness Fixer sports medicine.
In today's workout I'm sharing four upper back stretches that will make your spine. This 10 minute Pilates workout video will help you reduce low back pain by.
Pilates exercise is an exercise program that can provide back pain relief and help prevent future episodes of back pain.
Pilates is all about relieving muscle tension through stretching. Stress and poor. Prevent upper-back pain by practicing Pilates stretches. Pilates is all about.
How to Treat Upper Back Pain. Upper back pain (in the thoracic region of the spine, below the neck and along the length of the ribs) is often the result of.
Mar 1, 2017. Joining a Pilates class can dramatically improve your back pain, just. Begin with the upper back and work your way down, vertebrae by.
An expert explains how Pilates can help you maintain good posture and prevent back pain.
PhysioAdvisor offers detailed physiotherapy information on upper back exercises including upper back rehabilitation and upper back strengthening exercises. Antero-Lateral Ankle Impingement · Complex Regional Pain Syndrome. Balls ( For Self Massage); Foam Rollers (For Self Massage and Pilates Exercises).
Pilates exercises can help decrease back pain. Learn these beginner exercises that promote core stability, and stretch and strengthen the back.
More Back Pains Articles ...
- Mid Back Pain From Golf: Looking for back pain relief? Back pain sufferers need to try chiropractic, the all-natural approach to back pain without risky drugs or surgery. Golf often leads to low back pain and muscle strain. Find out how to prevent low back pain when golfing ...
- Back Pain Nerve Diagram: Excessive Gas Lower Back Pains Fatigue Additionally, high cholesterol may be due to eating excess carbohydrates, and calories. Tiredness or fatigue; Poor memory, depression, excessive emotions and or drop in. Aching pain (felt at particular parts; an...
- Prevention Of Low Back Pain: Prevention of Low Back Pain. KRAUS, HANS M.D. Journal of Occupational Medicine: November 1967 - Volume 9 - Issue 11 - ppg 555-559. Original Article: PDF Only. There is no clear evidence that you can prevent low back pain. But there are some things yo...
- Why Is My Back In So Much Pain: I have had a pain in my lower back now for 8+ weeks. The pain is only really when im sat down on a chair or driving in the car etc. I can sometimes feel. Is It Okay To Workout With Lower Back Pain Back pain can be treated and prevented with exercise,...
- Lower Back Pain When I Stand Up: Mar 26, 2014. Here is one of our Pain Stop patients, Kevin Baldock, sharing how having a stand up office has made a big difference in his lower back pain. Deadlifting And Your Lower Back. You see, for many guys, having a sore lower back after deadlif...
- Unilateral Low Back Pain Diagnosis: Suggestions for Urinary Tract Infection (UTI) If symptoms such as lower back pain or burning while urinating are too uncomfortable, try placing a heated. When evaluating LBP, assess whether the patient has nonspecific LBP, back pain with radiculopath...

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OIOpublisher There are fewer than four weeks to go until the UK's annual Ice Cream and Gelato Expo in North Yorkshire. Taking place from 12-14th February at the Yorkshire Event
Posts From Catering Scotland
Tying in with today's launch of the 2019 CIS Excellence Awards, in partnership with Caterer.com, our friends at Scotland Food & Drink interviewed Kevin McGillivray, Scottish Culinary Team Director and
Entries and nominations for the 16th annual CIS Excellence Awards, in partnership with Caterer.com, are now OPEN. Aimed at ALL businesses and individuals involved in Scotland's catering, hospitality and tourism
The organisers of ScotHot have announced that the show has just 20% remaining exhibitor capacity for 2019. The event, which takes place from 13th-14th March at the SEC Glasgow, provids exhibitors and
Willie MacLeod explains why the majority of accommodation businesses in the city (including hotels, serviced apartments, B&Bs, hostels and self-catering properties) are
With no fewer than 122 active distilleries across the country, the Scottish whisky sector is enjoying one of its greatest
Chartered surveyors Graham & Sibbald are offering to market a popular and successful restaurant premises in the centre of Blairgowrie. Situated
With the growth of food tourism proving a major contributor to Scotland's burgeoning hospitality sector, demand for holiday rentals is
Craig Haddow has been confirmed as the new general manager of the newly revamped Kingshouse Hotel and Bunkhouse in Glencoe.
Scotland's national culinary team returned home from the Culinary World Cup in Luxembourg last month with a silver medal win under


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text: Crypto Top altcoins for May 2018 and crypto tech analysis by Mark Gary the Crow May 18, 2018 No Comments Prev Article Next Article Facebook Prev Article Next Article About The Author Gary the Crow More from this Author BuzzingCrow.com Curator and Mascot - Very powerful; capable of collecting and disseminating information instantaneously. Possesses ability to sense auras and see through political deception. Enjoys holidays in Montego Bay with his cousin Henry, who is currently wanted for lifting wallets and other petty crimes. Known in several circles as "Unhairy Gary". Related Posts Short Term Bottom? Stellar & BAT Looking Bullish + XRP & ETH Gary the Crow November 16, 2018 All Fiat Currencies will Eventually Become Cryptocurrencies – Today's Crypto News Gary the Crow June 21, 2018 Cryptocurrency Trading with Altcoin Buzz and Blockedge Capital! Gary the Crow April 15, 2018 Altcoin News – Cryptocurrency and Bitcoin Bullish? Abu Dhabi Markets, T-Mobile Blockchain, Bitstrade Gary the Crow February 12, 2018 WHY THE JULY CRYPTO BREAKOUT MAY HAPPEN SOON??? 🤑 Gary the Crow July 13, 2018 Altcoin News – South Korea Rules, Russia, Bitcoin Exchange, BlackRock, Ripple to Soar? BlockDelhi Gary the Crow January 30, 2018 Add Comment Cancel reply


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The last advantage I would love to go over, in fact includes two benefits. Coloring allows your kid's creativity to blossom, but it likewise gives understanding right into a child's emotions, as well as typically youngster psychologists will certainly utilize this device to find out more regarding a kid's feelings or mindset at a particular time.
To obtain the alphabet tinting web pages it is extremely straightforward. You just need to click the web pages detailed in the site and also select them. As new window opens you locate the complete view of the web pages. Now go to the choice Publish in the File Food selection as well as command 'Publish'. The printer linked to your computer system or laptop computer would print the page/s. When you are done, shut the home window. It is that easy. You can find hundreds of such valuable tinting pages with alphabetical video games that enable your kids not just to find out the alphabets, but also remember them and compose them correctly.
We have yet to review the benefit that your child will be learning more about the different colors as they color their pages. And the more exposure your child has to tinting, the even more they will discover the typical shades of things, and they will start to select specific colors for particular products, such as red apples, or environment-friendly fallen leaves. As well as, as they get older, you will likewise start to see that they will certainly tint pets the shade that they absolutely are. This might appear obvious to somebody who has actually known their colors since they can bear in mind, but you had to learn it eventually as well as this is a great means for your youngster to discover theirs.
This creative art that is moved to the children by supplying extremely productive tinting sheets is intended to cope up with his/her consistent search for the latest things and also topics. As an example, you can pick an unique tinting topic such as Christmas; by choosing a special topic, you will aid the child discover more about a particular issue. This matter will certainly be illustrated on the web page thus establishing the kid's coloring skills; the fine electric motor and coloring abilities will certainly thus be established because these abilities are very essential especially when dealing with the young children.


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LIVONIA, Mich. -- A123 Systems Inc. today opened a lithium ion battery plant to supply advanced technology for the coming wave of electric vehicles.
President Barack Obama heralded the plant as "central to the next generation of cars."
Obama -- highlighting his administration's efforts to encourage battery technology development through last year's economic stimulus -- called A123 Systems CEO David Vieau during dedication ceremonies at the suburban Detroit plant.
"This is about the birth of an entire new industry in America -- an industry that's going to be central to the next generation of cars," Obama said in the phone call, according to a transcript provided by the White House.
It is the largest lithium ion battery plant in the United States -- at 291,000 square feet -- and should strengthen the nation's presence in battery manufacturing, now dominated by Asian companies, the White House says.
A123 Systems has signed battery supply agreements this year with domestic and foreign automakers such as Fisker Automotive Inc., Navistar Inc. and Modec Ltd.'s joint venture Navistar-Modec EV Alliance.
Analyst A.T. Kearney predicts the global market for electric and hybrid cars will rise to $21.8 billion by 2015 from about $31.9 million in 2009 because of increased government incentives.
The state of Michigan has awarded A123 $238 million in incentives and plans to continue to invest in alternative energy technologies.
With the forthcoming launch of the Chevrolet Volt plug-in hybrid and Nissan Motor Co.'s all-electric Leaf, America is seeing the beginning of a new era in car manufacturing.
Michigan Gov. Jennifer Granholm said Asia currently dominates 98 percent of the advanced battery technology market. The United States aims to hold 40 percent of the market by 2015.
"This is the thing that will pull the U.S. auto industry out of the last few years," said Micky Bly, a General Motors Co. spokesman.
A123 already has hired 300 employees in Michigan and plans to create up to 3,000 additional jobs by 2012 as production increases. Granholm noted that about half of the 250 employees in the plant were unemployed before to joining the company.
Although the company lost the contract to supply batteries for the Volt to Korea's LG Chem, A123 Systems is still working closely with GM and may be the supplier for the next version of the Volt. A123 raised $391 million during an initial public offering last year. A portion of the money raised in the IPO will be used to match government funding of nearly $250 million granted by the U.S. Department of Energy.
"State and federal money has made manufacturing a possibility on the front end, but this is not something the company will rely on long term," Jason, Forcier, A123 Systems' vice president of automotive solutions, said in a recent interview with Automotive News.


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You can see my latest speeches and appearances in Parliament here:
I am grateful to my hon. Friend; he is of course correct on all counts.
Indeed, the Government listened very carefully when the House passed the so-called Brady amendment and have pursued the strands of work t
My hon. Friend has long been a keen student of these issues.
I have not been seeking to blame anybody.
I can agree with the hon.
My hon. Friend knows the Government's position.
I have not yet read the speech, so it would be wholly premature of me to assume what my right hon.
I note with care the hon. Gentleman's position and I have observed what he is doing to represent his constituents.
The hon. Gentleman, with his deep knowledge of the border, speaks absolute truth when he talks about its complexity.
Well, well. My hon. Friend tempts me down an interesting path.


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Little improvements in php proyect
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*** WHO IS ELIGIBLE TO APPLY *** You must live in: China ***PROJECT SUMMARY*** I intend to order some custom-made men's leather dress shoes made in China which will be shipped to me in Los Angeles, California. How much would you charge me in US dollars here on Freelancer.com to walk into ten (10) shoemaker stores (cobbler shops) that normally make custom-made men's leather dress sh...


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King Arthur's Tools 45822 Lancelot 22 tooth, 5/8" center hole
King Arthur's Tools
Regular price $32.47
Lancelot Woodcarving Discs take the muscle work out of woodcarving with their speed, power and maneuverability. The secret is in the special chain saw blade which is securely held between two stainless steel plates. Mount the 4" diameter Lancelot in your 4" or 4-1/2" angle grinder and watch the chips fly! It easily cuts the hardest woods regardless of grain or knots. The 14-tooth model is great for "roughing out" the 22-tooth model and leaves a smoother "finished" surface. Teeth can be resharpened using a standard chain saw file. Maximum 14,000 RPM. Chains can not be interchanged between models. Squire Mini Woodcarving Discs can be attached to another disc for the ultimate in power carving! Although it can be used alone as a small carving disc, by attaching the 3-3/8" diameter Squire to a Lancelot Disc with the Universal Mounting Nut you can effectively double your cutting capacity. You not only remove waste material faster but curved work, like the inside of bowls, is easier and smoother than when using a single disc. Fits all mini grinders with 5/8" x 11 TPI arbors.
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Ray Charles Modern Sounds in Country & Western Music Vol. 1 & 2, with Bonus Tracks (2-CD)
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sku: ZNOT 539
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CD Details
- Number of Discs: 2
- Released: 2014
- Originally Released: 2014
- Label: Not Now Music
Entertainment Reviews:
Rolling Stone - 12/11/03, p.120Ranked #104 in Rolling Stone's "500 Greatest Albums Of All Time" - "[A] model of folk-pop healing music..."
Tracks on Disc 1:
- 1.Bye Bye, Love
- 2.You Don't Know Me
- 3.Half As Much
- 4.I Love You so Much It Hurts
- 5.Just A Little Lovin'
- 6.Born To Lose
- 7.Worried Mind
- 8.It Makes No Difference Now
- 9.You Win Again
- 10.Careless Love
- 11.I Can't Stop Loving You
- 12.Hey Good Lookin'
- 13.I'm Movin' On
- 14.Leave My Woman Alone
- 15.Unchain My Heart
Tracks on Disc 2:
- 1.You Are My Sunshine
- 2.No Letter Today
- 3.Someday (You'll Want Me To Want You)
- 4.Don't Tell Me Your Troubles
- 5.Midnight
- 6.Oh, Lonesome Me
- 7.Take These Chains From My Heart
- 8.Your Cheating Heart
- 9.I'll Never Stand In Your Way
- 10.Making Believe
- 11.Teardrops In My Heart
- 12.Hang Your Head In Shame
- 13.Georgia On My Mind
- 14.Carry Me Back To Old Virginny
- 15.Deep In The Heart of Texas
Product Description:
Personnel includes: Ray Charles (vocals, piano); David "Fathead" Newman (saxophone).
Enginners include: Gene Thompson, Bill Putnam, Johnny Cue.
Recorded in 1962-1963 at Capitol Studios, New York, New York; United Recording Studios, Hollywood, California; RPM International Studios, Los Angeles, California. Includes liner notes by Todd Everett.
Ray Charles had dabbled with country music at Atlantic, notably 'I'm Movin' On', but the move to ABC-Paramount prompted him to record a full album. His version of Don Gibson's 'I Can't Stop Loving You' was a transatlantic number 1 and not far behind his bittersweet performance of Eddy Arnold's 'You Don't Know Me'. Ray's own favourite was 'I Love You So Much It Hurts'. The album was so successful that he recorded a second volume and had hits with 'Take These Chains From My Heart' and 'Cryin' Time'. Although the album showed that black soul and white country could be merged, Ray Charles lost his momentum, tending to cruise along on the same theme and never again writing a song to equal 'What'd I Say'.
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Intro - Account Settings (~30 seconds)
To get into Account Settings, make sure to click on the gear at the top right hand corner of the screen.
You'll also notice a gear next to Available Fields in the Kibana Discover tab. However, this is a different feature that we'll cover during our Search and Filtering training.


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Journal of Nanomaterials
Volume 2019, Article ID 6461493, 10 pages
Production of Methanol from Aqueous CO2 by Using Co3O4 Nanostructures as Photocatalysts
Facultad de Química, Universidad Nacional Autónoma de México, Avenida Universidad 3000, Ciudad Universitaria, Coyoacán, CP 04510 Mexico City, Mexico
Correspondence should be addressed to Salvador Pocoví-Martínez; email@example.com and David Diaz; xm.manu@divad
Received 18 June 2018; Accepted 2 October 2018; Published 9 January 2019
Academic Editor: Giuseppe Compagnini
Copyright © 2019 Salvador Pocoví-Martínez et al. This is an open access article distributed under the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.
In this work, we report for the first time the photocatalytic activity of Co3O4 nanostructures for the reduction of aqueous CO2 to methanol (MeOH). This could be considered a simple example of artificial photosynthesis. The photocatalysis experiments were developed under simulated solar light of 100 mW/cm2 and without using any sacrificial agent. To carry out this study, nanostructured mixed valence cobalt oxide (Co3O4) powders, with porous nanoparticle aggregates of different morphologies, have been prepared by two synthesis methods. The characterization of structural (PXRD, XPS, SEM, and TEM) and optical (UV-vis-NIR, Raman, and FT-IR) properties, magnetization curves, and surface area (BET) was accomplished.
1. Introduction
Global warming is the major issue that humanity has to face in the next 50 years. Some effects that could be devastating for humankind are the increase of global temperature, rise of sea level, extreme droughts, devastating floods, destructive storms, among others [1–5]. The reduction of gases that contribute to the Earth's surface warming can solve some problems that we are experiencing right now as the weather changes and the global temperature is rising. A great number of authors claim that the main cause of global warming is CO2 [6–9]. Almost all the excess of this gas in the atmosphere is produced by the combustion of mineral fuels, like gasoline or coal. Many efforts have been done in the last years aiming to reduce CO2 emissions to the atmosphere: imposition of taxes for CO2 emissions, CO2 sequestration using different methods [10–20], or the conversion of this gas using different techniques to obtain value added products, e.g., fuels [21–33]. In order to reduce CO2 quantity in the atmosphere and produce fuels using this gas and water, different materials and methods have been applied: metal complexes [21], microalgae [28, 33], syngas procedure [24], polymers [31], electrochemical transformations [26, 32], photothermal and thermochemical conversions [23, 25], semiconductors [27, 30], and several others.
One of the most attractive ways of producing fuels from CO2 and water is through photocatalytic semiconductor-mediated solar energy conversion. This fascinating fundamental and technological problem has challenged the scientific community for many years. A great variety of semiconductors, sometimes combined with metal nanostructures, carbon-based materials, and/or organometallic molecules have been tested with the mentioned purpose, and important progresses have been reached [34]. However, typical semiconductors with an adequate band gap for solar energy absorption (Si, CdSe, CdTe, GaAs, GaP, PbS, SbS, among others) are unstable in contact with electrolytes, and those with higher stability (TiO2, ZnO, SnO, ZnS, inter alia) cannot absorb a huge component of solar radiation [35]. A group of semiconductors, such as CuO, Fe2O3, or BiVO4, display both a wide spectral range of solar light absorption as well as stability when in contact with aqueous solutions of electrolytes. This last group of semiconductors has been largely studied in photocatalytic water splitting and/or CO2 photoreduction [36]. Another interesting semiconductor is Co3O4; it is stable in aqueous suspensions and oxygen-rich atmospheres and thus can be prepared and easily manipulated under usual laboratory conditions. This material has unique optical properties because it shows several band gaps in different regions of the electromagnetic spectrum (0.7–4.4 eV) [37–39]. Because it absorbs light in the UV, visible, and infrared regions, it can be a good candidate to carry out photocatalytic reactions when Co3O4 interacts with light. In addition, the preparation of different sizes and shapes of this material could potentially enhance the photocatalytic activity, since the optical properties may change and the area and surface defects of the material can increase with regard to its bulk counterpart. Despite the ad hoc properties of this material, only two studies have been reported regarding nanostructured Co3O4 as an active photocatalyst for CO2 reduction [40, 41]. Formic acid and formaldehyde were considered as major products for CO2 reduction assisted by randomly oriented Co3O4 nanocrystals [40], while formate was the only product using highly texturized {121} nanostructured Co3O4 [41]. However, Mendoza et al. [40] only used a small wavelength range in the visible spectrum (510 to 620 nm), neglecting the much wider absorption range (from UV to NIR) of this material. In the work of Huang et al. [41], the CO2 photocatalytic reduction was assisted by an external electric potential in a photoelectrochemical cell configuration, adding additional energy to that of the radiation. These reasons make it interesting to explore the possibilities that can be offered by an abundant, inexpensive, and stable material such as Co3O4 when it is only excited with solar light irradiation. Thus, here we report the properties of Co3O4. Herein, two different morphologies of this oxide were prepared based on synthesis procedures previously published. They were used as a heterogeneous catalyst for photochemical reactions with CO2 and H2O under artificial solar light irradiation, in order to evaluate their catalytic capabilities to generate hydrocarbons. In this work, the photocatalytic activity of Co3O4 (nanoparticles and porous structure) was evaluated for CO2 reduction in water and under visible light. The photocatalytic reactions were carried out in aqueous dispersions without the use of sacrificial agents, under normal conditions, i.e., room temperature and atmospheric pressure.
2. Experimental
2.1. Preparation of Co3O4 Nanoparticles (Co3O4-NPs) Photocatalyst
The synthesis of these nanoparticles was accomplished using an analogous method to that reported by Xie et al. [42]. Briefly, 1.19 g of CoCl2⋅6H2O (Mallinckrodt Pharmaceuticals, 99.63%) was added to 30 mL of ethylene glycol (EG) (Analytyka, 99.1%), and the suspension was stirred and gradually heated to 80°C. Then, 100 mL of a 0.2 M solution of Na2CO3 (Reproquifin, 99% min.) in deionized water (15 MΩ cm) was added dropwise and the mixture was further aged for 1 h under argon gas (Praxair, grade 4.8, extra pure, 99.998% min.). The purple solid obtained was filtered, washed several times with deionized water until neutralization, and dried overnight at 100°C under vacuum. The obtained purple powder was characterized using powder X-ray diffraction (PXRD) and infrared (IR) spectroscopy. As shown in Figure S1 it corresponds to cobalt hydroxycarbonate [43]. Finally, the solid was calcined for 4 h at 450°C, obtaining a black powder.
2.2. Preparation of a Porous and Nanostructured Co3O4 (Co3O4-P-NS) Photocatalyst
This sort of cobalt (II, III) oxide was synthesized using the gel-combustion method, similarly to that previously reported by Makhlouf et al. [44]. In our case, the quantities used were 1.46 g of Co(NO3)2⋅6H2O (Fermont, 99.6%) and 2.5 g of glycine (Sigma-Aldrich, 99%). Both powders were dissolved in 100 mL of deionized water under vigorous stirring. 3 mL of concentrated HNO3 (J. T. Baker, 65.8%) was added when both powders were completely dissolved, and the heating of this reaction mixture started at 300°C. A purple gel was formed when almost all the water was evaporated, and then the temperature was increased up to 400°C. Finally, the combustion of the organic material took place and a black solid was obtained. The PXRD pattern is shown in Figure S2. After that, the solid was calcined for 4 h at 700°C in order to obtain the final material.
2.3. Characterization Techniques of the Photocatalysts
PXRD patterns were taken on a Bruker D2-Phaser diffractometer equipment using Cu Kα radiation (10 mA, 30 kV, ) and an integration time of 0.5 s. Raman spectra were recorded with an EZRaman-N (Enwave Optronics Inc.) Raman analyzer coupled to a Leica DM300 microscope with a 40x objective, using an excitation laser source of 532 (∼30 mW) or 905 (∼160 mW) nm wavelengths. The infrared spectra were collected on a PerkinElmer Spotlight 400 FT-IR-FIR spectrometer with a Universal ATR sampling accessory. UV-visible-NIR electronic absorption spectra (under a diffuse reflectance regime) were recorded on a Varian Cary 5E, and the Kubelka-Munk function was computed. The transmission electron microscopy (TEM) micrograph and the selected area electron diffraction (SAED) pattern were obtained using a JEOL JEM-2012 microscope operating at a voltage of 200 kV. The scanning electron microscopy (SEM) images were obtained using a field-emission scanning electron microscope, JEOL JSM-5900-LV, operating at 20 kV. This microscope is equipped with an Oxford-ISIS for elemental analysis using energy-dispersive spectroscopy (EDS). The magnetic hysteresis loops (M–H) were measured in a vibrating sample magnetometer (VSM-LDJ 9600, 30,000 Oe) at room temperature with a standard magnetization curve routine. BET measurements were carried out by N2 at −196°C in a Quantacore Nova 2000. Before the physisorption, the samples were degassed for 12 h at 150°C. XPS was performed in a spectrometer equipped with an Al Kα X-ray source of 1486.6 eV. The analyzer energy was 23.5 eV and the base pressure was about 4.5 × 10−8 Pa.
2.4. Light Irradiation of CO2 Bubbled in Water in the Presence of a Photocatalyst
In a general procedure, 20 mL of deionized water in a Schlenk vessel were bubbled for 1 h with gaseous CO2 (Praxair, grade 3.0, 99.9%) in order to saturate water with CO2. Then, 4.15 × 10−2 mmol of a photocatalyst (Co3O4-NPs or Co3O4-P-NS) was suspended in the CO2 solution. A stirring bar was introduced, the glass vessel was sealed, and the irradiation was carried out with a 150 W arc xenon lamp (Osram XBO 150 W/CR OFR), which roughly simulates the solar spectrum. The lamp was located at a distance from the vessel so that 100 mW/cm2 of intensity was reached; a calibrated silicon photodiode (Thorlabs SM05PD2B) was used for that purpose. The experiments were accomplished at room temperature. After 6 hours of irradiation, the produced gases were collected in a Tedlar® bag and the resultant gaseous mixture was analyzed by gas chromatography (GC) in an Agilent 6890 series gas chromatograph with a 30-meter PerkinElmer PE-5 column ((5%-phenyl)-methylpolysiloxane). The temperature of the injector was 100°C, the oven was at 100°C, and the FID detector was at 150°C. Note that all the dispersions were prepared in deionized water. All the experiments were performed at least twice.
3. Results and Discussion
3.1. Characterization of Co3O4-NPs and Co3O4-P-NS
The powder diffraction pattern of the Co3O4-NP sample, displayed in Figure 1(a), agrees well with that of Co3O4 (PDF no. 42-1467). The synthesized nanoparticles have cubic symmetry and its space group is Fd-3m. In this material, the lattice is formed with mixed-valence cobalt: Co2+ (33%) and Co3+ (66%). It has a spinel structure where the atoms of Co2+ are in a tetrahedral coordination and the atoms of Co3+ are in an octahedral coordination with oxygen atoms. The average crystallite size of Co3O4-NPs estimated from the full width at half maximum of the (311) diffraction peak by applying the Scherrer equation is about 15 nm. The PXRD pattern of the prepared particles indicates the formation of the single spinel phase without any observable traces of cobalt hydroxide or cobalt monoxide. When Co3O4-P-NS was synthesized by combustion, the dark grey solid obtained was also analyzed by PXRD. A mixture of Co3O4, CoO, and Co was identified in the corresponding diffractogram (Figure S2). This is due to the presence of reducing and oxidizing species in the combustion reaction. The average crystallite size, obtained by the same method used for the Co3O4-NPs, was 21 nm. After the solid was calcined for 4 h at 700°C, as can be observed in Figure 1(b), the diffractogram only shows the Co3O4 cubic phase (PDF no. 42-1467) and its space group is Fd-3m. Due to the calcination process, the crystallite size increased to 45 nm. When the sample was annealed, the presence of Co and CoO was not detected, showing the formation of the single spinel phase. It is important to mention that the shape of the baseline in both diffractograms is due to the mathematical subtraction of the background, in order to remove the distortion produced by the fluorescence generated in the interaction of the Cu Kα radiation with the Co atoms.
The electronic absorption spectrum of Co3O4-NPs in the UV-visible-NIR region, using the diffuse reflectance mode displayed in Figure 2(a), shows different bands. Using Tauc's plot, different band gap energies were calculated. In the present study, the best fit of versus photon energy was obtained for for Co3O4-NPs, which corresponds to direct band gap transitions. Then, the obtained gap energy values for Co3O4-NPs were 0.78, 1.55, and 2.19 eV (see Figure 2(b)). The transition at 0.78 eV was recently attributed to a direct dipole-dipole forbidden d-d transition between the tetrahedral site of Co2+ cations [38]. The gaps at 1.55 and 2.19 eV are direct allowed transitions. These transitions are assigned to a charge transfer O2−➔Co3+ (the former) and a transition O2−➔Co2+ (the latter) [45–49]. The corresponding spectrum of Co3O4-P-NS in Figure 2(c) shows, as in the case of Co3O4-NPs, different direct band gap transitions. Using Tauc's plot, the calculated band gap energies for Co3O4-P-NS (Figure 2(d)) were 1.96, 1.48, and 0.76 eV. The band gap values found for the Co3O4-NP sample are slightly higher than those of the Co3O4-P-NS. This fact could be due to a small quantum confinement effect in the Co3O4-NPs [50, 51]; this is in accordance with the smaller crystallite size observed in the PXRD analysis. In addition, the colors of the two powders are different (Figure S5): the nanoparticles are black and the porous material is dark grey.
A representative SEM micrograph of the Co3O4-NP sample is shown in Figure 3(a). Considering the crystallite size obtained for this sample (15 nm), the observed microstructures in Figure 3(a) must be composed of "nanoblocks." In the SEM image of Co3O4-P-NS (Figure 3(b)), large nanostructured arrays (crystallite size about 45 nm) with different pore sizes are observed. In this sample, the size of the observed pores are in the order of microns; this can be due to the high volume of gases produced during the combustion reaction [44].
It is clearly revealed in the TEM micrograph of Figure 4 that the microstructures observed in Figure 3(a) are in fact Co3O4-NP porous agglomerates with a size in the order of submicrons. The corresponding pore sizes are in the range of 5–15 nm. These nanoparticles are agglomerated and have a rectangular shape and a mean size of 15.1 ± 3.6 nm (Figure S12). This value fairly matches the crystallite size found from the PXRD analysis.
For more details about the composition and structural characterization of the materials, see the supplementary materials.
3.2. Photocatalytic CO2 Reduction
After characterization, the materials were dispersed in CO2-saturated water and irradiated. The purpose of our work was to evaluate the catalytic activity of the catalysts under normal conditions of temperature, pressure, and quantity of CO2 determined by the solubility of the gas in water at atmospheric pressure. The reader can find elsewhere [52] more information about the different equilibria related to the solubility of CO2 in water at different pH values; thus, the starting pH of the reaction solution was between 4.5 and 5. It is important to note that no sacrificial agent was used in the reaction. The collected gases were analyzed with a gas-chromatograph with a FID detector. Figure 5(a) shows the sharp band of the gas obtained after irradiation of the reaction suspension containing either Co3O4-NPs or Co3O4-P-NS. These peaks matched well with those corresponding to the methanol standard. As can be seen, the gas obtained with the two materials is the same, since the signal appears at the same retention time as that of methanol. Though this material has been widely used for water splitting and water oxidation, this is the first time MeOH production is reported when Co3O4 is used as a photocatalyst in a system as described herein. It is noteworthy that the reaction product obtained here is different from those reported in the two previous works using Co3O4 as a photocatalyst, which at the same time are different from each other [40, 41]. This apparent discrepancy may be explained, since different excitation conditions were used in every report: (i) In the work of Mendoza et al. [40], the irradiation was carried out using a small window of the visible spectrum (510 to 620 nm); the light intensity in the reaction medium was not reported. (ii) In the report of Huang et al. [41], a Xe lamp was used to irradiate the reaction system at an intensity of 9 mW/cm2 and the photoelectrode was polarized at 0.9 V (vs. SCE) during the experiments. (iii) In our case, the intensity of the irradiation in the reaction system was 100 mW/cm2, coming from a Xe arc lamp typically used in solar simulators. These different excitation conditions, together with slightly different light absorption capabilities, cause different concentrations of photogenerated carriers, different Fermi level positions, and consequently, different potential distributions across the semiconductor/electrolyte interface [53]. Thus, different reactions could be expected. The exposed planes of the materials could make a difference too, with regard to the photocatalytic activity. It is well known that the plane (110) mainly contains Co3+ ions in an octahedral coordination that are good for the oxidation of, e.g., CO and alcohols [42, 54, 55]. Also, the planes (001) and (111) mainly contain Co2+ ions in a tetrahedral coordination that are almost inactive for the oxidation [56–58]. It is worth saying that the plane (111) is the one that we found in the HR-TEM images. Other possible reasons, like different relative band positions, different electrolyte compositions affecting the redox equilibrium, and different Co3O4 crystalline textures affecting the corresponding surface activities, cannot be discarded.
For the products obtained in this work, the signals obtained were used by means of qualitative detection, not for quantitative purposes, due to the fact that very small amounts of them were obtained in these studies [59, 60]. Attempts to fully characterize MeOH in the remnant solution were unsuccessful due to the lower amounts of gas produced. The fact that methanol was detected as a gas and none was detected in the remnant solution is not surprising. This is probably due to the fact that the methanol produced in the reaction evaporated, since the reaction solution reaches 35°C upon irradiation and atmospheric pressure in our room conditions is 585 mm Hg. A possible general mechanism explaining the photoreduction of CO2 and the production of methanol can be seen in Figure 5(b). As it is well known, the reduction of CO2 to methanol needs protons and electrons. In our experimental conditions, there are two possible proton sources: (1) the oxidation of water with Co3O4 and the production of H+ [61] and (2) the dissociation equilibrium of H2CO3/HCO3− [62, 63]. For the initial pH values encountered in the solution reaction (4.5–5), the expected species are CO2(aq), H2CO3, and a small quantity of HCO3− in equilibrium with the carbonic acid. In the literature, it is reported that the concentration of CO2(aq) in a solution is approximately 500 times the concentration of H2CO3 in standard reaction conditions [63]. As mentioned above, the pH determines the species you can find and their concentration in the solution. That is, the concentration of H2CO3 in a solution is from 23 to 71 times greater than the concentration of HCO3−; consequently, the concentration of CO2(aq) is from 11,500 to 35,500 times larger than the concentration of HCO3− (the calculations are developed in Appendix A of the supporting information). Considering the different carbon-containing species present in the reaction medium and their corresponding potential reduction (see Figure 6), we suggest that at least two pathways in the formation of methanol are possible. One path is where CO2(aq) is combined with protons and photogenerated electrons to produce methanol, and the other path is where carbonic acid is combined with protons and reduced to give MeOH. In terms of the concentration of the two species, the former pathway is favored because the concentration of CO2(aq) is 500 higher than that of the H2CO3 in solution; however, in thermodynamic terms, the second path is preferred because the reduction potential of the H2CO3/CH3OH pair is more positive than that of CO2/CH3OH (Figure 6). We do not have enough experimental evidences to establish which of these two possible mechanisms has a higher contribution.
For the Co3O4-NPs, the highest direct gap energy transition is 2.19 eV, while that of Co3O4-P-NS is 1.96 eV. In Figure 6, the redox potentials of different possible products are shown. Taking into account the band gap obtained for our materials, methanol production, and possible water oxidation [61], it is possible to assume that the conduction band could be more reductive than the redox potential of the CO2/CH3OH pair and the valence band might be more oxidizing than the oxidation potential of the water.
By preparing two different morphologies of Co3O4, it was expected to obtain different products, quantities, or both. Nevertheless, no significant differences were observed between the two morphologies regarding their photocatalytic behavior. It is important to mention that CO32− anions are not formed in the pH range of our experiments. At the end of the experiment, the pH of the remnant solution was 7, which means that the concentration of dissolved CO2 (or the H2CO3/HCO3− pair) significantly decreased in the solution.
Once the reaction was completed, the materials were collected with a centrifuge and dried in a vacuum oven at 80°C overnight. After that, the PXRD of the two materials were recorded again (Figure S16(a) and S16(b)). When the average size of a crystallite was calculated for Co3O4-NPs, it increased from 19 nm to 21 nm. For Co3O4-P-NS, the crystallite size increased from 45 nm to 51 nm. Considering that the smallest particles could be retained in the final reaction solution, the increase of the crystallite was not significant in the two cases. In addition, no signal of cobalt hydroxides or carbonates was observed, so the materials did not change in composition or in size by means of PXRD. No changes were observed in their Raman spectrum either (Figure S16(c) and S16(d)). These results indicate that no significant changes in the structure of the catalysts were produced after the first cycle. Moreover, the optical properties remained unaltered (not shown).
The reaction was carried out again under the same conditions as the experiment mentioned above, using the recovered catalytic materials. Even more interesting was to corroborate that those materials conserved their activity for the reduction of CO2. As can be seen in Figure 7, the chromatograms revealed that methanol was obtained again with the reutilized materials.
After the second cycle, we tried to recover the catalysts in order to characterize the structural and optical properties to evaluate possible changes, but we did not succeed. The solids remained stuck on the walls of the reactor.
It is worth mentioning that the viability of these catalysts for long-term use is still under investigation.
4. Conclusions
We have an unprecedented report of methanol production using a photocatalytic system with a very simple architecture working under ordinary reaction conditions. Co3O4 nanostructures showed photocatalytic activity in the CO2 reduction process, and methanol is the only detected reaction product. It is possible to assert that this is a simple example of artificial photosynthesis. Co3O4 has been widely used for water splitting and water oxidation, but this is the first time MeOH production is reported when this material is used as a photocatalyst.
Co3O4-NPs and Co3O4-P-NS were satisfactorily synthesized by adding changes to two reported methods. No impurities were detected in the synthesized Co3O4-P-NS powder. A small quantum confinement was found for the two samples compared with the bulk material, being higher for Co3O4-NPs. No significant differences were observed between the two reported morphologies regarding the photocatalytic behavior.
Data Availability
The data used to support the findings of this study are included within the article and the supplementary information files.
Inti Zumeta-Dube's current address is Centro de Investigación en Ciencia Aplicada y Tecnología Avanzada, Unidad Legaria, Instituto Politécnico Nacional, Calzada Legaria No. 694, Col. Irrigación, Del. Miguel Hidalgo, CP 11500, México D.F., Mexico.
Conflicts of Interest
The authors declare that there is no conflict of interest regarding this publication of this paper.
This research has received partial funding from the European Community's Seventh Framework Programme (FP7-NMP-2010-EU-MEXICO) and CONACYT (BisNano), under Grant Agreement nos. 263878 and 125141, respectively. Inti Zumeta-Dube is grateful to CONACYT (project number 174247), ICyTDF, BisNano, and the project CM-SECITI/095/2017 "Planta piloto sustentable operada con energía solar para el tratamiento de agua pluvial de la CDMX" for the postdoctoral fellowship. Salvador Pocoví-Martínez is thankful for the postdoctoral fellowship from DGAPA-UNAM. David Diaz thanks DGAPA-UNAM (IN115212 and IN116214 PAPIIT projects) and CONACYT (Redes193850 and SEP-CB-132094 projects) for the financial support. The authors want to thank Dr. Edilso Reguera-Ruiz (CICATA-U Legaria, IPN), Dr. Aida Gutiérrez Alejandre (FQ-UNAM), and Dr. Tobías Noel Nava-Entzama (IMP) for the access to several instrumental facilities.
Supplementary Materials
Figure S1: (a) XRD pattern and (b) IR spectrum of CoCO3(OH)2. Figure S2: XRD pattern of the black solid after combustion. Figure S3: Raman spectra recorded using a wavelength excitation laser source of 532 nm for (a) Co3O4-NPs and (b) Co3O4-P-NS. Figure S4: IR spectra of (a) Co3O4-NPs and (b) Co3O4-P-NS. Figure S5: pictures of (a) Co3O4-NPs and (b) Co3O4-P-NS powders. Figure S6: EDS spectra of (a) Co3O4-NPs and (b) Co3O4-P-NS. Figure S7: SEM images of Co3O4-NPs. Figure S8: SEM images of Co3O4-NPs. Figure S9: SEM images of Co3O4-NPs. Figure S10: (a) HR-TEM, (b) FFT of the framed region, and (c) reciprocal lattice of 2 different zones of Co3O4-NPs. Figure S11: (a) SAED pattern and (b) unit cell representation of Co3O4-NPs. Figure S12: size distribution of Co3O4-NPs. Figure S13: magnetization curve of (a) Co3O4-NPs and (b) Co3O4-P-NS. Figure S14: XPS of Co3O4-NPs: (a) wide-range spectra and high-resolution spectra of (b) Co2p, (c) C1s, and (d) O1s. Figure S15: isotherm plot for adsorption-desorption of (a) Co3O4-NPs and (c) Co3O4-P-NS; BET surface area plot of (b) Co3O4-NPs and (d) Co3O4-P-NS. Figure S16: XRD patterns and Raman spectrum after photocatalytic reaction of (a, c) Co3O4-NPs and (b, d) Co3O4-P-NS. Appendix A: calculation of the different concentration relations of species in solution. (Supplementary Materials)
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Ground Rules for Grade-Level Decks | Professional Deck Builder .,May 31, 2017 . Breyer Construction & Landscape A low deck can be a cost-effective alternative to hardscaping, especially when the framing for a shade structure can be factored into the design. .. If the decking is close to the ground, be sure to follow the manufacturers' guidelines, to prevent performance problems
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text: Bgosnell151 1,097 Report post Posted February 11 Nope, still not sweet. But I decided to create a stew using beef broth, red wine, and worcestshire sauce. Wifey was more than pleasantly surprised with the outcome. Also had some wings in for my appetizer. 9 Rob_grill_apprentice, Red River Smoke, KismetKamado and 6 others reacted to this Share this post Link to post Share on other sites


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