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    • 2018-11-26 10:05:22
    • Article ID: 704352

    Light-Activated, Single-Ion Catalyst Breaks Down Carbon Dioxide

    X-ray studies reveal structural details that may point the way to designing better catalysts for converting pollutant gas into useful products

    • National Synchrotron Light Source II (NSLS-II) QAS beamline scientist Steven Ehrlich, Stony Brook University (SBU) graduate student Jiahao Huang, and Brookhaven Lab-SBU joint appointee Anatoly Frenkel at the QAS beamline at NSLS-II.

    • Credit: University of New Hampshire

      Gonghu Li, lead author on the study

    • Schematic of a single-site catalyst in which single cobalt ions (Co2+) supported on a graphitic carbon nitrogen layer (C3N4) reduce carbon dioxide (C02) to carbon monoxide (CO) in the presence of visible light (red wavy arrow). If cobalt were bound with oxygen to form a cobalt oxide (CoOx), the reaction would not proceed.

    UPTON NY – A team of scientists has discovered a single-site, visible-light-activated catalyst that converts carbon dioxide (CO2) into “building block” molecules that could be used for creating useful chemicals. The discovery opens the possibility of using sunlight to turn a greenhouse gas into hydrocarbon fuels.

    The scientists used the National Synchrotron Light Source II, a U.S. Department of Energy (DOE) Office of Science user facility at Brookhaven National Laboratory, to uncover details of the efficient reaction, which used a single ion of cobalt to help lower the energy barrier for breaking down CO2. The team describes this single-site catalyst in a paper just published in the Journal of the American Chemical Society.

    Converting CO2 into simpler parts—carbon monoxide (CO) and oxygen—has valuable real-world applications. “By breaking CO2, we can kill two birds with one stone—remove CO2 from the atmosphere and make building blocks for making fuel,” said Anatoly Frenkel, a chemist with a joint appointment at Brookhaven Lab and Stony Brook University. Frenkel led the effort to understand the activity of the catalyst, which was made by Gonghu Li, a physical chemist at the University of New Hampshire.

    “We now have evidence that we have made a single-site catalyst. No previous work has reported solar CO2 reduction using a single ion,” said Frenkel.

    Breaking the bonds that hold CO2 together takes a lot of energy and a long time. So, Li set out to develop a catalyst to lower the energy barrier and speed up the process.

    “The question is, between several possible catalysts, which are efficient and practical to implement in industry?” said Frenkel.

     

    One key ingredient required to break the bonds of CO2 is a supply of electrons. These electrons can be generated when a material known as a semiconductor gets activated by energy in the form of light. The light “kicks” electrons out, so to speak, making them available to the catalyst for chemical reactions. Sunlight could be a natural source of such light. But many semiconductors can only be activated by ultraviolet light, which makes up less than a five percent of the solar spectrum.

    “The challenge is to find another semiconductor material where the energy of natural sunlight will make a perfect match to kick out the electrons,” Frenkel said.

    The scientists also needed the semiconductor to be bound to a catalyst made from materials that could be found abundantly in nature, rather than rare, expensive metals such as platinum. And they wanted the catalyst to be selective enough to drive only the reaction that converts CO2 to CO.

    “We don’t want the electrons to be used for reactions other than reducing CO2,” Frenkel said.

    Cobalt ions bound to graphitic carbon nitride (C3N4), a semiconductor made of carbon, nitrogen, and hydrogen atoms, ticked all the boxes for these requirements.

    “There has been significant interest in using C3N4 as a metal-free semiconductor to harvest visible light and drive chemical reactions,” said Li. “Electrons generated by C3N4 under light irradiation have energy high enough to reduce CO2. Such electrons often don’t have lifetimes long enough to allow them to travel to the semiconductor surface for use in chemical reactions. In our study, we adopted a common and effective strategy to build up enough energetic electrons for the catalyst by using a sacrificial electron donor. This strategy allowed us to focus on the catalysis for CO2 reduction. Ultimately, we want to use water molecules as the electron donor for our catalysis,” he added.

    Peipei Huang, a postdoctoral researcher in Li’s lab, made the catalyst by simply depositing cobalt ions on a C3N4 material made from commercially available urea. The team then extensively examined the synthesized catalyst using a variety of techniques in collaboration with Christine Caputo at the University of New Hampshire and Ronald Grimm at Worcester Polytechnic Institute.

    The catalyst worked in CO2 reduction under visible-light irradiation.

    “This catalyst did what it was supposed to do—break down CO2 and make CO with very good selectivity in visible light,” Frenkel said. “But the next goal was to see why it worked. If you can understand why it works you can make new and better materials based on those principles.”

    So Frenkel and Li brainstormed experiments that would show the structure of the catalyst with precision. Structural studies would give the scientists information about the number of cobalt atoms, their location relative to the carbon and nitrogen atoms, and other characteristics the scientists could potentially adjust to try to improve the catalyst further.

    They turned to the Quick x-ray Absorption and Scattering (QAS) beamline at NSLS-II to use x-ray absorption spectroscopy. With help from lead beamline scientist Steven Ehrlich, Frenkel’s student Jiahao Huang took the data and analyzed the spectra.

    In this technique, the x-rays from NSLS-II get absorbed by atoms in the sample, which then eject waves of electrons. The spectra show how these electron waves interact with surrounding atoms, similar to the way ripples on the surface of a lake get disrupted when they encounter rocks.

    “To be able to do x-ray absorption spectroscopy (XAS), we need to tune and scan the energy of the x-ray beam hitting the sample,” said Ehrlich. “Each element can absorb x-rays at distinct energies, called absorption edges. At the new QAS beamline we can scan the energy of the x-rays across the absorption edge energy of different elements, such as cobalt in this case. We then measure the number of photons absorbed by the sample for each value of the x-ray energy.”

    In addition, Frenkel explained, “each type of atom produces a different kind of electronic ripple, when excited by x-rays, or when hit by other ripples, so the x-ray absorption spectrum tells you what the surrounding atoms are as well as how far apart and how many there are.”

    The analysis showed that the catalyst breaking down CO2 was made of single ions of cobalt surrounded on all sides by nitrogen atoms.

    “There were no cobalt-cobalt pairs. So, this was evidence that they were in fact single atoms of cobalt dispersed on the surface,” Frenkel said.

    “This data also narrows down the possible structural arrangements, which provides information for theorists to fully evaluate and understand the reactions,” Frenkel added.

    Though the science outlined in the paper is not yet in practical use, there are abundant possibilities for applications, Frenkel said. In the future, such single-site catalysts could be used in large-scale areas with abundant sunlight to break down excess CO2 in the atmosphere, similar to the way plants break down CO2 and reuse its building blocks to build sugars in the process of photosynthesis. But instead of making sugars, scientists might use the CO building blocks to generate synthetic fuels or other useful chemicals.

    This research was supported by the DOE Office of Science and partly by the National Science Foundation.

    Brookhaven National Laboratory is supported by the Office of Science of the U.S. Department of Energy. The Office of Science is the single largest supporter of basic research in the physical sciences in the United States, and is working to address some of the most pressing challenges of our time. For more information, please visit science.energy.gov.

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    Defining Quality Virus Data(sets)

    In Nature Biotechnology, as more and more researchers continue to assemble new genome sequences of uncultivated viruses, researchers at the U.S. Department of Energy (DOE) Joint Genome Institute (JGI) led a community effort to develop guidelines and best practices for defining virus data quality.

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    Distortion of water droplet surface may increase the likelihood of the droplet freezing.

    Future Loss of Arctic Sea-Ice Cover Could Contribute to the Substantial Decrease in California's Rainfall

    A new modeling framework helps understand the consequences of future sea-ice loss in the Arctic.

    Tangled magnetic fields power cosmic particle accelerators

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    Argonne scientists maximize the effectiveness of platinum in fuel cells

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    Drawn into a Whirlpool: A New Way to Stop Dangerous Fast Electrons in a Fusion Device

    A new phenomena forms vortices that trap particles, impeding electron avalanches that harm fusion reactors.

    Barely scratching the surface: A new way to make robust membranes

    Argonne researchers have demonstrated a new technique's viability for membranes.

    During Droughts, Bacteria Help Sorghum Continue Growing

    Researchers discover how certain bacteria may safeguard plant growth during a drought, making way for strategies to improve crop productivity.

    Sierra Snowpack Could Drop Significantly By End of Century

    A future warmer world will almost certainly feature a decline in fresh water from the Sierra Nevada mountain snowpack. Now a new study by Lawrence Berkeley National Laboratory that analyzed the headwater regions of California's 10 major reservoirs, representing nearly half of the state's surface storage, found they could see on average a 79 percent drop in peak snowpack water volume by 2100.

    The Biermann Battery Effect: Spontaneous Generation of Magnetic Fields and Their Severing

    The mechanism responsible for creating intense magnetic fields in laser-driven plasmas also helps tear the fields apart.


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    DOE approves technical plan and cost estimate to upgrade Argonne facility; Project will create X-rays that illuminate the atomic scale, in 3D

    The U.S. Department of Energy has approved the technical scope, cost estimate and plan of work for an upgrade of the Advanced Photon Source, a major storage-ring X-ray source at Argonne.

    Costas Soukoulis elected to National Academy of Inventors

    Costas Soukoulis, Ames Laboratory senior scientist and Iowa State University Frances M. Craig Endowed Chair and Distinguished Professor, has been named as a 2018 National Academy of Inventors (NAI) Fellow.

    Biophysicist F. William Studier Elected Fellow of the National Academy of Inventors

    F. William Studier, a Senior Biophysicist Emeritus at the U.S. Department of Energy's Brookhaven National Laboratory and Adjunct Professor of Biochemistry at Stony Brook University, has been elected as a Fellow of the National Academy of Inventors (NAI). He is among 148 renowned academic inventors being recognized by NAI for 2018.

    Blast to the future

    A grant from DOE's Technology Commercialization Fund will help researchers at Argonne and industry partners seek improvements to U.S. manufacturing by making discovery and design of new materials more efficient.

    Department of Energy to Provide $24 Million for Computer-Based Materials Design

    The U.S. Department of Energy (DOE) announced plans to provide $24 million in new and renewal research awards to advance the development of sophisticated software for computer-based design of novel materials.

    Argonne scientists recognized for decades of pioneering leadership in research

    Argonne scientists Ali Erdemir and Jack Vaughey were named 2018 Fellows of the American Association for the Advancement of Science (AAAS).

    Kurfess, Smith join ORNL to lead advanced manufacturing initiatives

    Two leaders in US manufacturing innovation, Thomas Kurfess and Scott Smith, are joining the Department of Energy's Oak Ridge National Laboratory to support its pioneering research in advanced manufacturing.

    Four Berkeley Lab Scientists Named AAAS Fellows

    Four Berkeley Lab scientists - Allen Goldstein, Sung-Hou Kim, Susannah Tringe, and Katherine Yelick - have been named Fellows of the American Association for the Advancement of Science, the world's largest general scientific society.

    U.S. Department of Energy to Host Nationwide CyberForce Competition(tm) December 1

    Students from dozens of colleges/universities will participate in the U.S. Department of Energy's CyberForce Competition(tm) this weekend

    Seven ORNL researchers named 2019 INCITE award winners

    Seven researchers from the Department of Energy's Oak Ridge National Laboratory have been chosen by the Innovative and Novel Computational Impact on Theory and Experiment, also known as INCITE, program to lead scientific investigations that require the nation's most powerful computers. The ORNL-based projects span a broad range of the scientific spectrum and represent the potential of high-performance computing in ensuring America's scientific competitiveness and energy security.


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    Ice Formed by Contact Freezing: Pressure Matters, Not Just Temperature

    Distortion of water droplet surface may increase the likelihood of the droplet freezing.

    Future Loss of Arctic Sea-Ice Cover Could Contribute to the Substantial Decrease in California's Rainfall

    A new modeling framework helps understand the consequences of future sea-ice loss in the Arctic.

    Drawn into a Whirlpool: A New Way to Stop Dangerous Fast Electrons in a Fusion Device

    A new phenomena forms vortices that trap particles, impeding electron avalanches that harm fusion reactors.

    During Droughts, Bacteria Help Sorghum Continue Growing

    Researchers discover how certain bacteria may safeguard plant growth during a drought, making way for strategies to improve crop productivity.

    The Biermann Battery Effect: Spontaneous Generation of Magnetic Fields and Their Severing

    The mechanism responsible for creating intense magnetic fields in laser-driven plasmas also helps tear the fields apart.

    Subtlety and the Selective Art of Separating Lanthanides

    Unexpected molecular interactions involving water clusters have a subtle, yet profound, effect on extractants picking their targets.

    Review Examines the Science and Needs of Nitrogen-Based Transformations

    Advances in biochemistry and catalysis could lead to faster, greener nitrogen-rich fertilizer.

    Quickly Capture Tiny Particles Reacting

    New method takes a snapshot every millisecond of groups of light-scattering particles, showing what happens during industrially relevant reactions.

    New Technology Consistently Identifies Proteins from a Dozen Cells

    A new platform melding microfluidics and robotics allows more in-depth bioanalysis with fewer cells than ever before.

    Optimal Foraging: How Soil Microbes Adapt to Nutrient Constraints

    How microbial communities adjust to nutrient-poor soils at the genomic and proteomic level gives scientists insights into land use.


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