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    • 2018-06-05 15:50:23
    • Article ID: 695645

    Exploring Greener Approaches to Nitrogen Fixation

    A fundamental understanding of nitrogen chemistry could lead to more sustainable routes for producing nitrogen-containing commodities such as fertilizers and nitric acid

    • Credit: Brookhaven National Laboratory

      Brookhaven Lab chemists Jingguang Chen (left) and Sergei Lymar were among the experts in nitrogen research who gathered in October 2016 at a U.S. Department of Energy–sponsored workshop, the conclusions of which were recently published in the journal Science.

    • Credit: National Science Foundation

      Nitrogen fixation occurs naturally in bacteria containing the nitrogenase enzyme and can be carried out artificially through a high-temperature and high-pressure industrial process that relies on iron-based catalysts and large quantities of hydrogen obtained from natural gas.

    • Credit: Brookhaven National Laboratory

      There are several possible routes for transforming nitrogen gas (N2), ammonia (NH3), and nitrogen oxides (NOy) that eliminate or minimize the need for fossil fuels. Nitrogenase enzymes, like those found in bacteria; different types of catalysts; and nonthermal plasmas consisting of ions, electrons, and excited molecules are among the possibilities that scientists are investigating.

    About half of the nitrogen in our bodies today comes from bacteria via the enzyme nitrogenase, which converts, or “fixes,” unreactive nitrogen gas in the atmosphere into a form that plants can use for growth. The other half is produced artificially through an energy-intensive industrial process developed more than 100 years ago. This process, called Haber-Bosch (H-B) after the two chemists who developed it, produces ammonia by using iron-based catalysts to promote the reaction of nitrogen from the air and hydrogen derived primarily from methane. Through another chemical process (Ostwald), the ammonia gets oxidized (reacts with oxygen) to produce nitric acid—a key fertilizer ingredient.

    While the H-B process revolutionized our ability to grow food, it is largely driven by the use of fossil fuels, consuming about two percent of global energy. It also massively contributes to greenhouse gas emissions, releasing two percent of global carbon dioxide.

    A roadmap for nitrogen chemistry research

    Finding more environmentally and energy-friendly routes for transforming nitrogen will require the development of new catalysts to speed up the chemical reactions and renewable energy sources to drive these reactions. In October 2016, the U.S. Department of Energy (DOE) Office of Science sponsored a two-day workshop for national lab and university scientists with the relevant expertise to focus on the challenges and opportunities of nitrogen activation. A review article, primarily based on presentations and discussions from this workshop, was published on May 25 in the journal Science.

    “The article provides a roadmap for fundamental research on nitrogen transformation reactions,” said first and co-corresponding author Jingguang Chen, a senior chemist at DOE’s Brookhaven National Laboratory and the Thayer Lindsley Professor of Chemical Engineering at Columbia University. “Many of these reactions can occur under relatively mild conditions—without the high temperatures or pressures required in H-B—but the challenge is to identify catalysts that are active, selective, and stable.” Chen; co-corresponding author Richard Crooks, the Robert A. Welch Chair in Materials Chemistry at The University of Texas at Austin; and Lance Seefeldt, a professor in the Department of Chemistry and Biochemistry at Utah State University, jointly proposed the topic and co-chaired the workshop. 

    Research on alternative routes for nitrogen transformation without the use of fossil fuels as the energy source begins with an analysis of thermodynamics. In order for nitrogen gas to be reduced or oxidized, the very stable triple bond that tightly holds the two nitrogen atoms together must be broken.

    “Before trying to find new catalysts with the appropriate properties, we need to determine if the reaction pathways of the alternative routes are energetically feasible,” explained co-author and Brookhaven Lab chemist Sergei Lymar. “Many thermodynamically feasible routes do exist, but they have largely been overlooked for the past 100 years because H-B has been so successful. While there is no guarantee that we will be able to run these reactions on a large scale, the thermodynamic calculations provide us with a starting point from which we can screen potential catalytic materials.”

    Possible routes for transforming nitrogen   

    The Science article describes several alternative processes for oxidative and reductive nitrogen transformations. On the reduction side, one possibility is to replace methane with water as the hydrogen source in the H-B process. A catalyst could split water into hydrogen and oxygen, using energy generated by solar panels or wind turbines. Another idea is to eliminate the H-B process altogether, instead directly producing ammonia in electrochemical cells with electrocatalysts or photocatalysts (light-responsive materials) at the electrodes. The cells could be powered by renewable energy or even nitrogen-fixing bacteria.

    "Electrochemical transformations are intrinsically clean," said Crooks. "But the limited amount of research that has been directed toward the electrochemistry of nitrogen has really not even established a clear direction for future investigations."

    Scientists are also trying to understand how nitrogenase works at low temperatures and pressures and without hydrogen gas. If they can mimic the function of this enzyme, they could design new molecular nitrogen-reduction catalysts that operate under less-harsh conditions than those of H-B.

    Such sustainable approaches would enable ammonia to be produced in a distributed manner rather than through the centralized H-B facilities currently in place. This distributed production is especially important in developing countries that are facing rapid population growth but do not have enough capital to build large chemical plants and the infrastructure to transport fertilizers. If solar panels are installed near farming fields, for example, the energy from sunlight could create the energetic electrons required for reducing nitrogen to ammonia, if appropriate catalysts are available.

    On the oxidation side, scientists are investigating the direct reaction between nitrogen and oxygen gas to produce nitric acid. Nearly all of the 50 million tons of nitric acid produced annually is manufactured indirectly through the Ostwald process by the oxidation of H-B-generated ammonia.

    “The current way nitric acid is produced is kind of backwards from an electron flow point of view,” said Lymar. “First, nitrogen is reduced all the way to ammonia and then ammonia is oxidized all the way to nitric acid, spanning all of nitrogen’s eight oxidation states. It would be more practical to directly oxidize nitrogen with oxygen, but this reaction becomes spontaneous only at extreme temperatures.”

    One idea to overcoming this problem is to oxidize nitrogen in low-temperature, nonthermal plasmas—weakly ionized gases that contain “hot” energetic electrons and near-room-temperature molecules, atoms, and ions. By vibrationally exciting nitrogen molecules, nonthermal plasmas could help catalysts accelerate the oxidation reaction.

    The article also describes approaches to reduce air-polluting nitrogen oxides. These gases are produced when nitrogen and oxygen react during combustion. The exhaust from vehicles is a major source of nitrogen oxides, which contribute to the formation of smog and acid rain. Certain bacteria have enzymes that reduce nitrogen oxides to nitrogen gas, and these denitrifying bacteria will likely be a source of inspiration for scientists seeking to design new catalysts for environmental protection.

    “Progress in any of these areas will require a molecular-level understanding of natural and artificial nitrogen transformation reactions,” said Chen. “The goal of this article is to provide directions for basic research, hopefully leading to the development of simple, low-energy routes for manipulating the redox states of nitrogen.”   

    The workshop was organized by the Council on Chemical Sciences, Geosciences, and Biosciences, convened by the Chemical Sciences, Geosciences, and Biosciences Division of the Office of Basic Energy Sciences within DOE’s Office of Science. 

    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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    A Challenging Future for Tropical Forests

    Mortality rates of moist tropical forests are on the rise due to environmental drivers and related mechanisms.

    Stronger, lighter, greener

    A new award-winning magnet technology invented at the U.S. Department of Energy's Argonne National Laboratory could help drive the nation's transition from gas-powered vehicles to electric and hybrid power more rapidly, at lower cost, and in a more environmentally friendly way.

    Science Up-Close: Developing a Cookbook for Efficient Fusion Energy

    To develop a future fusion reactor, scientists need to understand how and why plasma in fusion experiments moves into a "high-confinement mode" where particles and heat can't escape. Scientists at the Department of Energy's Princeton Plasma Physics Laboratory simulated the transition into that mode starting from the most basic physics principles.

    Peering into the Mist: How Water Vapor Changes Metal at the Atomic Level

    New insights into molecular-level processes could help prevent corrosion and improve catalytic conversion.

    Neutron science publications reach new highs at ORNL's flagship facilities

    The High Flux Isotope Reactor and the Spallation Neutron Source at the Department of Energy's Oak Ridge National Laboratory have reached new levels of increased science productivity. In 2018, a record high of more than 500 scientific instrument publications were produced between HFIR and SNS--based on neutron beamline experiments conducted by more than 1,200 US and international researchers who used the world-leading facilities.

    Fiery sighting: A new physics of eruptions that damage fusion experiments

    Feature describes first direct sighting of a trigger for bursts of heat that can disrupt fusion reactions.

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    Scientists discover key types of microbes that degrade organic matter and release carbon dioxide and methane into the atmosphere.

    An effect that Einstein helped discover 100 years ago offers new insight into a puzzling magnetic phenomenon

    Experiments at the Department of Energy's SLAC National Accelerator Laboratory have seen for the first time what happens when magnetic materials are demagnetized at ultrafast speeds of millionths of a billionth of a second: The atoms on the surface of the material move, much like the iron bar did. The work, done at SLAC's Linac Coherent Light Source (LCLS) X-ray laser, was published in Nature earlier this month.

    Found: A precise method for determining how waves and particles affect fusion reactions

    Like surfers catching ocean waves, particles within plasma can ride waves oscillating through the plasma during fusion energy experiments. Now a team of physicists led by PPPL has devised a faster method to determine how much this interaction contributes to efficiency loss in tokamaks.

    Discovery adapts natural membrane to make hydrogen fuel from water

    In a recent study from the U.S. Department of Energy's (DOE) Argonne National Laboratory, scientists have combined two membrane-bound protein complexes to perform a complete conversion of water molecules to hydrogen and oxygen.


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    Journal Special Issues Honor Chemists Radoslav Adzic and Jan Hrbek

    The Journal of the Electrochemical Society and Surface Science recognized the contributions of Brookhaven Lab chemists Radoslav Adzic and Jan Hrbek to electrocatalysis and catalysis.

    Argonne scientist elected as SAE Fellow

    Scientist Michael Wang from the U.S. Department of Energy's (DOE) Argonne National Laboratory was recently inducted as a Fellow of the professional engineering organization SAE (Society of Automotive Engineers). The organization reserves this prestigious grade of membership for thosewho have made significant contributions to mobility technology and have demonstrated leadership in their field.

    Top 10 Discoveries of 2018

    Every year, the U.S. Department of Energy's (DOE) Brookhaven National Laboratory compiles a list of the biggest advances made by the Lab's staff scientists, engineers, and visiting researchers. From uncovering mysteries of the universe to building better batteries, here, in no particular order, are our picks for the top 10 discoveries of 2018.

    U.S. Department of Energy Announces $33 Million for Small Business Research and Development Grants

    The U.S. Department of Energy announced it will award 189 grants totaling $33 million to 149 small businesses in 32 states.

    DOE to Provide $16 Million for New Research into Atmospheric and Terrestrial Processes

    The U.S. Department of Energy (DOE) announced a plan to provide $16 million for new observational research aimed at improving the accuracy of today's climate and earth system models.

    Machine learning award powers Argonne leadership in engine design

    When attempting to design engines to be more fuel-efficient and emissions-free, automotive manufacturers have to take into account all the complexity inherent in the combustion process.

    ORNL partners with industry to address multiple nuclear technology challenges

    The Department of Energy's Oak Ridge National Laboratory is collaborating with industry on six new projects focused on advancing commercial nuclear energy technologies that offer potential improvements to current nuclear reactors and move new reactor designs closer to deployment.

    Lithium earns honors for three physicists working to bring the energy that powers the sun to Earth

    Feature describes research of three PPPL physicists who have won the laboratory's 2018 outstanding research awards

    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.


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    Observing Clouds in Four Dimensions

    Six cameras are revolutionizing observations of shallow cumulus clouds.

    A Challenging Future for Tropical Forests

    Mortality rates of moist tropical forests are on the rise due to environmental drivers and related mechanisms.

    Rapid Lake Draining on Ice Sheets Changes How Water Moves in Unexpected Ways

    Widespread fracturing during lake drainage triggers vertical shafts to form that affect the Greenland Ice Sheet.

    New Historical Emissions Trends Estimated with the Community Emissions Data System

    The data system will allow for more detailed, consistent, and up-to-date global emissions trends that will aid in understanding aerosol effects.

    Peering into the Mist: How Water Vapor Changes Metal at the Atomic Level

    New insights into molecular-level processes could help prevent corrosion and improve catalytic conversion.

    Microbial Types May Prove Key to Gas Releases from Thawing Permafrost

    Scientists discover key types of microbes that degrade organic matter and release carbon dioxide and methane into the atmosphere.

    New Method Knocks Out Yeast Genes with Single-Point Precision

    Researchers can precisely study how different genes affect key properties in a yeast used industrially to produce fuel and chemicals.

    How Plants Regulate Sugar Deposition in Cell Walls

    Identified genes involved in plant cell wall polysaccharide production and restructuring could aid in engineering bioenergy crops.

    Scientists Identify Gene Cluster in Budding Yeasts with Major Implications for Renewable Energy

    How yeast partition carbon into a metabolite may offer insights into boosting production for biofuels.

    More Designer Peptides, More Possibilities

    A combined experimental and modeling approach contributes to understanding small proteins with potential use in industrial, therapeutic applications.


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