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      Rational design of electrocatalysts and photo(electro)catalysts for nitrogen reduction to ammonia (NH3) under ambient conditions

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          This perspective highlights the rational design of efficient electrocatalysts and photo(electro)catalysts for N 2 reduction to ammonia (NH 3) under ambient conditions.


          As one of the most important chemicals and carbon-free energy carriers, ammonia (NH 3) has a worldwide annual production of ∼150 million tons, and is mainly produced by the traditional high-temperature and high-pressure Haber–Bosch process which consumes massive amounts of energy. Very recently, electrocatalytic and photo(electro)catalytic reduction of N 2 to NH 3, which can be performed at ambient conditions using renewable energy, have received tremendous attention. The overall performance of these electrocatalytic and photo(electro)catalytic systems is largely dictated by their core components, catalysts. This perspective for the first time highlights the rational design of electrocatalysts and photo(electro)catalysts for N 2 reduction to NH 3 under ambient conditions. Fundamental theory of catalytic reaction pathways for the N 2 reduction reaction and the corresponding material design principles are introduced first. Then, recently developed electrocatalysts and photo(electro)catalysts are summarized, with a special emphasis on the relationship between their physicochemical properties and NH 3 production performance. Finally, the opportunities in this emerging research field, in particular, the strategy of combining experimental and theoretical techniques to design efficient and stable catalysts for NH 3 production, are outlined.

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          Ti3C2 MXene co-catalyst on metal sulfide photo-absorbers for enhanced visible-light photocatalytic hydrogen production

          Scalable and sustainable solar hydrogen production through photocatalytic water splitting requires highly active and stable earth-abundant co-catalysts to replace expensive and rare platinum. Here we employ density functional theory calculations to direct atomic-level exploration, design and fabrication of a MXene material, Ti3C2 nanoparticles, as a highly efficient co-catalyst. Ti3C2 nanoparticles are rationally integrated with cadmium sulfide via a hydrothermal strategy to induce a super high visible-light photocatalytic hydrogen production activity of 14,342 μmol h−1 g−1 and an apparent quantum efficiency of 40.1% at 420 nm. This high performance arises from the favourable Fermi level position, electrical conductivity and hydrogen evolution capacity of Ti3C2 nanoparticles. Furthermore, Ti3C2 nanoparticles also serve as an efficient co-catalyst on ZnS or Zn x Cd1−x S. This work demonstrates the potential of earth-abundant MXene family materials to construct numerous high performance and low-cost photocatalysts/photoelectrodes.
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            Efficient Visible Light Nitrogen Fixation with BiOBr Nanosheets of Oxygen Vacancies on the Exposed {001} Facets.

            Even though the well-established Haber-Bosch process has been the major artificial way to "fertilize" the earth, its energy-intensive nature has been motivating people to learn from nitrogenase, which can fix atmospheric N2 to NH3 in vivo under mild conditions with its precisely arranged proteins. Here we demonstrate that efficient fixation of N2 to NH3 can proceed under room temperature and atmospheric pressure in water using visible light illuminated BiOBr nanosheets of oxygen vacancies in the absence of any organic scavengers and precious-metal cocatalysts. The designed catalytic oxygen vacancies of BiOBr nanosheets on the exposed {001} facets, with the availability of localized electrons for π-back-donation, have the ability to activate the adsorbed N2, which can thus be efficiently reduced to NH3 by the interfacial electrons transferred from the excited BiOBr nanosheets. This study might open up a new vista to fix atmospheric N2 to NH3 through the less energy-demanding photochemical process.
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              Challenges in reduction of dinitrogen by proton and electron transfer.

              Ammonia is an important nutrient for the growth of plants. In industry, ammonia is produced by the energy expensive Haber-Bosch process where dihydrogen and dinitrogen form ammonia at a very high pressure and temperature. In principle one could also reduce dinitrogen upon addition of protons and electrons similar to the mechanism of ammonia production by nitrogenases. Recently, major breakthroughs have taken place in our understanding of biological fixation of dinitrogen, of molecular model systems that can reduce dinitrogen, and in the electrochemical reduction of dinitrogen at heterogeneous surfaces. Yet for efficient reduction of dinitrogen with protons and electrons major hurdles still have to be overcome. In this tutorial review we give an overview of the different catalytic systems, highlight the recent breakthroughs, pinpoint common grounds and discuss the bottlenecks and challenges in catalytic reduction of dinitrogen.

                Author and article information

                Energy & Environmental Science
                Energy Environ. Sci.
                Royal Society of Chemistry (RSC)
                : 11
                : 1
                : 45-56
                [1 ]School of Chemical Engineering
                [2 ]The University of Adelaide
                [3 ]Adelaide
                [4 ]Australia
                [5 ]School of Material Science and Engineering
                © 2018


                Self URI (article page): http://xlink.rsc.org/?DOI=C7EE02220D


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