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Single Atoms of Iron on MoS2 Nanosheets for N2 Electroreduction into Ammonia
Authors:Hongyang Su  Lanlan Chen  Yizhen Chen  Prof Rui Si  Yuting Wu  Xiaonan Wu  Dr Zhigang Geng  Prof Wenhua Zhang  Prof Jie Zeng
Institution:1. Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui, 230026 P. R. China

These authors contributed equally to this work.;2. Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion and Synergetic Innovation Centre of Quantum Information & Quantum Physics, University of Science and Technology of China, Hefei, Anhui, 230026 P. R. China

These authors contributed equally to this work.;3. Shanghai Synchrotron Radiation Facility, Shanghai Advanced Research Institute, Chinese Academy of Sciences, Shanghai, 201210 P. R. China;4. Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Strongly-Coupled Quantum Matter Physics, Key Laboratory of Surface and Interface Chemistry and Energy Catalysis of Anhui Higher Education Institutes, Department of Chemical Physics, University of Science and Technology of China, Hefei, Anhui, 230026 P. R. China;5. Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion and Synergetic Innovation Centre of Quantum Information & Quantum Physics, University of Science and Technology of China, Hefei, Anhui, 230026 P. R. China

Abstract:Efforts have been devoted to achieving a highly efficient artificial synthesis of ammonia (NH3). Reported herein is a novel Fe-MoS2 catalyst with Fe atomically dispersed onto MoS2 nanosheets, imitating natural nitrogenase, to boost N2 electroreduction into NH3 at room temperature. The Fe-MoS2 nanosheets exhibited a faradic efficiency of 18.8 % with a yield rate of 8.63 μgurn:x-wiley:00448249:media:ange202009217:ange202009217-math-0001 mgcat.−1 h−1 for NH3 at −0.3 V versus the reversible hydrogen electrode. The mechanism study revealed that the electroreduction of N2 was promoted and the competing hydrogen evolution reaction was suppressed by decorating the edge sites of S in MoS2 with the atomically dispersed Fe, resulting in high catalytic performance for the electroreduction of N2 into NH3. This work provides new ideas for the design of catalysts for N2 electroreduction and strengthens the understanding about N2 activation over Mo-based catalysts.
Keywords:ammonia  electrochemistry  heterogeneous catalysis  iron  nanostructures
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