Transition metal decorated bismuthene for ammonia synthesis: A density functional theory study |
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| Institution: | 1. School of Energy and Power Engineering, Jiangsu University of Science and Technology, Zhenjiang 212003, China;2. School of Chemistry and Chemical Engineering, Institute for Computation in Molecular and Materials Science, Nanjing University of Science and Technology, Nanjing 210094, China;3. Institut Charles Gerhardt Montpellier, UMR-5253, Université de Montpellier, CNRS, ENSCM, Place E. Bataillon, Cedex 05, Montpellier 34095, France;4. Advanced Interdisciplinary Institute of Environment and Ecology, Beijing Normal University, Zhuhai 519087, China;1. College of Mechanics and Materials, Hohai University, Nanjing 210098, China;2. Guangzhou Key Laboratory Environmental Catalysis and Pollution Control, Guangdong Key Laboratory of Environmental Catalysis and Health Risk Control, Institute of Environmental Health and Pollution Control, School of Environmental Science and Engineering, Guangdong University of Technology, Guangzhou 510006, China;1. State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China;2. University of Science and Technology of China, Hefei 230026, China;3. Key Laboratory of Automobile Materials, Ministry of Education, Jilin University, Changchun 130022, China;1. School of Energy and Power Engineering, Jiangsu University of Science and Technology, 212003, Zhenjiang, Jiangsu, China;2. School of Materials Science and Engineering, Xi''an University of Science and Technology, Xi''an 710054, China;3. The State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Dingxi Road, Shanghai 200050, PR China;1. Institute of Functional Material Chemistry, National & Local United Engineering Lab for Power Battery, Key Laboratory of Polyoxometalate Science of Ministry of Education, Faculty of Chemistry, Northeast Normal University, Changchun 130024, PR China;2. School of Material and Environmental Engineering, Hangzhou Dianzi University, Hangzhou 310018, PR China;3. Institute Centre for Advanced Optoelectronic Functional Materials Research and Key Laboratory of UV-Emitting Materials and Technology, Ministry of Education, Northeast Normal University, Changchun 130024, PR China;4. Institute of Theoretical Chemistry, Jilin University, Changchun 130023, PR China;1. School of Energy and Power Engineering, Jiangsu University of Science and Technology, Zhenjiang 212003, China;2. The State Key Laboratory of High Performance Ceramics and Superfine Microstructure, Shanghai Institute of Ceramics, Chinese Academy of Sciences, 1295 Dingxi Road, Shanghai 200050, China;3. School of Materials Science and Engineering, Xi''an University of Science and Technology, Xi''an 710054, China |
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| Abstract: | The electrochemical nitrogen reduction reaction (NRR) for the ammonia production under ambient conditions is regarded as a sustainable alternative to the industrial Haber–Bosch process. However, the electrocatalytic systems that efficiently catalyze nitrogen reduction remain elusive. In the work, the nitrogen reduction activity of the transition metal decorated bismuthene TM@Bis is fully investigated by means of density functional theory calculations. Our results demonstrate that W@Bis delivers the best efficiency, wherein the potential-determining step is located at the last protonation step of *NH2 + H+ + e– → *NH3 via the distal mechanism with the limiting potential UL of 0.26 V. Furthermore, the dopants of Re and Os are also promising candidates for experimental synthesis due to its good selectivity, in despite of the slightly higher UL of NRR with the value of 0.55 V. However, the candidates of Ti, V, Nb and Mo delivered the relative lower UL of 0.35, 0.37, 0.41 and 0.43 V might be suffered from the side hydrogen evolution reaction. More interestingly, a volcano curve is established between UL and valence electrons of metal elements wherein W with 4 electrons in d band located at the summit. Such phenomenon originates from the underlying acceptance-back donation mechanism. Therefore, our work provides a fundament understanding for the material design for nitrogen reduction electrocatalysis. |
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