Citation: Jiazhi Wang, Kai Li, Qi Hao, Dongxue Liu, Xinbo Zhang. Electroreduction NO to NH₃ over single metal atom anchored on pyrrole type defective graphene: A DFT study[J]. Chinese Chemical Letters, ;2023, 34(5): 107567. doi: 10.1016/j.cclet.2022.05.081 shu

Electroreduction NO to NH₃ over single metal atom anchored on pyrrole type defective graphene: A DFT study

Jiazhi Wang ^{a, b} ,
Kai Li ^a ,
Qi Hao ^{a, c} ,
Dongxue Liu ^c ,
Xinbo Zhang ^{a, b, *,}

a.
State Key Laboratory of Rare Earth Resource Utilization, Changchun Institute of Applied Chemistry, Chinese Academy of Sciences, Changchun 130022, China
b.
University of Science and Technology of China, Hefei 230026, China
c.
Key Laboratory of Automobile Materials, Ministry of Education, Jilin University, Changchun 130022, China

xbzhang@ciac.ac.cn

Received Date: 30 April 2022
Revised Date: 5 May 2022
Accepted Date: 26 May 2022
Available Online: 29 May 2022

Figures(5)

Electrochemical is considered an attractive approach to recycling the pollution NO (NORR) and producing the valuable NH₃, which could simultaneously solve the two challenging problems, i.e., NO removal and NH₃ synthesis. Current research efforts focus less on NORR due to the lack of effective catalysts. Herein, based on DFT calculation, we try to explore effective pyrrole-type TM-N₄ (TM = V, Cr, Mn, Fe, Co, Ni, Cu, Ru, Rh, Ta) catalysts for achieving the direct NORR. Among the investigated systems, Fe-N₄ exhibits excellent catalytic activity and high NH₃ selectivity. Moreover, the free energy of adsorption of N^* has been proposed as a descriptor to predict and screen the effective TM-N₄ catalyst for NORR and the crystal orbital halmilton populations (COHP) is used to describe the intrinsic relationship between metal atoms and the adsorption free energy of N^* intermediate. This work has provided a theoretical picture of TM-N₄ catalyzing NO to NH₃, which will establish guidelines for the rational design of NORR catalysts and other electrochemical reactions.
- DFT calculation,
- Pyrrole-type,
- Descriptor,
- NORR,
- COHP
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沈阳化工大学材料科学与工程学院沈阳 110142

Electroreduction NO to NH3 over single metal atom anchored on pyrrole type defective graphene: A DFT study

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通讯作者: 陈斌, bchen63@163.com

Electroreduction NO to NH₃ over single metal atom anchored on pyrrole type defective graphene: A DFT study