Citation: Fang Yuan, Risheng Sun, Ling Fu, Guozheng Zhao. Defect engineering for high-selection-performance of N₂ activation over CeO₂(111) surface[J]. Chinese Chemical Letters, ;2022, 33(4): 2188-2194. doi: 10.1016/j.cclet.2021.09.003 shu

Defect engineering for high-selection-performance of N₂ activation over CeO₂(111) surface

Fang Yuan ^a ,
Risheng Sun ^b ,
Ling Fu ^{b, *,} ,
Guozheng Zhao ^{a, *,}

a.
Key Laboratory of Magnetic Molecules and Magnetic Information Materials Ministry of Education, The School of Chemistry and Material Science, Shanxi Normal University, Linfen 041004, China
b.
Institute of Environment and Energy Catalysis, Shaanxi Key Laboratory of Optoelectronic Functional Materials and Devices, School of Materials Science and Chemical Engineering, Xi'an Technological University, Xi'an 710021, China

ful263@nenu.edu.cn

zhaoguozheng@sxnu.edu.cn

Received Date: 8 August 2021
Revised Date: 20 August 2021
Accepted Date: 2 September 2021
Available Online: 9 September 2021

Figures(4)

Nitrogen reduction reactions (NRR) under room conditions remain the challenge for N₂ activation on metal-based catalysis materials. Herein, the M-doped CeO₂(111) (M = Ca, Ti, V, Cr, Mn, Fe, Co, Ni, Cu and Zn) with oxygen vacancies, are systematically investigated by spin-polarized DFT + U calculations. We discuss briefly the situation of OVs on pure and reduced cerium, and we found that (1) doping TMs can promote the formation of oxygen defects, apart from Ti and V-dopant, (2) the O atoms are easier to escape connecting to M atoms than the ones of adjacent atoms connecting to the Ce(III), the value of OVs formation energies decrease as the TMs radius decrease. Also, our computational results show that Cr-doped, Mn-doped, Fe-doped, and Co-doped CeO₂(111) adsorbs N₂ strongly than the stoichiometric surface and other M-doped CeO₂ surfaces with adsorption energies of −0.82, −1.02, −0.83 and −1.05 eV. Through COHP analysis, it is found that the predicted active sites have good catalytic performance.
- Nitrogen reduction,
- CeO₂(111),
- Defect,
- Mechanism
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通讯作者: 陈斌, bchen63@163.com

1.
沈阳化工大学材料科学与工程学院沈阳 110142

Defect engineering for high-selection-performance of N2 activation over CeO2(111) surface

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通讯作者: 陈斌, bchen63@163.com

Defect engineering for high-selection-performance of N₂ activation over CeO₂(111) surface