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https://doi.org/10.1007/s12274-020-3202-1

Theory-guided construction of electron-deficient sites via removal of lattice oxygen for the boosted electrocatalytic synthesis of ammonia

Li Zhang1,§, Shilong Jiao2,§, Xin Tan3,§, Yuliang Yuan1, Yu Xiang4, Yu-Jia Zeng2, Jingyi Qiu4 (✉), Ping Peng1 (✉), Sean C. Smith3, and Hongwen Huang1 (✉)

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1 College of Materials Science and Engineering, Hunan University, Changsha 410082, China
2 College of Physics and Optoelectronic Engineering, Shenzhen University, Shenzhen 518061, China
3 Integrated Materials Design Laboratory, Department of Applied Mathematics, Research School of Physics, The Australian National University, Canberra, ACT 2601, Australia
4 Research Institute of Chemical Defense, Beijing 100191, China
§ Li Zhang, Shilong Jiao, and Xin Tan contributed equally to this work.

Keywords: nitrogen reduction, density functional theory, oxygen vacancies, electron-deficient sites
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  • Abstract
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Rational design of catalytic sites to activate the inert N≡N bond is of paramount importance to advance N2 electroreduction. Here, guided by the theoretical predictions, we construct a NiFe layered double hydroxide (NiFe-LDH) nanosheet catalyst with a high density of electron-deficient sites, which were achieved by introducing oxygen vacancies in NiFe-LDH. Density functional theory calculations indicate that the electron-deficient sites show a much lower energy barrier (0.76 eV) for the potential determining step compared with that of the pristine NiFe-LDH (2.02 eV). Benefiting from this, the NiFe-LDH with oxygen vacancies exhibits the greatly improved electrocatalytic activity, presenting a high NH3 yield rate of 19.44 μg·h−1·mgcat−1, Faradaic efficiency of 19.41% at −0.20 V vs. reversible hydrogen electrode (RHE) in 0.1 M KOH electrolyte, as well as the outstanding stability. The present work not only provides an active electrocatalyst toward N2 reduction but also offers a facile strategy to boost the N2 reduction.
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Theory-guided construction of electron-deficient sites via removal of lattice oxygen for the boosted electrocatalytic synthesis of ammonia. Nano Res. https://doi.org/10.1007/s12274-020-3202-1

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