@article{Zhang2021, 
author = {Li Zhang and Shilong Jiao and Xin Tan and Yuliang Yuan and Yu Xiang and Yu-Jia Zeng and Jingyi Qiu and Ping Peng and Sean C. Smith and Hongwen Huang},
title = {Theory-guided construction of electron-deficient sites via removal of lattice oxygen for the boosted electrocatalytic synthesis of ammonia},
year = {2021},
journal = {Nano Research},
volume = {14},
number = {5},
pages = {1457-1464},
keywords = {density functional theory, nitrogen reduction, oxygen vacancies, electron-deficient sites},
url = {https://www.sciopen.com/article/10.1007/s12274-020-3202-1},
doi = {10.1007/s12274-020-3202-1},
abstract = {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.}
}