TY  - JOUR
AU  - Zhang, Li
AU  - Jiao, Shilong
AU  - Tan, Xin
AU  - Yuan, Yuliang
AU  - Xiang, Yu
AU  - Zeng, Yu-Jia
AU  - Qiu, Jingyi
AU  - Peng, Ping
AU  - Smith, Sean C.
AU  - Huang, Hongwen
PY  - 2021
TI  - Theory-guided construction of electron-deficient sites via removal of lattice oxygen for the boosted electrocatalytic synthesis of ammonia
JO  - Nano Research
SN  - 1998-0124
SP  - 1457
EP  - 1464
VL  - 14
IS  - 5
AB  - 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.
UR  - https://doi.org/10.1007/s12274-020-3202-1
DO  - 10.1007/s12274-020-3202-1