Details

Autor(en) / Beteiligte

• Han, Wen‐Kai
• Wei, Jin‐Xin
• Xiao, Kang
• Ouyang, Ting
• Peng, Xinwen
• Zhao, Shenlong
• Liu, Zhao‐Qing

Titel

Activating Lattice Oxygen in Layered Lithium Oxides through Cation Vacancies for Enhanced Urea Electrolysis

Ist Teil von

• Angewandte Chemie International Edition, 2022-08, Vol.61 (31), p.e202206050-n/a

Auflage

International ed. in English

Ort / Verlag

Germany: Wiley Subscription Services, Inc

Erscheinungsjahr

2022

Quelle

Alma/SFX Local Collection

Beschreibungen/Notizen

• Despite the fact that high‐valent nickel‐based oxides exhibit promising catalytic activity for the urea oxidation reaction (UOR), the fundamental questions concerning the origin of the high performance and the structure–activity correlations remain to be elucidated. Here, we unveil the underlying enhanced mechanism of UOR by employing a series of prepared cation‐vacancy controllable LiNiO2 (LNO) model catalysts. Impressively, the optimized layered LNO‐2 exhibits an extremely low overpotential at 10 mA cm−2 along with excellent stability after the 160 h test. Operando characterisations combined with the theoretical analysis reveal the activated lattice oxygen in layered LiNiO2 with moderate cation vacancies triggers charge disproportion of the Ni site to form Ni4+ species, facilitating deprotonation in a lattice oxygen involved catalytic process. Beginning with cation‐vacancy controllable LiNiO2, the origin of the high performance and the structure–activity correlations was studied. The results indicate that lattice oxygen activated by cation vacancies triggered charge disproportionation to form high‐activity Ni4+, resulting in facilitating deprotonation in a lattice oxygen involved catalytic process.