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

作者：Han, Wen-Kai; Wei, Jin-Xin; Xiao, Kang; Ouyang, Ting; Peng, Xinwen; Zhao, Shenlong^*; Liu, Zhao-Qing^*

来源：Angewandte Chemie - International Edition, 2022, 61(31): e202206050.

DOI：10.1002/anie.202206050

• Charge Disproportionation
• Delithium
• Lattice Strain
• LiNiO2
• Urea Oxidation Reaction

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.

• 单位
  广州大学