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

被引：112

作者：

Han, Wen-Kai ^{[1
]}

Wei, Jin-Xin ^{[1
]}

Xiao, Kang ^{[1
]}

Ouyang, Ting ^{[1
]}

Peng, Xinwen ^{[2
]}

Zhao, Shenlong ^{[3
]}

Liu, Zhao-Qing ^{[1
]}

机构：

[1] Guangzhou Univ, Sch Chem & Chem Engn, Guangzhou Key Lab Clean Energy & Mat,Minist Educ, Key Lab Water Qual & Conservat Pearl River Delta, 230 Wai Huan Xi Rd, Guangzhou 510006, Peoples R China

[2] Univ Sydney, Sch Chem & Biomol Engn, Sydney, NSW 2006, Australia

[3] South China Univ Technol, Sch Light Ind Sci & Engn, Wushan St, Guangzhou 510641, Peoples R China

来源：

ANGEWANDTE CHEMIE-INTERNATIONAL EDITION | 2022年 / 61卷 / 31期

基金：

中国国家自然科学基金; 澳大利亚研究理事会;

关键词：

Charge Disproportionation; Delithium; Lattice Strain; LiNiO2; Urea Oxidation Reaction; ANIONIC REDOX ACTIVITY; METAL; EFFICIENT; ARRAYS; NI;

D O I：

10.1002/anie.202206050

中图分类号：

O6 [化学];

学科分类号：

0703 ;

摘要：

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.

引用

页数：9

共 45 条

[31] Operando Observations of a Manganese Oxide Electrocatalyst for Water Oxidation Using Hard/Tender/Soft X-ray Absorption Spectroscopy [J].