Heterojunction-Induced Local Charge Redistribution Boosting Energy-Saving Hydrogen Production via Urea Electrolysis

被引:6
|
作者
Ding, Haoran [1 ]
Zhao, Zhanhong [1 ]
Zeng, He [1 ]
Li, Xin [1 ]
Cui, Kuixin [1 ]
Zhang, Yi [1 ]
Chang, Xinghua [1 ]
机构
[1] Cent South Univ, Sch Minerals Proc & Bioengn, Changsha 410083, Peoples R China
来源
ACS MATERIALS LETTERS | 2024年 / 6卷 / 03期
基金
中国国家自然科学基金;
关键词
ELECTROCATALYTIC ACTIVITY; NICKEL; ELECTROOXIDATION; NANOPARTICLES; OXIDATION; CATALYST; LANIO3; FILMS; GOLD;
D O I
10.1021/acsmaterialslett.3c01578
中图分类号
T [工业技术];
学科分类号
08 ;
摘要
Substituting the oxygen evolution reaction by the urea oxidation reaction (UOR) is thermodynamically more favorable for energy-saving hydrogen production. However, UOR suffers from sluggish reaction kinetics due to its complex six-electron transfer processes combined with conversion of complicated intermediates. Herein, LaNiO3-NiO heterojunctions successfully constructed to accelerate UOR. Systematic experimental investigation and theoretical calculation endorse that self-driven local charge redistribution takes place at the Janus LaNiO3/NiO interface, generating local nucleophilic and electrophilic regions. Such a unique structure is favorable for targeted adsorption of amino groups and electrophilic carbonyl groups, thus promoting the rupture of C-N bonds in urea. In addition, the build-in electric field triggered by LaNiO3-NiO heterojunction could effectively diminish the stepwise energy barrier, accelerating desorption of *CO2. As a result, the LaNiO3-NiO exhibits superior UOR performance, delivering a current density of 10 mA cm(-2) at 1.34 V (vs RHE). This work supplies valuable insights for fundamental understanding and rational construction of efficient heterojunction UOR catalyst.
引用
收藏
页码:1029 / 1041
页数:13
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