Heterojunction-Induced Local Charge Redistribution Boosting Energy-Saving Hydrogen Production via Urea Electrolysis
Haoran Ding, Zhanhong Zhao, Zeng He, Xin Li, Kuixin Cui, Yi Zhang, Xinghua Chang
Abstract
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, LaNiO 3 –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 LaNiO 3 /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 LaNiO 3 –NiO heterojunction could effectively diminish the stepwise energy barrier, accelerating desorption of *CO 2 . As a result, the LaNiO 3 –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.