Comprehensive Understanding of the Electrocatalytic Mechanism for Co/Fe/Cu Doped Ni(OH)₂ on Urea Oxidation Reactions: Theory and Experiment

Chen, Lu1; Jiang, Wenjie1; Zhang, Jiayu1; Chu, Bingxian1,2; Zhai, Zhixiang1; Yu, Tianqi1; He, Haixiang1; Yin, Shibin1

2024-07-01

10.1021/acssuschemeng.4c02596

ACS SUSTAINABLE CHEMISTRY & ENGINEERING   影响因子和分区

2168-0485

alpha-Ni(OH)(2) is an efficient candidate for urea oxidation reaction (UOR) but its instability and high energy barriers restrict its application. The introduction of transition metals is a strategy to solve these problems, but systematic investigations of mechanisms are limited. Herein, a range of isoelectronic transition metals (ITMs) (M = Co, Fe, and Cu) doped Ni(OH)(2) catalysts on UOR are studied simultaneously in theory and experiment. By introducing Co and Fe into the lattice of Ni(OH)(2), electronic structure transfer is facilitated, resulting in effective promotion of the urea absorption and CO2 desorption, and intrinsic activity can be increased. Among these catalysts, Co-Ni(OH)(2) with the lowest energy barrier (1.76 eV) for rate-determining steps might exhibit excellent activity. To verify the theoretical prediction, samples are synthesized via the one-step hydrothermal method. ITMs incorporation can stabilize the alpha phase of Ni(OH)(2), confirmed by chronopotentiometry and X-ray diffraction results. Agreeing with the calculation, Co-Ni(OH)(2) manifests superior UOR properties than other catalysts, providing the smallest onset potential (1.304 V vs RHE) and Tafel slope (24 mV dec(-1)). This study can provide a comprehensive understanding of the ITMs-Ni(OH)(2) catalytic on UOR mechanism, which could be instructive for designing UOR catalysts with higher activity.

urea oxidation reaction density functional theory nickel hydroxide transition metal dopant rate-determining step

SCI ; EI

英语

其他

National Natural Science Foundation of China[21963002] ; Natural Science Foundation of Guangxi province[2018GXNSFAA050095] ; Guangxi Science and Technology Major Program[AA23062020]

Chemistry ; Science & Technology - Other Topics ; Engineering

Chemistry, Multidisciplinary ; Green & Sustainable Science & Technology ; Engineering, Chemical

WOS:001260678900001

AMER CHEMICAL SOC

20242716619596

Catalyst activity ; Copper compounds ; Electrocatalysis ; Electronic structure ; Energy barriers ; Iron ; Metabolism ; Nickel compounds ; Oxidation ; Urea

Iron:545.1 ; Thermodynamics:641.1 ; Physical Chemistry:801.4 ; Electrochemistry:801.4.1 ; Chemical Reactions:802.2 ; Chemical Agents and Basic Industrial Chemicals:803 ; Chemical Products Generally:804 ; Organic Compounds:804.1 ; Probability Theory:922.1 ; Atomic and Molecular Physics:931.3 ; Quantum Theory; Quantum Mechanics:931.4

Web of Science

1.Guangxi Univ, Guangxi Key Lab Electrochem Energy Mat, Coll Chem & Chem Engn, Key Lab Appl Chem Technol & Resource Dev,Guangxi C, Nanning 530004, Peoples R China
2.Southern Univ Sci & Technol, Dept Chem, Shenzhen 518055, Peoples R China

Chen, Lu,Jiang, Wenjie,Zhang, Jiayu,et al. Comprehensive Understanding of the Electrocatalytic Mechanism for Co/Fe/Cu Doped Ni(OH)₂ on Urea Oxidation Reactions: Theory and Experiment[J]. ACS SUSTAINABLE CHEMISTRY & ENGINEERING,2024,12:10466-10474.

Chen, Lu.,Jiang, Wenjie.,Zhang, Jiayu.,Chu, Bingxian.,Zhai, Zhixiang.,...&Yin, Shibin.(2024).Comprehensive Understanding of the Electrocatalytic Mechanism for Co/Fe/Cu Doped Ni(OH)₂ on Urea Oxidation Reactions: Theory and Experiment.ACS SUSTAINABLE CHEMISTRY & ENGINEERING,12,10466-10474.

Chen, Lu,et al."Comprehensive Understanding of the Electrocatalytic Mechanism for Co/Fe/Cu Doped Ni(OH)₂ on Urea Oxidation Reactions: Theory and Experiment".ACS SUSTAINABLE CHEMISTRY & ENGINEERING 12(2024):10466-10474.