首页|Microwave-assisted exploration of the electron configuration-dependent electrocatalytic urea oxidation activity of 2D porous NiCo2O4 spinel

Microwave-assisted exploration of the electron configuration-dependent electrocatalytic urea oxidation activity of 2D porous NiCo2O4 spinel

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Urea holds promise as an alternative water-oxidation substrate in electrolytic cells.High-valence nickel-based spinel,especially after heteroatom doping,excels in urea oxidation reactions(UOR).However,traditional spinel synthesis methods with prolonged high-temperature reactions lack kinetic precision,hindering the balance between controlled doping and highly active two-dimensional(2D)porous struc-tures design.This significantly impedes the identification of electron configuration-dependent active sites in doped 2D nickel-based spinels.Herein,we present a microwave shock method for the preparation of 2D porous NiCo2O4 spinel.Utilizing the transient on-off property of microwave pulses for precise heteroatom doping and 2D porous structural design,non-metal doping(boron,phosphorus,and sulfur)with distinct extranuclear electron disparities serves as straightforward examples for investigation.Precise tuning of lattice parameter reveals the impact of covalent bond strength on NiCo2O4 structural stability.The introduced defect levels induce unpaired d-electrons in transition metals,enhancing the adsorption of electron-donating amino groups in urea molecules.Simultaneously,Bode plots confirm the impact mechanism of rapid electron migration caused by reduced band gaps on UOR activity.The pre-pared phosphorus-doped 2D porous NiCo2O4,with optimal electron configuration control,outperforms most reported spinels.This controlled modification strategy advances understanding theoretical structure-activity mechanisms of high-performance 2D spinels in UOR.

2D materialsSpinelMicrowaveElectrocatalysisUrea oxidation reaction

Jun Wan、Zhiao Wu、Guangyu Fang、Jinglin Xian、Jiao Dai、Jiayue Guo、Qingxiang Li、Yongfei You、Kaisi Liu、Huimin Yu、Weilin Xu、Huiyu Jiang、Minggui Xia、Huanyu Jin

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State Key Laboratory of New Textile Materials and Advanced Processing Technologies,Hubei Key Laboratory of Biomass Fibers and Eco-Dyeing & Finishing,Wuhan Textile University,Wuhan 430200,Hubei,China

Future Industries Institute,University of South Australia,Mawson Lakes Campus,Adelaide,SA 5095,Australia

Institute for Sustainability,Energy and Resources,The University of Adelaide,Adelaide,SA 5005,Australia

国家自然科学基金Open Fund of State Key Laboratory of New Textile Materials and Advanced Processing TechnologiesOpen Fund of Hubei Key Laboratory of Biomass Fiber and Ecological Dyeing and Finishing

52203070FZ2022005STRZ202203

2024

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子:0.654
ISSN:2095-4956
年,卷(期):2024.91(4)
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