首页|Dynamic in situ reconstruction of NiSe2 promoted by interfacial Ce2(CO3)2O for enhanced water oxidation

Dynamic in situ reconstruction of NiSe2 promoted by interfacial Ce2(CO3)2O for enhanced water oxidation

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Understanding and manipulating the structural evolution of water oxidation electrocatalysts lays the foundation to finetune their catalytic activity.Herein,we present a synthesis of NiSe2-Ce2(CO3)2O heterostructure and demonstrate the efficacy of interfacial Ce2(CO3)2O in promoting the formation of cat-alytically active centers to improve oxygen evolution activity.In-situ Raman spectroscopy shows that incorporation of Ce2(CO3)2O into NiSe2 causes a cathodic shift of the Ni2+→Ni3+transition potential.Operando electrochemical impedance spectroscopy reveals that strong electronic coupling at heteroge-neous interface accelerates charge transfer process.Furthermore,density functional theory calculations suggest that actual catalytic active species of NiOOH transformed from NiSe2,which is coupled with Ce2(CO3)2O,can optimize electronic structure and decrease the free energy barriers toward fast oxygen evolution reaction(OER)kinetics.Consequently,the resultant NiSe2-Ce2(CO3)2O electrode exhibits remarkable electrocatalytic performance with low overpotentials(268/304 mV@50/100 mA cm-2)and excellent stability(50 mA cm-2 for 120 h)in the alkaline electrolyte.This work emphasizes the signifi-cance of modulating the dynamic changes in developing efficient electrocatalyst.

Dynamic reconstructionOxygen evolution reactionHeterostructureIn situ characterizationDensity functional theory

Fengli Wei、Jinghao Shen、Jiayin Xie、Zuyang Luo、Luyan Shi、Tayirjan Taylor Isimjan、Xiulin Yang、Jieshan Qiu、Bin Wu

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Guangxi Key Laboratory of Low Carbon Energy Materials,School of Chemistry and Pharmaceutical Sciences,Guangxi Normal University,Guilin 541004,Guangxi,China

Saudi Arabia Basic Industries Corporation(SABIC)at King Abdullah University of Science and Technology(KAUST),Thuwal 23955-6900,Saudi Arabia

State Key Laboratory of Chemical Resource Engineering,State Key Laboratory of Organic-Inorganic Composites,College of Chemical Engineering,Beijing University of Chemical Technology,Beijing 100029,China

Helmholtz-Zentrum Berlin für Materialien und Energie GmbH,Albert-Einstein-Straße 15,Berlin 12489,Germany

Institute of Physics,Humboldt University Berlin,Newton-Straße 15,Berlin 12489,Germany

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2024

10.1016/j.jechem.2024.06.048

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)：2024.98(11)