首页|Antagonism effect of residual S triggers the dual-path mechanism for water oxidation

Antagonism effect of residual S triggers the dual-path mechanism for water oxidation

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Transition metal chalcogenides(TMCs)are recognized as pre-catalysts,and their(oxy)hydroxides derived from electrochemical reconstruction are the active species in the water oxidation.However,understand-ing the role of the residual chalcogen in the reconstructed layer is lacking in detail,and the corresponding catalytic mechanism remains controversial.Here,taking Cu1-xCoxS as a platform,we explore the regulat-ing effect and existence form of the residual S doped into the reconstructive layer for oxygen evolution reaction(OER),where a dual-path OER mechanism is proposed.First-principles calculations and oper-ando 18O isotopic labeling experiments jointly reveal that the residual S in the reconstructive layer of Cu1-xCoxS can wisely balance the adsorbate evolution mechanism(AEM)and lattice oxygen oxidation mechanism(LOM)by activating lattice oxygen and optimizing the adsorption/desorption behaviors at metal active sites,rather than change the reaction mechanism from AEM to LOM.Following such a dual-path OER mechanism,Cu0.4Co0.6S-derived Cu0.4Co0.6OSH not only overcomes the restriction of linear scaling relationship in AEM,but also avoids the structural collapse caused by lattice oxygen migration in LOM,so as to greatly reduce the OER potential and improved stability.

Electrochemical reconstructionAdsorbate evolution mechanismLattice oxygen oxidation mechanismOxygen evolution reactionResidual sulfur

Li Liu、Jinming Cao、Siqi Hu、Tinghui Liu、Can Xu、Wensheng Fu、Xinguo Ma、Xiaohui Yang

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Chongqing Key Laboratory of Green Catalytic Materials and Technology,College of Chemistry,Chongqing Normal University,Chongqing 401331,China

School of Science,Hubei University of Technology,Wuhan 430068,Hubei,China

Chongqing Institute of Green and Intelligent Technology,Chinese Academy of Sciences,Chongqing 400714,China

Science and Technology Research Program of Chongqing Municipal Education CommissionNatural Science Foundation Joint Fund for Innovation and Development of Chongqing Municipal Education CommissionNational Natural Science Foundation of ChinaScience and Technology Research Program of Natural Science Foundation of ChongqingScience and Technology Research Program of Chongqing Municipal Education CommissionChongqing Innovation Research Group ProjectDoctor Start/Talent Introduction Program of Chongqing Normal University

KJQN202200550CSTB2022NSCQ-LZX007752100065cstc2021ycjhbgzxm0037KJZD-M202200503CXQT2101502060404/2020009000321

2024

10.1016/j.jechem.2024.02.028

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)：2024.93(6)
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