首页|Manipulating d-d orbital hybridization induced by Mo-doped Co9S8 nanorod arrays for high-efficiency water electrolysis

Manipulating d-d orbital hybridization induced by Mo-doped Co9S8 nanorod arrays for high-efficiency water electrolysis

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Precisely refining the electronic structure of electrocatalysts represents a powerful approach to further optimize the electrocatalytic performance.Herein,we demonstrate an ingenious d-d orbital hybridization concept to construct Mo-doped Co9S8 nanorod arrays aligned on carbon cloth(CC)substrate(abbreviated as Mo-Co9S8@CC hereafter)as a high-efficiency bifunctional electrocatalyst toward water electrolysis.It has experimentally and theoretically validated that the 4d-3d orbital coupling between Mo dopant and Co site can effectively optimize the H2O activation energy and lower H*adsorption energy barrier,thereby leading to enhanced hydrogen evolution reaction(HER)and oxygen evolution reaction(OER)activities.Thanks to the unique electronic and geometrical advantages,the optimized Mo-Co9S8@CC with appropriate Mo content exhibits outstanding bifunctional performance in alkaline solution,with the overpotentials of 75 and 234 mV for the delivery of a current density of 10 mA cm-2,small Tafel slopes of 53.8 and 39.9 mV dec-1 and long-term stabilities for at least 32 and 30 h for HER and OER,respectively.More impressively,a water splitting electrolylzer assembled by the self-supported Mo-Co9S8@CC elec-trode requires a low cell voltage of 1.53 V at 10 mA cm-2 and shows excellent stability and splendid reversibility,demonstrating a huge potential for affordable and scalable electrochemical H2 production.The innovational orbital hybridization strategy for electronic regulation herein provides an inspirable avenue for developing progressive electrocatalysts toward new energy systems.

d-d orbital hybridizationTransition metal sulfidesNanorods arraysWater electrolysis

Xue Zhou、Jing Li、Guangyao Zhou、Weiran Huang、Yucan Zhang、Jun Yang、Huan Pang、Mingyi Zhang、Dongmei Sun、Yawen Tang、Lin Xu

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Jiangsu Key Laboratory of New Power Batteries,Jiangsu Collaborative Innovation Centre of Biomedical Functional Materials,School of Chemistry and Materials Science,Nanjing Normal University,Nanjing 210023,Jiangsu,China

College of Science,Jinling Institute of Technology,Nanjing 211169,Jiangsu,China

State Key Laboratory of Multiphase Complex Systems,Institute of Process Engineering,Chinese Academy of Sciences,Beijing 100190,China

Nanjing IPE Institute of Green Manufacturing Industry,Nanjing 211100,Jiangsu,China

School of Chemistry and Chemical Engineering,Yangzhou University,Yangzhou 225009,Jiangsu,China

Key Laboratory for Photonic and Electronic Bandgap Materials,Ministry of Education,School of Physics and Electronic Engineering,Harbin Normal University,Harbin 150025,Heilongjiang,China

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National Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaNational Natural Science Foundation of ChinaHighlevel Talents Project of Jinling Institute ofTechnology

219720682207206722232004jitb-202164

2024

10.1016/j.jechem.2024.02.033

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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