Sequential reactant water management by complementary multisite catalysts for surpassing platinum hydrogen evolution activity  

作　　者：Yu Lin Defang Ding Shicheng Zhu Qunlei Wen Huangjingwei Li Zhen Li Youwen Liu Yi Shen 

机构地区：[1]China Engineering Research Center of Nano-Geomaterials of Ministry of Education,Faculty of Materials Science and Chemistry,China University of Geosciences,Wuhan 430078,China [2]State Key Laboratory of Materials Processing and Die&Mould Technology,and School of Materials Science and Engineering,Huazhong University of Science and Technology,Wuhan 430074,China

出　　处：《Nano Research》2024年第3期1232-1241,共10页纳米研究（英文版）

摘　　要：Alkaline hydrogen evolution reaction(HER)offers a near-zero-emission approach to advance hydrogen energy.However,the activity limited by the multiple reaction steps involving H_(2)O molecules transfer,absorption,and activation still unqualified the thresholds of economic viability.Herein,we proposed a multisite complementary strategy that incorporates hydrophilic Mo and electrophilic V into Ni-based catalysts to divide the distinct steps on atomically dispersive sites and thus realize sequential regulation of the HER process.The Isotopic labeled in situ Raman spectroscopy describes 4-coordinated hydrogen bonded H_(2)O to be free H_(2)O passing the inner Helmholtz plane in the vicinity of the catalysts under the action of hydrophilic Mo sites.Furthermore,potential-dependent electrochemical impedance spectroscopy(EIS)reveals that electrophilic V sites with abundant 3d empty orbitals could activate the lone-pair electrons in the free H_(2)O molecules to produce more protic hydrogen,and dimerize into H_(2) at the Ni sites.By the sequential management of reactive H_(2)O molecules,NiMoV oxides multisite catalysts surpass Pt/C hydrogen evolution activity(49 mV@10 mA∙cm^(-2) over 140 h).Profoundly,this study provides a tangible model to deepen the comprehension of the catalyst–electrolyte interface and create efficient catalysts for diverse reactions.

关 键 词：hydrogen evolution activity complementary multisite catalysts sequential reactive water management interfacial water molecules 

分 类 号：O64[理学—物理化学]