Interfacial Electronic Modulation of Dual-Monodispersed Pt–Ni_(3)S_(2) as Efficacious Bi-Functional Electrocatalysts for Concurrent H_(2) Evolution and Methanol Selective Oxidation

作     者：Qianqian Zhao Bin Zhao Xin Long Renfei Feng Mohsen Shakouri Alisa Paterson Qunfeng Xiao Yu Zhang Xian‑Zhu Fu Jing‑Li Luo Qianqian Zhao;Bin Zhao;Xin Long;Renfei Feng;Mohsen Shakouri;Alisa Paterson;Qunfeng Xiao;Yu Zhang;Xian-Zhu Fu;Jing-Li Luo

作者机构：Shenzhen Key Laboratory of Energy Electrocatalytic MaterialsShenzhen Key Laboratory of Polymer Science and TechnologyGuangdong Research Center for Interfacial Engineering of Functional MaterialsCollege of Materials Science and EngineeringShenzhen UniversityShenzhen 518060People’s Republic of China Canadian Light Source Inc.SaskatoonSK S7N 0X4Canada Instrumental Analysis Center of Shenzhen University(Lihu Campus)Shenzhen UniversityShenzhen 518055People’s Republic of China 

出 版 物：《Nano-Micro Letters》 (纳微快报（英文版）)

年 卷 期：2024年第16卷第4期

页      面：415-431页

核心收录：

学科分类：081705[工学-工业催化] 08[工学] 0817[工学-化学工程与技术] 0805[工学-材料科学与工程（可授工学、理学学位）] 080502[工学-材料学] 0702[理学-物理学] 

基　　金：the financial support of Guangdong Basic and Applied Basic Research Foundation (No. 2023A1515010940) Shenzhen Natural Science Fund (the Stable Support Plan Program No. 20220809160022001) the Shenzhen Science and Technology Programs (No. ZDSYS20220527171401003, KQTD20190929173914967) 

主　　题：Dual-monodispersed heterostructure Electronic interactive modulation Reaction mechanism Methanol oxidation reaction Hydrogen generation 

摘      要：Constructing the efficacious and applicable bifunctional electrocatalysts and establishing out the mechanisms of organic electro-oxidation by replacing anodic oxygen evolution reaction(OER) are critical to the development of electrochemicallydriven technologies for efficient hydrogen production and avoid CO_(2) emission. Herein, the hetero-nanocrystals between monodispersed Pt(~ 2 nm) and Ni_(3)S_(2)(~ 9.6 nm) are constructed as active electrocatalysts through interfacial electronic modulation, which exhibit superior bi-functional activities for methanol selective oxidation and H_(2) generation. The experimental and theoretical studies reveal that the asymmetrical charge distribution at Pt–Ni_(3)S_(2) could be modulated by the electronic interaction at the interface of dual-monodispersed heterojunctions, which thus promote the adsorption/desorption of the chemical intermediates at the interface. As a result, the selective conversion from CH_(3)OH to formate is accomplished at very low potentials(1.45 V) to attain 100 m A cm^(-2) with high electronic utilization rate(~ 98%) and without CO_(2) emission. Meanwhile, the Pt–Ni_(3)S_(2) can simultaneously exhibit a broad potential window with outstanding stability and large current densities for hydrogen evolution reaction(HER) at the cathode. Further, the excellent bi-functional performance is also indicated in the coupled methanol oxidation reaction(MOR)//HER reactor by only requiring a cell voltage of 1.60 V to achieve a current density of 50 m A cm^(-2) with good reusability.