Nano-Au-decorated hierarchical porous cobalt sulfide derived from ZIF-67 toward optimized oxygen evolution catalysis:Important roles of microstructures and electronic modulation  

作　　者：Hongyu Gong Guanliang Sun Wenhua Shi Dongwei Li Xiangjun Zheng Huan Shi Xiu Liang Ruizhi Yang Changzhou Yuan 

机构地区：[1]Department of New Energy Materials,School of Environmental and Chemical Engineering,Jiangsu University of Science and Technology,Zhenjiang,Jiangsu,China [2]Advanced Materials Institute,Qilu University of Technology(Shandong Academy of Sciences),Jinan,Shandong,China [3]Shandong Saikesaisi Hydrogen Energy Co.,Ltd.,Jinan,Shandong,China [4]Department of Materials Science and Engineering,School of Materials Science&Engineering,University of Jinan,Jinan,Shandong,China [5]Department of New Energy Science and Engineering,College of Energy,Soochow Institute for Energy and Materials Innovations,Soochow University,Suzhou,Jiangsu,China

出　　处：《Carbon Energy》2024年第5期1-14,共14页碳能源（英文）

基　　金：National Natural Science Foundation of China,Grant/Award Numbers:52102260,52171211,51972220,61903235,U22A20145;Shandong Provincial Natural Science Foundation,Grant/Award Numbers:ZR2020QB069,ZR2022ME051;National Key Research and Development Program of China,Grant/Award Number:2022YFB4002004;Scientific and Technological Innovation Ability Improvement Project of Minor Enterprises in Shandong Province,Grant/Award Number:2022TSGC1021;Announce the List and Take Charge Project in Jinan,Grant/Award Number:202214012;Major innovation project for integrating science,education and industry of Qilu University of Technology (Shandong Academy of Sciences),Grant/Award Numbers:2022JBZ01-07,2022PY044;China Postdoctoral Science Foundation,Grant/Award Number:2022M711545。

摘　　要：Enhancing both the number of active sites available and the intrinsic activity of Co-based electrocatalysts simultaneously is a desirable goal.Herein,a ZIF-67-derived hierarchical porous cobalt sulfide decorated by Au nanoparticles(NPs)(denoted as HP-Au@CoxSy@ZIF-67)hybrid is synthesized by low-temperature sulfuration treatment.The well-defined macroporous-mesoporous-microporous structure is obtained based on the combination of polystyrene spheres,as-formed CoxSy nanosheets,and ZIF-67 frameworks.This novel three-dimensional hierarchical structure significantly enlarges the three-phase interfaces,accelerating the mass transfer and exposing the active centers for oxygen evolution reaction.The electronic structure of Co is modulated by Au through charge transfer,and a series of experiments,together with theoretical analysis,is performed to ascertain the electronic modulation of Co by Au.Meanwhile,HP-Au@CoxSy@ZIF-67 catalysts with different amounts of Au were synthesized,wherein Au and NaBH4 reductant result in an interesting“competition effect”to regulate the relative ratio of Co^(2+)/Co^(3+),and moderate Au assists the electrochemical performance to reach the highest value.Consequently,the optimized HP-Au@CoxSy@ZIF-67 exhibits a low overpotential of 340 mV at 10 mA cm^(-2)and a Tafel slope of 42 mV dec-1 for OER in 0.1 M aqueous KOH,enabling efficient water splitting and Zn-air battery performance.The work here highlights the pivotal roles of both microstructural and electronic modulation in enhancing electrocatalytic activity and presents a feasible strategy for designing and optimizing advanced electrocatalysts.

关 键 词：Au nanoparticles cobalt sulfide electronic modulation hierarchical porous structure oxygen evolution reaction 

分 类 号：O64[理学—物理化学]