Enabling built-in electric fields on rhenium-vacancy-rich heterojunction interfaces of transition-metal dichalcogenides for pH-universal efficient hydrogen and electric energy generation  

作　　者：Benzhi Wang Lixia Wang Ji Hoon Lee Tayirjan Taylor Isimjan Hyung Mo Jeong Xiulin Yang 

机构地区：[1]Guangxi Key Laboratory of Low Carbon Energy Materials,School of Chemistry and Pharmaceutical Sciences,Guangxi Normal University,Guilin,China [2]Department of Smart Fab.Technology,School of Mechanical Engineering,Sungkyunkwan University,Suwon,Republic of Korea [3]School of Materials Science and Engineering,Kyungpook National University,Daegu,Republic of Korea [4]Saudi Arabia Basic Industries Corporation(SABIC)at King Abdullah University of Science and Technology(KAUST),Thuwal,Saudi Arabia

出　　处：《Carbon Energy》2024年第9期195-209,共15页碳能源（英文）

基　　金：This study was supported by the National Research Foundation of Korea(NRF-2021R1A2C4001777,NRF-2022M3H4A1A04096482 and RS-2023-00229679),the National Natural Science Foundation of China(No.21965005,52363028);the Natural Science Foundation of Guangxi Province(2021GXNSFAA076001);the Guangxi Technology Base and Talent Subject(GUIKE AD20297039).

摘　　要：Most advanced hydrogen evolution reaction(HER)catalysts show high activity under alkaline conditions.However,the performance deteriorates at a natural and acidic pH,which is often problematic in practical applications.Herein,a rhenium(Re)sulfide–transition-metal dichalcogenide heterojunc-tion catalyst with Re-rich vacancies(NiS_(2)-ReS_(2)-V)has been constructed.The optimized catalyst shows extraordinary electrocatalytic HER performance over a wide range of pH,with ultralow overpotentials of 42,85,and 122 mV under alkaline,acidic,and neutral conditions,respectively.Moreover,the two-electrode system with NiS_(2)-ReS_(2)-V1 as the cathode provides a voltage of 1.73 V at 500 mA cm^(-2),superior to industrial systems.Besides,the open-circuit voltage of a single Zn–H_(2)O cell with NiS_(2)-ReS_(2)-V1 as the cathode can reach an impressive 90.9% of the theoretical value,with a maximum power density of up to 31.6 mW cm^(-2).Moreover,it shows remarkable stability,with sustained discharge for approximately 120 h at 10 mA cm^(-2),significantly outperforming commercial Pt/C catalysts under the same conditions in all aspects.A series of systematic characterizations and theoretical calculations demonstrate that Re vacancies on the heterojunction interface would generate a stronger built-in electric field,which profoundly affects surface charge distribution and subsequently enhances HER performance.

关 键 词：built-in electric field ELECTROCATALYSTS hydrogen evolution reaction self-powered system water splitting Zn-H_(2)O cell 

分 类 号：O64[理学—物理化学] TM91[理学—化学]