Assembly of low-voltage driven co-production of hydrogen and sulfur via Ru nanoclusters on metal-sulfur coordination:Insights from DFT calculations  

作　　者：Ahreum Min Velusamy Maheskumar Dong Hyeon Lee Anuj Kumar Cheol Joo Moon Raja Arumugam Senthil Myong Yong Choi 

机构地区：[1]Core-Facility Center for Photochemistry&Nanomaterials,Gyeongsang National University,Jinju 52828,Gyeongsangnam do,Republic of Korea [2]Department of Chemistry(BK21 FOUR),Research Institute of Natural Sciences,Gyeongsang National University,Jinju 52828,Gyeongsangnam do,Republic of Korea [3]Nano-Technology Research Laboratory,Department of Chemistry,GLA University,Mathura,Uttar Pradesh 281406,India

出　　处：《Journal of Energy Chemistry》2024年第12期541-552,共12页能源化学（英文版）

基　　金：supported by the Korea Basic Science Institute(National research Facilities and Equipment Center)grant funded by the Ministry of Education(No.2019R1A6C1010042);the financial support from the National Research Foundation of Korea(NRF)(2022R1A2C2010686,2022R1A4A3033528,2021R1C1C2010726)。

摘　　要：Herein,we propose a simple and rapid approach for synthesizing a CuS/Ru composite that serves as a bifunctional electrocatalyst to promote hydrogen production and concurrently convert sulfion into a value-added sulfur product.This composite comprises Ru nanoclusters supported on the CuS nanostructure,achieved through simple pulsed laser irradiation in liquid approach.The optimized CuS/Ru-30 electrocatalyst demonstrates remarkable bifunctional electrocatalytic activity,exhibiting a negligible working potential of 0.28 V(vs.RHE)for the anodic sulfion oxidation reaction(SOR)and a minimal overpotential of 182 m V for cathodic hydrogen evolution reaction(HER)to achieve 10 mA cm^(-2)of current density.Moreover,the Cu S/Ru-30 electrocatalyst shows exceptional selectivity for converting sulfion into valuable sulfur during anodic oxidation reactions.Remarkably,in a two-electrode electrolyzer system utilizing Cu S/Ru-30 as both the anode and cathode,the SOR+HER coupled water electrolysis system demands only 0.52 V to reach 10 mA cm^(-2),which is considerably lesser compared to the OER+HER coupled water electrolysis(1.85 V).The experimental results and density function theory(DFT)calculations reveal that the strong electron interaction between CuS and Ru nanoclusters generates a built-in electric field,greatly enhancing electron transfer efficiency.This significantly boosts the HER performance and facilitates the adsorption and production of sulfur intermediates.This study presents a rapid and simple strategy for synthesizing a dual-functional catalyst suitable for low-voltage hydrogen generation while facilitating the recovery of valuable sulfur sources.

关 键 词：Copper sulfide Ru nanoclusters Pulsed laser irradiation in liquids Sulfion oxidation reaction Hydrogen evolution reaction 

分 类 号：TQ116.2[化学工程—无机化工] O643.36[理学—物理化学] TQ125.1[理学—化学]