{"title":"Pulsed Laser-patterned high-entropy single-atomic sites and alloy coordinated graphene oxide for pH-universal water electrolysis","authors":"Yeryeong Lee, Theerthagiri Jayaraman, Wanwisa Limphirat, Ganga Periyasamy, Gyoung Hwa Jeong, Soorathep Kheawhom, Yongbing Tang, Myong Yong Choi","doi":"10.1039/d5ta00117j","DOIUrl":null,"url":null,"abstract":"Synthesizing catalysts with multiple single-metal atoms remains challenging. We introduce high-entropy single-atom catalysts (HESACs) co-coordinated with six elements from a FeRuPtNiCoPd high-entropy alloy (HEA) on graphene oxide supports (HESAC–HEA/GO) via single-pot pulsed laser irradiation in liquids (PLIL). This method leverages tailored surface composition and diverse active sites for electrochemical overall water splitting (OWS) across a wide pH range. The synergistic interactions in high-entropy systems and rapid photoreduction of Fe2+ via PLIL enhance nuclei generation and active sites compared to Fe3+, achieving high HER in 0.5 M H2SO4 with η of 49 mV at 10 mA/cm2, and record-high OER in 1.0 M KOH with η of 398 mV. Optimized HESAC–HEA/GO–Fe2+ shows exceptional OWS performance with lower cell voltage compared to HESACC–HEA/GO–Fe3+ and Pt/C. This study offers a robust pathway for fabricating versatile catalysts and facilitates mechanistic insights through in situ Raman and density functional theory analyses.","PeriodicalId":82,"journal":{"name":"Journal of Materials Chemistry A","volume":"11 1","pages":""},"PeriodicalIF":10.7000,"publicationDate":"2025-02-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":null,"platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Materials Chemistry A","FirstCategoryId":"88","ListUrlMain":"https://doi.org/10.1039/d5ta00117j","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
引用次数: 0
Abstract
Synthesizing catalysts with multiple single-metal atoms remains challenging. We introduce high-entropy single-atom catalysts (HESACs) co-coordinated with six elements from a FeRuPtNiCoPd high-entropy alloy (HEA) on graphene oxide supports (HESAC–HEA/GO) via single-pot pulsed laser irradiation in liquids (PLIL). This method leverages tailored surface composition and diverse active sites for electrochemical overall water splitting (OWS) across a wide pH range. The synergistic interactions in high-entropy systems and rapid photoreduction of Fe2+ via PLIL enhance nuclei generation and active sites compared to Fe3+, achieving high HER in 0.5 M H2SO4 with η of 49 mV at 10 mA/cm2, and record-high OER in 1.0 M KOH with η of 398 mV. Optimized HESAC–HEA/GO–Fe2+ shows exceptional OWS performance with lower cell voltage compared to HESACC–HEA/GO–Fe3+ and Pt/C. This study offers a robust pathway for fabricating versatile catalysts and facilitates mechanistic insights through in situ Raman and density functional theory analyses.
期刊介绍:
The Journal of Materials Chemistry A, B & C covers a wide range of high-quality studies in the field of materials chemistry, with each section focusing on specific applications of the materials studied. Journal of Materials Chemistry A emphasizes applications in energy and sustainability, including topics such as artificial photosynthesis, batteries, and fuel cells. Journal of Materials Chemistry B focuses on applications in biology and medicine, while Journal of Materials Chemistry C covers applications in optical, magnetic, and electronic devices. Example topic areas within the scope of Journal of Materials Chemistry A include catalysis, green/sustainable materials, sensors, and water treatment, among others.