Yuanyuan Sun , Wen Zhao , Wei Cai , Yuhua Chi , Hao Ren , Zhongtao Li
{"title":"通过串联水氧化实现乙烯电化学转化的单原子 M/GDY 催化剂","authors":"Yuanyuan Sun , Wen Zhao , Wei Cai , Yuhua Chi , Hao Ren , Zhongtao Li","doi":"10.1016/j.apsusc.2025.162865","DOIUrl":null,"url":null,"abstract":"<div><div>Electrocatalysis offers a promising approach for the oxidation of ethylene to high-value oxygenated products under ambient conditions, contributing to the balance between fossil energy consumption and environmental protection. However, the ethylene oxidation process requires conjunction with the oxygen evolution reaction (OER). In this study, first-principles calculations are employed to systematically investigate the catalytic performance of supported single-atom catalysts M/GDY for ethylene oxidation in OER-assisted. Our study focuses on using the adjustment of metal sites to influence the adsorption and activation of reaction intermediates, thereby regulating the reaction pathways and selectivity of final products in ethylene oxidation. The results show that Co, Cu, and Rh metal sites effectively stabilize the *OHCH<sub>2</sub>-CH<sub>2</sub>OH intermediate, promoting the formation of ethylene glycol oxidation products (HCOOH and OHCH<sub>2</sub>-COOH). Notably, the Rh/GDY catalyst exhibits excellent catalytic performance with a low voltage of 0.60 eV. Electronic structure analysis reveals that the interaction between the π electrons of ethylene and the metal atoms is crucial for ethylene activation. This study provides new insights into the mechanisms of ethylene oxidation and offers guidance for the development of efficient electrocatalysts.</div></div>","PeriodicalId":247,"journal":{"name":"Applied Surface Science","volume":"695 ","pages":"Article 162865"},"PeriodicalIF":6.9000,"publicationDate":"2025-03-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Single-atom M/GDY catalysts for electrochemical ethylene conversion via tandem water oxidation\",\"authors\":\"Yuanyuan Sun , Wen Zhao , Wei Cai , Yuhua Chi , Hao Ren , Zhongtao Li\",\"doi\":\"10.1016/j.apsusc.2025.162865\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Electrocatalysis offers a promising approach for the oxidation of ethylene to high-value oxygenated products under ambient conditions, contributing to the balance between fossil energy consumption and environmental protection. However, the ethylene oxidation process requires conjunction with the oxygen evolution reaction (OER). In this study, first-principles calculations are employed to systematically investigate the catalytic performance of supported single-atom catalysts M/GDY for ethylene oxidation in OER-assisted. Our study focuses on using the adjustment of metal sites to influence the adsorption and activation of reaction intermediates, thereby regulating the reaction pathways and selectivity of final products in ethylene oxidation. The results show that Co, Cu, and Rh metal sites effectively stabilize the *OHCH<sub>2</sub>-CH<sub>2</sub>OH intermediate, promoting the formation of ethylene glycol oxidation products (HCOOH and OHCH<sub>2</sub>-COOH). Notably, the Rh/GDY catalyst exhibits excellent catalytic performance with a low voltage of 0.60 eV. Electronic structure analysis reveals that the interaction between the π electrons of ethylene and the metal atoms is crucial for ethylene activation. This study provides new insights into the mechanisms of ethylene oxidation and offers guidance for the development of efficient electrocatalysts.</div></div>\",\"PeriodicalId\":247,\"journal\":{\"name\":\"Applied Surface Science\",\"volume\":\"695 \",\"pages\":\"Article 162865\"},\"PeriodicalIF\":6.9000,\"publicationDate\":\"2025-03-04\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Applied Surface Science\",\"FirstCategoryId\":\"88\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S0169433225005793\",\"RegionNum\":2,\"RegionCategory\":\"材料科学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Applied Surface Science","FirstCategoryId":"88","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S0169433225005793","RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Single-atom M/GDY catalysts for electrochemical ethylene conversion via tandem water oxidation
Electrocatalysis offers a promising approach for the oxidation of ethylene to high-value oxygenated products under ambient conditions, contributing to the balance between fossil energy consumption and environmental protection. However, the ethylene oxidation process requires conjunction with the oxygen evolution reaction (OER). In this study, first-principles calculations are employed to systematically investigate the catalytic performance of supported single-atom catalysts M/GDY for ethylene oxidation in OER-assisted. Our study focuses on using the adjustment of metal sites to influence the adsorption and activation of reaction intermediates, thereby regulating the reaction pathways and selectivity of final products in ethylene oxidation. The results show that Co, Cu, and Rh metal sites effectively stabilize the *OHCH2-CH2OH intermediate, promoting the formation of ethylene glycol oxidation products (HCOOH and OHCH2-COOH). Notably, the Rh/GDY catalyst exhibits excellent catalytic performance with a low voltage of 0.60 eV. Electronic structure analysis reveals that the interaction between the π electrons of ethylene and the metal atoms is crucial for ethylene activation. This study provides new insights into the mechanisms of ethylene oxidation and offers guidance for the development of efficient electrocatalysts.
期刊介绍:
Applied Surface Science covers topics contributing to a better understanding of surfaces, interfaces, nanostructures and their applications. The journal is concerned with scientific research on the atomic and molecular level of material properties determined with specific surface analytical techniques and/or computational methods, as well as the processing of such structures.