Ze Lin , Yahui Li , Ruilong Li , Xingen Lin , Bincheng Xu , Zhixuan Chen , Yuen Wu , Ying Wang
{"title":"缺陷工程诱导碳点上的高金属负载共单原子催化剂用于高效 H2O2 电合成","authors":"Ze Lin , Yahui Li , Ruilong Li , Xingen Lin , Bincheng Xu , Zhixuan Chen , Yuen Wu , Ying Wang","doi":"10.1016/j.cej.2024.157661","DOIUrl":null,"url":null,"abstract":"<div><div>Co-single atom catalysts (Co-SACs) exhibit high selectivity and efficiency for H<sub>2</sub>O<sub>2</sub> electrosynthesis via the two-electron oxygen reduction reaction (2e<sup>−</sup>ORR), with the catalytic activity as significantly influenced by the loading content of Co atoms. However, the loading of Co atoms is typically confined to a low level (<1.0 wt%), which restricts their overall catalytic performance. Herein, we proposed a defect engineering strategy that utilized the carbon dots (CDs) as a platform to capture Co atoms, and constructed a series of Co-SACs with high Co atoms loading (with a maximum of 6.16 wt%), representing a substantial improvement compared to existing benchmarks in the literature. Experimental and characterization results revealed that the defect sites on CDs allowed adequate spacing between the Co atoms, effectively preventing their aggregation and promoting the generation of highly loaded metal atoms. It is worth noting that ECDs-CoSA demonstrated remarkable efficacy and catalytic activity with 93.70 % H<sub>2</sub>O<sub>2</sub> selectivity and an impressive H<sub>2</sub>O<sub>2</sub> yield of 9.71 mol L<sup>−1</sup> h<sup>−1</sup> g<sub>cat.</sub><sup>−1</sup> in neutral condition. This study presents an effective route for the controlled prepared of Co-SACs with high metal loading, aiming at sustainable and the efficient H<sub>2</sub>O<sub>2</sub> electrosynthesis.</div></div>","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"501 ","pages":"Article 157661"},"PeriodicalIF":13.3000,"publicationDate":"2024-11-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Defect engineering induced high metal loading Co-single-atom catalyst on carbon dots for efficient H2O2 electrosynthesis\",\"authors\":\"Ze Lin , Yahui Li , Ruilong Li , Xingen Lin , Bincheng Xu , Zhixuan Chen , Yuen Wu , Ying Wang\",\"doi\":\"10.1016/j.cej.2024.157661\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Co-single atom catalysts (Co-SACs) exhibit high selectivity and efficiency for H<sub>2</sub>O<sub>2</sub> electrosynthesis via the two-electron oxygen reduction reaction (2e<sup>−</sup>ORR), with the catalytic activity as significantly influenced by the loading content of Co atoms. However, the loading of Co atoms is typically confined to a low level (<1.0 wt%), which restricts their overall catalytic performance. Herein, we proposed a defect engineering strategy that utilized the carbon dots (CDs) as a platform to capture Co atoms, and constructed a series of Co-SACs with high Co atoms loading (with a maximum of 6.16 wt%), representing a substantial improvement compared to existing benchmarks in the literature. Experimental and characterization results revealed that the defect sites on CDs allowed adequate spacing between the Co atoms, effectively preventing their aggregation and promoting the generation of highly loaded metal atoms. It is worth noting that ECDs-CoSA demonstrated remarkable efficacy and catalytic activity with 93.70 % H<sub>2</sub>O<sub>2</sub> selectivity and an impressive H<sub>2</sub>O<sub>2</sub> yield of 9.71 mol L<sup>−1</sup> h<sup>−1</sup> g<sub>cat.</sub><sup>−1</sup> in neutral condition. This study presents an effective route for the controlled prepared of Co-SACs with high metal loading, aiming at sustainable and the efficient H<sub>2</sub>O<sub>2</sub> electrosynthesis.</div></div>\",\"PeriodicalId\":270,\"journal\":{\"name\":\"Chemical Engineering Journal\",\"volume\":\"501 \",\"pages\":\"Article 157661\"},\"PeriodicalIF\":13.3000,\"publicationDate\":\"2024-11-14\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chemical Engineering Journal\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1385894724091526\",\"RegionNum\":1,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q1\",\"JCRName\":\"ENGINEERING, CHEMICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Chemical Engineering Journal","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1385894724091526","RegionNum":1,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q1","JCRName":"ENGINEERING, CHEMICAL","Score":null,"Total":0}
Defect engineering induced high metal loading Co-single-atom catalyst on carbon dots for efficient H2O2 electrosynthesis
Co-single atom catalysts (Co-SACs) exhibit high selectivity and efficiency for H2O2 electrosynthesis via the two-electron oxygen reduction reaction (2e−ORR), with the catalytic activity as significantly influenced by the loading content of Co atoms. However, the loading of Co atoms is typically confined to a low level (<1.0 wt%), which restricts their overall catalytic performance. Herein, we proposed a defect engineering strategy that utilized the carbon dots (CDs) as a platform to capture Co atoms, and constructed a series of Co-SACs with high Co atoms loading (with a maximum of 6.16 wt%), representing a substantial improvement compared to existing benchmarks in the literature. Experimental and characterization results revealed that the defect sites on CDs allowed adequate spacing between the Co atoms, effectively preventing their aggregation and promoting the generation of highly loaded metal atoms. It is worth noting that ECDs-CoSA demonstrated remarkable efficacy and catalytic activity with 93.70 % H2O2 selectivity and an impressive H2O2 yield of 9.71 mol L−1 h−1 gcat.−1 in neutral condition. This study presents an effective route for the controlled prepared of Co-SACs with high metal loading, aiming at sustainable and the efficient H2O2 electrosynthesis.
期刊介绍:
The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.