Ziqiang Tu, Xuan He, Xing Du, Weixin Li, Daheng Wang, Wei Fang, Haijun Zhang, Hui Chen, Lei Zhao, Cheng Wang
{"title":"Ce-UiO-66缺失连接缺陷对质子交换膜燃料电池自由基清除效率和质子电导率的影响","authors":"Ziqiang Tu, Xuan He, Xing Du, Weixin Li, Daheng Wang, Wei Fang, Haijun Zhang, Hui Chen, Lei Zhao, Cheng Wang","doi":"10.1016/j.cej.2025.159357","DOIUrl":null,"url":null,"abstract":"Ce-based scavengers are well known as free radical scavengers due to its fast Ce<sup>3+</sup>/Ce<sup>4+</sup> conversion. However, the compatibility of redox capability and proton conductivity for long-life proton exchange membrane fuel cells (PEMFC) is a crucial consideration relevant to the rational development of Ce-based radical scavengers. In this study, the rational design of Ce-UiO-66 (d-UiO-66) with missing-linker defects was achieved by introducing acetic acid during the synthesis. The systematical investigation referring to redox capability and proton conductivity of d-UiO-66 demonstrated that, on one hand, the missing-linker defects in d-UiO-66 can reduce the energy barrier for the feasible Ce<sup>3+</sup>/Ce<sup>4+</sup> conversion to enhance the free radical scavenging performance. On the other hand, it is also benefit for the delocalization of π-electron, which not only contributes to form hydrogen bonds formation with high density to establish effective pathways for proton hopping, but also gives rise to the enhanced mobility of π-electrons for the efficient proton transfer. Consequently, single-cell testing with missing-linker radical scavengers supports improved PEMFC performance with the highest voltage retention (94 %) and the lowest degradation of limiting powers around 12.2 % even after 100 h of open circuit voltage testing. The proof-of-concept demonstrates the potential of concurrent radical scavenging efficiency and proton conductivity for advancing PEMFC performance.","PeriodicalId":270,"journal":{"name":"Chemical Engineering Journal","volume":"14 3 1","pages":""},"PeriodicalIF":13.2000,"publicationDate":"2025-01-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Missing-linker defects of Ce-UiO-66 for enhanced radical scavenging efficiency and proton conductivity in proton exchange membrane fuel cells\",\"authors\":\"Ziqiang Tu, Xuan He, Xing Du, Weixin Li, Daheng Wang, Wei Fang, Haijun Zhang, Hui Chen, Lei Zhao, Cheng Wang\",\"doi\":\"10.1016/j.cej.2025.159357\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"Ce-based scavengers are well known as free radical scavengers due to its fast Ce<sup>3+</sup>/Ce<sup>4+</sup> conversion. However, the compatibility of redox capability and proton conductivity for long-life proton exchange membrane fuel cells (PEMFC) is a crucial consideration relevant to the rational development of Ce-based radical scavengers. In this study, the rational design of Ce-UiO-66 (d-UiO-66) with missing-linker defects was achieved by introducing acetic acid during the synthesis. The systematical investigation referring to redox capability and proton conductivity of d-UiO-66 demonstrated that, on one hand, the missing-linker defects in d-UiO-66 can reduce the energy barrier for the feasible Ce<sup>3+</sup>/Ce<sup>4+</sup> conversion to enhance the free radical scavenging performance. On the other hand, it is also benefit for the delocalization of π-electron, which not only contributes to form hydrogen bonds formation with high density to establish effective pathways for proton hopping, but also gives rise to the enhanced mobility of π-electrons for the efficient proton transfer. Consequently, single-cell testing with missing-linker radical scavengers supports improved PEMFC performance with the highest voltage retention (94 %) and the lowest degradation of limiting powers around 12.2 % even after 100 h of open circuit voltage testing. The proof-of-concept demonstrates the potential of concurrent radical scavenging efficiency and proton conductivity for advancing PEMFC performance.\",\"PeriodicalId\":270,\"journal\":{\"name\":\"Chemical Engineering Journal\",\"volume\":\"14 3 1\",\"pages\":\"\"},\"PeriodicalIF\":13.2000,\"publicationDate\":\"2025-01-06\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Chemical Engineering Journal\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://doi.org/10.1016/j.cej.2025.159357\",\"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://doi.org/10.1016/j.cej.2025.159357","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}
Missing-linker defects of Ce-UiO-66 for enhanced radical scavenging efficiency and proton conductivity in proton exchange membrane fuel cells
Ce-based scavengers are well known as free radical scavengers due to its fast Ce3+/Ce4+ conversion. However, the compatibility of redox capability and proton conductivity for long-life proton exchange membrane fuel cells (PEMFC) is a crucial consideration relevant to the rational development of Ce-based radical scavengers. In this study, the rational design of Ce-UiO-66 (d-UiO-66) with missing-linker defects was achieved by introducing acetic acid during the synthesis. The systematical investigation referring to redox capability and proton conductivity of d-UiO-66 demonstrated that, on one hand, the missing-linker defects in d-UiO-66 can reduce the energy barrier for the feasible Ce3+/Ce4+ conversion to enhance the free radical scavenging performance. On the other hand, it is also benefit for the delocalization of π-electron, which not only contributes to form hydrogen bonds formation with high density to establish effective pathways for proton hopping, but also gives rise to the enhanced mobility of π-electrons for the efficient proton transfer. Consequently, single-cell testing with missing-linker radical scavengers supports improved PEMFC performance with the highest voltage retention (94 %) and the lowest degradation of limiting powers around 12.2 % even after 100 h of open circuit voltage testing. The proof-of-concept demonstrates the potential of concurrent radical scavenging efficiency and proton conductivity for advancing PEMFC performance.
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.