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

IF 13.2 1区 工程技术 Q1 ENGINEERING, CHEMICAL
Ziqiang Tu, Xuan He, Xing Du, Weixin Li, Daheng Wang, Wei Fang, Haijun Zhang, Hui Chen, Lei Zhao, Cheng Wang
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引用次数: 0

摘要

铈基清除剂因其快速的Ce3+/Ce4+转化而被称为自由基清除剂。然而,长寿命质子交换膜燃料电池(PEMFC)的氧化还原能力和质子电导率的相容性是影响ce基自由基清除剂合理开发的关键因素。本研究通过在合成过程中引入乙酸,实现了具有缺失连接缺陷的Ce-UiO-66 (d-UiO-66)的合理设计。通过对d-UiO-66的氧化还原能力和质子电导率的系统研究表明,d-UiO-66中缺失的连接体缺陷一方面可以降低Ce3+/Ce4+可行转化的能垒,从而增强其自由基清除能力;另一方面,π电子的离域化也有利于π电子的离域化,这不仅有助于形成高密度的氢键形成,为质子的跳跃建立有效的途径,而且可以提高π电子的迁移率,实现质子的有效转移。因此,使用缺失连接自由基清除剂的单细胞测试支持改善的PEMFC性能,即使在开路电压测试100 小时后,其最高电压保持率(94% %)和最低极限功率退化率(约12.2 %)。概念验证表明,同时具有自由基清除效率和质子导电性,可以提高PEMFC的性能。
本文章由计算机程序翻译,如有差异,请以英文原文为准。
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.
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来源期刊
Chemical Engineering Journal
Chemical Engineering Journal 工程技术-工程:化工
CiteScore
21.70
自引率
9.30%
发文量
6781
审稿时长
2.4 months
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.
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