Self-assembly-assisted dynamic placement of noble metals selectively on multifunctional carbide supports for alkaline hydrogen electrocatalysis†

IF 32.4 1区 材料科学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Seongbeen Kim, Seung-Jae Shin, Hoyoung Kim, Bupmo Kim, Namgyu Noh, Kug-Seung Lee, Jinkyu Park, Hyunwoo Jun, Jiwon Kim, Jaeho Byeon, Seonggyu Lee, Huawei Huang, Sunghyun Noh, Han Beom Jeong, Jong Hyun Jang, Jong Min Yuk, Wooyul Kim, Hyungjun Kim and Jinwoo Lee
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Abstract

Atomically dispersed catalysts are ideal for alkaline hydrogen electrocatalysis with low noble metal loadings. However, previous designs have exhibited insufficient *OH binding and low cell performance, which limit their application in anion-exchange membrane water electrolyzers. In this study, we employed a self-assembly-assisted dynamic placement to prepare atomically dispersed electrocatalysts on heterostructured MoxC–C. The multifunctional MoxC support bolsters the dynamic placement while optimizing the interfacial water structure. The self-assembly-assisted dynamic placement facilitates the selective loading of atomically dispersed noble metals on MoxC at 1373 K by leveraging molecular interactions and metal–support interactions. The dynamic placement enables the construction of interfacial active systems between noble metals and MoxC, enhancing the reaction kinetics, stability, and CO tolerance of alkaline hydrogen electrocatalysis. Specifically, selective loading enables the effective utilization of *OH binding sites on MoxC, promoting water dissociation by increasing the free-water population in the interfacial water structure. In an anion-exchange membrane water electrolyzer, the designed catalysts exhibited higher cell stability (500 h) than commercial PtRu/C. They also exhibited enhanced performance even with a low noble metal loading (0.060 mgPt cm−2), achieving the US Department of Energy's 2026 target for proton-exchange membrane water electrolyzers.

Abstract Image

碱氢电催化中贵金属在多功能碳化物载体上的自组装辅助动态选择性放置
原子分散催化剂是理想的碱性氢电催化与低贵金属负载。然而,先前的设计表现出*OH结合不足和低电池性能,这限制了它们在阴离子交换膜水电解槽中的应用。在这项研究中,我们采用自组装辅助的动态放置方法在异质结构MoxC-C上制备了原子分散的电催化剂。多功能MoxC支架在优化界面水结构的同时加强了动态放置。自组装辅助动态放置通过利用分子相互作用和金属支持相互作用,促进了原子分散的贵金属在1373 K时选择性地负载在MoxC上。这种动态放置使得贵金属和MoxC之间的界面活性体系得以构建,增强了反应动力学、稳定性和碱性氢电催化的CO耐受性。具体来说,选择性加载可以有效利用MoxC上的*OH结合位点,通过增加界面水结构中的自由水数量来促进水的解离。在阴离子交换膜水电解槽中,所设计的催化剂比商用PtRu/C具有更高的电池稳定性(500 h)。即使在低贵金属负载(0.060 mgPt cm-2)的情况下,它们也表现出了更高的性能,实现了美国能源部2026年质子交换膜水电解槽的目标。
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来源期刊
Energy & Environmental Science
Energy & Environmental Science 化学-工程:化工
CiteScore
50.50
自引率
2.20%
发文量
349
审稿时长
2.2 months
期刊介绍: Energy & Environmental Science, a peer-reviewed scientific journal, publishes original research and review articles covering interdisciplinary topics in the (bio)chemical and (bio)physical sciences, as well as chemical engineering disciplines. Published monthly by the Royal Society of Chemistry (RSC), a not-for-profit publisher, Energy & Environmental Science is recognized as a leading journal. It boasts an impressive impact factor of 8.500 as of 2009, ranking 8th among 140 journals in the category "Chemistry, Multidisciplinary," second among 71 journals in "Energy & Fuels," second among 128 journals in "Engineering, Chemical," and first among 181 scientific journals in "Environmental Sciences." Energy & Environmental Science publishes various types of articles, including Research Papers (original scientific work), Review Articles, Perspectives, and Minireviews (feature review-type articles of broad interest), Communications (original scientific work of an urgent nature), Opinions (personal, often speculative viewpoints or hypotheses on current topics), and Analysis Articles (in-depth examination of energy-related issues).
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