Hollow Pt-Encrusted RuCu Nanocages Optimizing OH Adsorption for Efficient Hydrogen Oxidation Electrocatalysis.

IF 16.1 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY Angewandte Chemie International Edition Pub Date : 2024-11-26 DOI:10.1002/anie.202420177
Licheng Wei, Yuanting Dong, Wei Yan, Yuqi Zhang, Changhong Zhan, Wei-Hsiang Huang, Chih-Wen Pao, Zhiwei Hu, Haixin Lin, Yong Xu, Hongbo Geng, Xiaoqing Huang
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Abstract

As one of the best candidates for hydrogen oxidation reaction (HOR), ruthenium (Ru) has attracted significant attention for anion exchange membrane fuel cells (AEMFCs), although it suffers from sluggish kinetics under alkaline conditions due to its strong hydroxide affinity. In this work, we develop ternary hollow nanocages with Pt epitaxy on RuCu (Pt-RuCu NCs) as efficient HOR catalysts for application in AEMFCs. Experimental characterizations and theoretical calculations confirm that the synergy in optimized Pt8.7-RuCu NCs significantly modifies the electronic structure and coordination environment of Ru, thereby balancing the binding strengths of H* and OH* species, which leads to a markedly enhanced HOR performance. Specifically, the optimized Pt8.7-RuCu NCs/C achieves a mass activity of 5.91 A mgPt+Ru-1, which is ~3.3, ~2.2, and ~15.0 times higher than that of RuCu NCs/C (1.38 A mgRu-1), PtRu/C (1.83 A mgPt+Ru-1) and Pt/C (0.37 A mgPt-1), respectively. Impressively, the specific peak power density of fuel cells reaches 15.9 W mgPt+Ru-1, significantly higher than those of most reported PtRu-based fuel cells.

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中空铂包壳 RuCu 纳米笼优化羟基吸附,实现高效氢氧化电催化。
作为氢氧化反应(HOR)的最佳候选催化剂之一,钌(Ru)在阴离子交换膜燃料电池(AEMFCs)中的应用备受关注,但由于其具有很强的氢氧化物亲和性,因此在碱性条件下会出现动力学迟缓的问题。在这项研究中,我们开发了在 RuCu 上外延铂的三元中空纳米笼(Pt-RuCu NCs),作为高效的 HOR 催化剂应用于 AEMFCs。实验表征和理论计算证实,优化的 Pt8.7-RuCu NCs 的协同作用显著改变了 Ru 的电子结构和配位环境,从而平衡了 H* 和 OH* 物种的结合强度,使 HOR 性能显著提高。具体而言,优化后的 Pt8.7-RuCu NCs/C 的质量活性达到 5.91 A mgPt+Ru-1,分别是 RuCu NCs/C(1.38 A mgRu-1)、PtRu/C(1.83 A mgPt+Ru-1)和 Pt/C (0.37 A mgPt-1)的约 3.3、约 2.2 和约 15.0 倍。令人印象深刻的是,燃料电池的比峰值功率密度达到 15.9 W mgPt+Ru-1,明显高于大多数已报道的铂钌基燃料电池。
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来源期刊
CiteScore
26.60
自引率
6.60%
发文量
3549
审稿时长
1.5 months
期刊介绍: Angewandte Chemie, a journal of the German Chemical Society (GDCh), maintains a leading position among scholarly journals in general chemistry with an impressive Impact Factor of 16.6 (2022 Journal Citation Reports, Clarivate, 2023). Published weekly in a reader-friendly format, it features new articles almost every day. Established in 1887, Angewandte Chemie is a prominent chemistry journal, offering a dynamic blend of Review-type articles, Highlights, Communications, and Research Articles on a weekly basis, making it unique in the field.
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