Rationally Designed Asymmetric Pt─O─Cu Ligand to Stabilize Active Sites Towards Superior Industrial-Standard Alkaline Hydrogen Evolution

IF 16.9 1区 化学 Q1 CHEMISTRY, MULTIDISCIPLINARY
Minming Jiang, Prof. Jiang Xu, Qi Zhou, Prof. Yujie Chen, Prof. Paul Munroe, Prof. Linlin Li, Prof. Zong-Han Xie, Prof. Yuping Wu, Prof. Shengjie Peng
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Abstract

Developing efficient and durable Pt-based catalysts via interface engineering remains a critical yet challenging task for water electrolysis under high-pH conditions. Herein, we design a unique asymmetric Pt─O─Cu ligand at the PtCu2(111)/CuO(002) heterojunction interface to promote alkaline HER kinetics. This ligand balances the adsorption and desorption of H* on the Pt site by accelerating electron transfer at the interface while enhancing the adsorption of H2O on the Cu site. Moreover, the strong d-d/sp hybridization and more delocalized d-DOS located at the Pt─O─Cu ligand enhance the interatomic interactions, which helps alleviate the dissolution and agglomeration of Pt and Cu atoms. As anticipated, the PtCu2/CuO requires ultra-low overpotentials of 10, 14 and 47 mV in, respectively, alkaline, acidic and neutral electrolytes to achieve a current density of 10 mA cm−2. Even more surprising is that the PtCu2/CuO||RuO2 dual-electrode hydrolysis cell can stably operate at a high current density of 1 A cm−2 for more than 500 h in a simulated industrial environment, demonstrating significant potential for industrial applications. This work provides a new paradigm for the design of industrially relevant high-performance Pt-based alkaline hydrogen evolution catalytic materials.

Abstract Image

合理设计不对称Pt-O-Cu配体,稳定活性位点,实现工业标准碱性析氢
通过界面工程开发高效耐用的pt基催化剂仍然是高ph条件下水电解的一个关键而具有挑战性的任务。在此,我们在PtCu2(111)/CuO(002)异质结界面设计了一种独特的不对称Pt-O-Cu配体,以促进碱性HER动力学。该配体通过加速界面上的电子转移来平衡H*在Pt位点上的吸附和解吸,同时增强H2O在Cu位点上的吸附。此外,Pt- o -Cu配体上的强d-d/sp杂化和更多的离域d-DOS增强了原子间的相互作用,有助于减轻Pt和Cu原子的溶解和团聚。正如预期的那样,PtCu2/CuO在碱性、酸性和中性电解质中分别需要10、14和47 mV的超低过电位才能达到10 mA cm−2的电流密度。更令人惊讶的是,在模拟工业环境中,PtCu2/CuO||RuO2双电极水解电池可以在1 a cm−2的高电流密度下稳定工作超过500小时,显示出巨大的工业应用潜力。本研究为工业相关的高性能pt基碱性析氢催化材料的设计提供了新的范例。
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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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