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铂/富勒烯界面处铂位点的多样性加速了碱性析氢。

Diversity of platinum-sites at platinum/fullerene interface accelerates alkaline hydrogen evolution.

机构信息

Department of Chemical and Biomolecular Engineering, National University of Singapore, 4 Engineering Drive 4, Singapore, Singapore.

Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore, Singapore.

出版信息

Nat Commun. 2023 Mar 27;14(1):1711. doi: 10.1038/s41467-023-37404-0.

Abstract

Membrane-based alkaline water electrolyser is promising for cost-effective green hydrogen production. One of its key technological obstacles is the development of active catalyst-materials for alkaline hydrogen-evolution-reaction (HER). Here, we show that the activity of platinum towards alkaline HER can be significantly enhanced by anchoring platinum-clusters onto two-dimensional fullerene nanosheets. The unusually large lattice distance (0.8 nm) of the fullerene nanosheets and the ultra-small size of the platinum-clusters (2 nm) leads to strong confinement of platinum clusters accompanied by pronounced charge redistributions at the intimate platinum/fullerene interface. As a result, the platinum-fullerene composite exhibits 12 times higher intrinsic activity for alkaline HER than the state-of-the-art platinum/carbon black catalyst. Detailed kinetic and computational investigations revealed the origin of the enhanced activity to be the diverse binding properties of the platinum-sites at the interface of platinum/fullerene, which generates highly active sites for all elementary steps in alkaline HER, particularly the sluggish Volmer step. Furthermore, encouraging energy efficiency of 74% and stability were achieved for alkaline water electrolyser assembled using platinum-fullerene composite under industrially relevant testing conditions.

摘要

基于膜的碱性水电解器有望实现具有成本效益的绿色氢气生产。其关键技术障碍之一是开发用于碱性析氢反应 (HER) 的活性催化剂材料。在这里,我们表明,通过将铂簇锚定在二维富勒烯纳米片上,可以显著提高铂对碱性 HER 的活性。富勒烯纳米片的异常大晶格距离(约 0.8nm)和超小的铂簇尺寸(约 2nm)导致铂簇的强限域,同时在紧密的铂/富勒烯界面处发生明显的电荷重新分布。结果,铂-富勒烯复合材料在碱性 HER 中的本征活性比最先进的铂/碳黑催化剂高 12 倍。详细的动力学和计算研究揭示了增强活性的起源是铂位点在铂/富勒烯界面处的不同结合特性,这为碱性 HER 中所有元步骤,特别是缓慢的沃尔默步骤生成了高活性位点。此外,在工业相关测试条件下,使用铂-富勒烯复合材料组装的碱性水电解器实现了令人鼓舞的 74%能量效率和稳定性。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/a368/10042996/e267a02a8ae9/41467_2023_37404_Fig1_HTML.jpg

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