Manipulating the Dynamic Proton Transport in Electrocatalysis at the Nanoscale

IF 13.1 1区 化学 Q1 CHEMISTRY, PHYSICAL ACS Catalysis Pub Date : 2025-02-27 DOI:10.1021/acscatal.5c00266
Lei Feng, Qin Liu, Guangyuan Xu, Min Ge, Wentuan Bi, Yi Huang, Jing Zhang, Xiaoye Liu, Si Chen, Fujing Nie, Zhendong Liu, Zhang Cai, Yuan Kong, Chengwei Wang, Junling Lu, Min Zhou, Huan Yan
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Abstract

Proton transport plays a crucial role in many hydrogen-based technologies. However, there is limited investigation on the manipulation of proton transport at the nanoscale, especially for the highly catalytic performance in electrocatalysis. Here, we encapsulated the polyoxometalate (POM, a well-known proton carrier) into the microchannel of a single-walled carbon nanotube (SWCNT) and selectively deposited the Pt clusters on the outside surface of the SWCNT, to establish a pseudo “proton shuttle” and achieve a fast proton transport and form a nanoscale “Pt–POM” kinetic coupling. With the enhanced proton transport, this proton nexus catalyst could accelerate the kinetic process of the probe reaction (hydrogen evolution reaction, HER) and outperform the counterparts. This strategy of manipulation of proton transport with the precise arrangement of functional sites is validated as a promising routine to obtain a highly catalytic performance in other proton-related electrocatalytic reactions.

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纳米级电催化中动态质子输运的操纵
质子输运在许多氢基技术中起着至关重要的作用。然而,在纳米尺度上操纵质子输运的研究有限,特别是对电催化中高催化性能的研究。本研究将质子载体多金属氧酸盐(POM)封装到单壁碳纳米管(SWCNT)的微通道中,并选择性地将Pt簇沉积在SWCNT的外表面,建立了一个伪“质子穿梭”,实现了质子的快速传输,形成了纳米尺度的“Pt - POM”动力学耦合。在质子输运增强的情况下,该质子联结催化剂可以加速探针反应(析氢反应,HER)的动力学过程,优于同类催化剂。这种通过精确安排功能位点来操纵质子输运的策略被证实是在其他质子相关的电催化反应中获得高催化性能的有希望的常规方法。
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阿拉丁
Trimethyl(methylcyclopentadienyl)-platinum(IV)
来源期刊
ACS Catalysis
ACS Catalysis CHEMISTRY, PHYSICAL-
CiteScore
20.80
自引率
6.20%
发文量
1253
审稿时长
1.5 months
期刊介绍: ACS Catalysis is an esteemed journal that publishes original research in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. It offers broad coverage across diverse areas such as life sciences, organometallics and synthesis, photochemistry and electrochemistry, drug discovery and synthesis, materials science, environmental protection, polymer discovery and synthesis, and energy and fuels. The scope of the journal is to showcase innovative work in various aspects of catalysis. This includes new reactions and novel synthetic approaches utilizing known catalysts, the discovery or modification of new catalysts, elucidation of catalytic mechanisms through cutting-edge investigations, practical enhancements of existing processes, as well as conceptual advances in the field. Contributions to ACS Catalysis can encompass both experimental and theoretical research focused on catalytic molecules, macromolecules, and materials that exhibit catalytic turnover.
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