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源自葫芦[6]脲的铱钼纳米团簇掺杂多孔碳电催化剂助力高效碱性析氢反应

IrMo Nanocluster-Doped Porous Carbon Electrocatalysts Derived from Cucurbit[6]uril Boost Efficient Alkaline Hydrogen Evolution.

作者信息

Xiao Xin, Li Zheng, Xiong Ying, Yang Ying-Wei

机构信息

College of Chemistry, Liaoning University, Shenyang 110036, P. R. China.

International Joint Research Laboratory of Nano-Micro Architecture Chemistry, College of Chemistry, Jilin University, 2699 Qianjin Street, Changchun 130012, P. R. China.

出版信息

J Am Chem Soc. 2023 Aug 2;145(30):16548-16556. doi: 10.1021/jacs.3c03489. Epub 2023 Jul 19.

Abstract

Electrocatalysts based on noble metals have been proven efficient for high-purity hydrogen production. However, the sluggish kinetics of the hydrogen evolution reaction (HER) in alkaline media caused by high water dissociation energy largely hampers this electrochemical process. To improve the electrocatalytic activity, we fabricate an effective porous carbon matrix derived from cucurbit[6]uril using a template-free method to support iridium-molybdenum (IrMo) nanoclusters. As proof of concept, the resulting IrMo-doped carbon electrocatalyst (IrMo-CBC) was found to boost the alkaline HER significantly. Owing to the unique in-plane hole structure and the nitrogen-rich backbone of cucurbit[6]uril as well as the ultrafine IrMo nanoclusters, IrMo-CBC exhibits pronounced alkaline HER activity with an extremely low overpotential of 12 mV at 10 mA cm, an ultrasmall Tafel slope (28.06 mV dec), a superior faradic efficiency (98%), and a TOF of 11.6 H s at an overpotential of 50 mV, outperforming most iridium-based electrocatalysts and commercial Pt/C.

摘要

基于贵金属的电催化剂已被证明对高纯度制氢有效。然而,由高水解离能导致的碱性介质中析氢反应(HER)缓慢动力学在很大程度上阻碍了这一电化学过程。为了提高电催化活性,我们采用无模板法制备了一种由葫芦[6]脲衍生的有效多孔碳基质,以负载铱-钼(IrMo)纳米团簇。作为概念验证,发现所得的IrMo掺杂碳电催化剂(IrMo-CBC)能显著促进碱性析氢反应。由于葫芦[6]脲独特的面内孔结构、富含氮的主链以及超精细的IrMo纳米团簇,IrMo-CBC在10 mA cm时表现出显著的碱性析氢活性,过电位极低,仅12 mV,塔菲尔斜率超小(28.06 mV dec),法拉第效率优异(98%),在50 mV过电位下的TOF为11.6 H s,性能优于大多数铱基电催化剂和商业Pt/C。

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