Zhu Sheng, Xu Qian, Guan Chong, Chang Yunzhen, Han Gaoyi, Deng Bing
Institute of Molecular Science, Key Laboratory of Chemical Biology and Molecular Engineering of Education Ministry, Shanxi University, Taiyuan 030006, China.
Institute for Carbon-Based Thin Film Electronics, Peking University, Shanxi (ICTFE-PKU), Taiyuan 030012, China.
Nano Lett. 2025 Feb 26;25(8):3066-3074. doi: 10.1021/acs.nanolett.4c05097. Epub 2025 Jan 2.
Exploiting cost-effective hydrogen evolution reaction (HER) catalysts is crucial for sustainable hydrogen production. However, currently reported nanocatalysts usually cannot simultaneously sustain high catalytic activity and long-term durability. Here, we report the efficient synthesis and activity tailoring of a chainmail catalyst, isolated platinum atom anchored tungsten carbide nanocrystals encapsulated inside carbon nanotubes (Pt/WC@CNTs), by confined flash Joule heating technique. The instantaneous carbothermal reduction reaction enables the millisecond formation of Pt/WC nanostructures from CNT-encapsulated polyoxometalates, where nanotubes serve as both heating conductors and robust chainmails. The Pt/WC@CNTs exhibit prominent catalytic performance toward acid HER with a low overpotential of 45.2 mV at 10 mA cm and long-term durability over 500 h of continuous running. Mechanism studies reveal the strong metal-support interaction on Pt/WC optimizes the charge redistribution at the Pt-WC interface and the hydrogen adsorption/desorption behavior. This study offers a potential avenue for ultrafast and activity-controllable synthesis of highly stable single-atom catalysts.
开发具有成本效益的析氢反应(HER)催化剂对于可持续制氢至关重要。然而,目前报道的纳米催化剂通常无法同时保持高催化活性和长期耐久性。在此,我们报告了一种链甲催化剂的高效合成及其活性调控,该催化剂是通过受限快速焦耳加热技术制备的,即碳纳米管(Pt/WC@CNTs)包裹的孤立铂原子锚定碳化钨纳米晶体。瞬间的碳热还原反应使得能够在毫秒级内由碳纳米管包裹的多金属氧酸盐形成Pt/WC纳米结构,其中纳米管既作为热导体又作为坚固的链甲。Pt/WC@CNTs对酸性析氢反应表现出卓越的催化性能,在10 mA cm下过电位低至45.2 mV,并且在连续运行500多小时后仍具有长期耐久性。机理研究表明,Pt/WC上强大的金属-载体相互作用优化了Pt-WC界面处的电荷重新分布以及氢吸附/解吸行为。这项研究为超快且可调控活性地合成高度稳定的单原子催化剂提供了一条潜在途径。