He Hongzhe, Ren Xiaoqiong, Zhang Ruoqun, Yang Sasha, Gu Jinxing, Wang Ke, Qian Binbin, Chen Ning, Zhang Lian, Yu Jianglong, Cheng Yuan, Dai Baiqian
Department of Chemical and Biological Engineering, Monash University, Victoria, 3800, Australia.
Suzhou Industry Park Monash Suzhou Research Institute, Suzhou Industry Park, Suzhou, 215123, China.
Adv Sci (Weinh). 2025 Aug 27:e11806. doi: 10.1002/advs.202511806.
Pt-group metal single-atom catalysts (SACs) with a large single-atom areal density are highly desirable for efficient electrocatalysis but remain challenging to synthesize. Herein, a facile vacuum direct current arc discharge (DCAD) strategy is reported for the rapid and scalable synthesis of Pt SACs with an unprecedented areal density of 10.6 atoms nm (3.82 wt.% Pt loading) firmly anchored on CoNi nanoalloy and confined by carbon nanotubes (CoNiPt@G). Notably, due to the strong electron trapping effect between Pt SA and CoNi substrates, CoNiPt@G retains its structural integrity at 1000 °C, demonstrating an outstanding thermal stability despite the ultra-high areal density. Moreover, the DCAD strategy is universal, which can be applied to other metals such as Iridium. It is also scalable, with a demonstrated gram-scale yield achieved within 0.5 h. The resulting CoNiPt@G catalyst exhibits exceptional hydrogen evolution reaction performance, achieving an overpotential of 23 mV at 10 mA cm, a mass activity over 5 times higher than that of 20 wt.% Pt/C catalyst and high stability during the 120 h test. This work provides a groundbreaking pathway for the large-scale production of high single-atom areal density, thermally robust SACs, advancing their practical applications in clean energy technologies.
具有大的单原子面密度的铂族金属单原子催化剂(SACs)对于高效电催化非常理想,但合成仍具有挑战性。在此,报道了一种简便的真空直流电弧放电(DCAD)策略,用于快速且可扩展地合成铂单原子催化剂,其具有前所未有的10.6个原子/纳米²的面密度(铂负载量为3.82 wt.%),牢固地锚定在钴镍纳米合金上并被碳纳米管限制(CoNiPt@G)。值得注意的是,由于铂单原子与钴镍基底之间的强电子俘获效应,CoNiPt@G在1000℃时仍保持其结构完整性,尽管面密度超高,但仍表现出出色的热稳定性。此外,DCAD策略具有通用性,可应用于其他金属,如铱。它也具有可扩展性,在0.5小时内实现了克级产量。所得的CoNiPt@G催化剂表现出优异的析氢反应性能,在10 mA/cm²时过电位为23 mV,质量活性比20 wt.%的铂碳催化剂高5倍以上,并且在120小时测试中具有高稳定性。这项工作为大规模生产高单原子面密度、热稳定性强的单原子催化剂提供了一条开创性途径,推动了它们在清洁能源技术中的实际应用。