Picello Silvia, Inico Elisabetta, Saetta Clara, Di Liberto Giovanni, Pacchioni Gianfranco
Department of Materials Science, University of Milano-Bicocca, Via Cozzi 55, 20125 Milano, Italy.
ACS Catal. 2025 Jun 13;15(13):11232-11242. doi: 10.1021/acscatal.5c01820. eCollection 2025 Jul 4.
In single-atom catalysis, the interaction between isolated metal atoms and the supporting matrix plays a crucial role in determining the stability and reactivity of the system. This has driven the search for supporting materials, particularly two-dimensional (2D) materials, where graphene has been the predominant choice. Simultaneously, increasing attention is being given to single-atom alloys (SAAs), a subclass of single-atom catalysts (SACs), where the supporting matrix itself is a metal. Recently, Kashiwaya et al. [ 744 (2024)] reported the synthesis of goldene, a 2D monolayer of Au(111) described as the gold analogue of graphene. Motivated by this breakthrough, we explored a class of SACs consisting of transition metal (TM) atoms stabilized on goldene. Through electronic structure calculations, we identified several systems that remain stable under both reducing and oxidizing conditions. We then investigated their catalytic performance in the hydrogen evolution reaction (HER) and oxygen evolution reaction (OER), discovering that certain TM-goldene systems exhibit promising activity, with reactivity significantly different from the same TMs supported on bulk Au(111). Our analysis included a comprehensive evaluation of potential reaction intermediates, extending beyond the conventional species typically assumed in HER and OER. This study provides strong theoretical evidence that SACs embedded in goldene could offer promising stability and catalytic reactivity.
在单原子催化中，孤立金属原子与支撑基质之间的相互作用对于确定体系的稳定性和反应活性起着关键作用。这推动了对支撑材料的探索，特别是二维（2D）材料，其中石墨烯一直是主要选择。同时，单原子合金（SAA）作为单原子催化剂（SAC）的一个子类，也越来越受到关注，在单原子合金中支撑基质本身就是一种金属。最近，柏谷等人[《自然》744（2024）]报道了合成金烯，一种被描述为石墨烯金类似物的二维单层Au(111)。受这一突破的启发，我们探索了一类由稳定在金烯上的过渡金属（TM）原子组成的SAC。通过电子结构计算，我们确定了几个在还原和氧化条件下都保持稳定的体系。然后，我们研究了它们在析氢反应（HER）和析氧反应（OER）中的催化性能，发现某些TM-金烯体系表现出有前景的活性，其反应活性与负载在块状Au(111)上的相同TMs有显著差异。我们的分析包括对潜在反应中间体的全面评估，超出了HER和OER中通常假设的传统物种。这项研究提供了有力的理论证据，表明嵌入金烯中的SAC可能具有有前景的稳定性和催化反应活性。
