Zou Sibei, Liang Yuhang, Zhang Xingmo, Gu Qinfen, Wang Lizhuo, Sun Haoyue, Liao Xiaozhou, Huang Jun, Masri Assaad R
Department: School of Aerospace, Mechanical and Mechatronic Engineering, Institution: The University of Sydney, J07 The University of Sydney, New South Wales, 2006, Australia.
Department: School of Chemical and Biomolecular Engineering, Institution: The University of Sydney, J01 The University of Sydney, New South Wales, 2006, Australia.
Angew Chem Int Ed Engl. 2025 Jan 2;64(1):e202412835. doi: 10.1002/anie.202412835. Epub 2024 Oct 25.
Single-atom alloy (SAA) catalysts exhibit huge potential in heterogeneous catalysis. Manufacturing SAAs requires complex and expensive synthesis methods to precisely control the atomic scale dispersion to form diluted alloys with less active sites and easy sintering of host metal, which is still in the early stages of development. Here, we address these limitations with a straightforward strategy from a brand-new perspective involving the 'islanding effect' for manufacturing SAAs without dilution: homogeneous RuNi alloys were continuously refined to highly dispersed alloy-islands (~1 nm) with completely single-atom sites where the relative metal loading was as high as 40 %. Characterized by advanced atomic-resolution techniques, single Ru atoms were bonded with Ni as SAAs with extraordinary long-term stability and no sintering of the host metal. The SAAs exhibited 100 % CO selectivity, over 55 times reverse water-gas shift (RWGS) rate than the alloys with Ru cluster sites, and over 3-4 times higher than SAAs by the dilution strategy. This study reports a one-step manufacturing strategy for SAA's using the wetness impregnation method with durable high atomic efficiency and holds promise for large-scale industrial applications.
单原子合金（SAA）催化剂在多相催化中展现出巨大潜力。制造单原子合金需要复杂且昂贵的合成方法，以精确控制原子尺度的分散，从而形成活性位点较少且主体金属易烧结的稀释合金，目前该领域仍处于发展初期。在此，我们从一个全新的角度采用一种直接的策略来解决这些限制，该策略涉及用于制造无稀释单原子合金的“岛状效应”：将均匀的RuNi合金连续精炼成高度分散的合金岛（约1纳米），这些合金岛具有完全的单原子位点，其中相对金属负载量高达40%。通过先进的原子分辨率技术表征，单个Ru原子与Ni键合形成具有非凡长期稳定性且主体金属不烧结的单原子合金。这些单原子合金表现出100%的CO选择性，逆水煤气变换（RWGS）速率比具有Ru簇位点的合金高出55倍以上，比通过稀释策略制备的单原子合金高出3 - 4倍以上。本研究报道了一种使用湿浸渍法制备单原子合金的一步制造策略，具有持久的高原子效率，并有望实现大规模工业应用。
