Wang Ke, Quan Xu, Cao Ning, Bao Ying, Li Wenbo, Yan Mi, Dai Sheng, Xie Pengfei
College of Chemical and Biological Engineering, Zhejiang University, Hangzhou, 310058, China.
Institute of Zhejiang University-Quzhou, Quzhou, 324000, China.
Small. 2025 Sep;21(35):e2505626. doi: 10.1002/smll.202505626. Epub 2025 Jul 9.
The photocatalytic conversion of CO and pure HO to ethanol has been challenged by low light utilization and sluggish C─C coupling kinetics. Here, single-atom AuCu alloys are synthesized with enhanced localized surface plasmon resonance (LSPR) effects. A strong chemical interaction is probed as electron transfer from the atomic Au site to the adjacent Cu host, giving rise to electron rearrangement and an upshift of the d band center toward the Fermi level of Cu nanoparticles. As a result, the high electron occupancy state in AuCu alloy is excited to abundant hot charge carriers under illumination. The catalyst with an optimal amount of gold dopants delivers an excellent ethanol yield of 940 µmol g h and a selectivity of 92.5% with outstanding stability exceeding 100 h. The structure-reactivity correlation and mechanism studies reveal that the LSPR effect induced by the doping of single-atom Au not only enhances light adsorption but also improves the accumulation of CO intermediates, which accounts for the reduced energy barrier for C─C coupling toward ethanol formation.
一氧化碳（CO）和纯过氧化氢（HO）光催化转化为乙醇一直受到低光利用率和缓慢的碳-碳偶联动力学的挑战。在此，合成了具有增强的局域表面等离子体共振（LSPR）效应的单原子金铜合金。研究发现，从金原子位点到相邻铜主体存在强烈的化学相互作用，导致电子重排以及d带中心向铜纳米颗粒的费米能级上移。结果，在光照下，金铜合金中的高电子占据态被激发为丰富的热载流子。具有最佳金掺杂量的催化剂实现了940 μmol g h的优异乙醇产率和92.5%的选择性，且具有超过100小时的出色稳定性。结构-反应活性相关性和机理研究表明，单原子金掺杂诱导的LSPR效应不仅增强了光吸附，还改善了CO中间体的积累，这是碳-碳偶联生成乙醇的能垒降低的原因。
