单原子合金的基本原理和催化应用

Fundamentals and catalytic applications of single-atom alloys

在惰性金属表面掺入原子级分散催化活性金属制备而成的单原子合金近年来引起了科研界的极大关注.单原子合金表面独特的几何和电子性质加速了反应物分子的解离并弱化了中间物种的吸附,使其在诸多催化反应中表现出高活性和高选择性.本文总结了单原子合金的结构特征和催化反应性能的最新进展.我们首先列举了一系列单原子合金的可控合成方法,并进一步总结了高端表征技术,特别是原位光谱技术用于识别单原子合金中活性金属原子的几何和电子结构的方法.然后,我们结合多种催化反应,深入探究了单原子合金的几何与电子特性与催化性能之间的构效关系.最后探讨了单原子合金当前面临的挑战和未来的前景.

Single-atom alloys that consist of a catalytically active metal atomically dispersed in a less-catalytic metal host have recently attracted significant concern from worldwide researchers.The unique geometric and electronic properties of single-atom alloys enable both facile dissociation of reactants and weak adsorption of intermediates on the surface,re-presenting two highly desirable elements for efficient and se-lective catalysis.This review article provides an overview of recent progress in the synthesis and properties of single-atom alloys in heterogeneous catalysis.First,we summarize recent advances in the controllable synthesis of single-atom alloys with various metal combinations.Second,we introduce key characterization techniques,especially operando spectroscopic techniques for the identification of the geometric and elec-tronic structures of diluted active metal atoms in single-atom alloys.Then,we discuss how these geometric and electronic properties of single-atom alloys affect their catalytic perfor-mances and thoroughly comprehend the reaction mechanism.Finally,insights into the current challenges and future pro-spects of single-atom alloys are provided.