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Precise synthesis at the atomic scale is a highly desirable and controllable route for the preparation of heterogeneous catalysts with the desired structure and properties, which promotes the rational design of highly efficient catalysts and facilitates the understanding of structure-properties relationship. The precise construction of the active sites of the catalysts provides important opportunities for atomic insight into the correlation between structure and catalytic performance. In this review, the atomic-level tuning strategies for the precise synthesis of heterogeneous catalysts are summarized with the emphasis on the precise control of the structure of active sites, including single atom sites, dual atom sites and complex active sites. Furthermore, we illustrate the crucial role of atomic-level regulation of structure in determining the catalytic performance by providing typical catalysis examples in different reactions. In the end, some perspectives on the further development of precise synthesis of catalysts at the atomic level are presented.

The hydrosilylation reaction is one of the largest-scale application of homogeneous catalysis and is widely used to enable the commercial manufacture of silicon products. However, considerable issues including disposable platinum consumption, undesired side reactions and unacceptable catalyst residues still remain. Here, we synthesize a heterogeneous partially charged single-atom platinum supported on anatase TiO2 (Pt1 δ+/TiO2) catalyst via an electrostatic-induction ion exchange and twodimensional confinement strategy, which can catalyze hydrosilylation reaction with almost complete conversion and produce exclusive adduct. Density functional theory calculations reveal that unexpected property of Pt1 δ+/TiO2 originates from atomic dispersion of active species and unique partially positive charge Ptδ+ electronic structure that conventional nanocatalysts do not possess. The fabrication of single-atom Pt1 δ+/TiO2 catalyst accomplishes a reasonable use of Pt through recycling and maximum atom-utilized efficiency, indicating the potential to achieve a green hydrosilylation industry. [ABSTRACT FROM AUTHOR]