Emerging Strategies for the Synthesis of Correlated Single Atom Catalysts

People have been looking for an energy-efficient and sustainable method to produce future chemicals for decades. Heterogeneous single-atom catalysts (SACs) with atomic dispersion of robust, well-characterized active centers are highly desirable. In particular, correlated SACs with cooperative interaction between adjacent single atoms allow the switching of the single-site pathway to the dual or multisite pathway, thus promoting bimolecular or more complex reactions for the synthesis of fine chemicals. Herein, the structural uniqueness of correlated SACs, including the intermetal distance and electronic interaction in homo/heteronuclear metal sites is featured. Recent advances in the production methods of correlated SACs, showcasing the research status and challenges in traditional methods (such as pyrolysis, wet impregnation, and confined synthesis) for building a comprehensive multimetallic SAC library, are summarized. Emerging strategies such as process automation and continuous-flow synthesis are highlighted, minimizing the inconsistency in laboratory batch production and allowing high throughput screening and upscaling toward the next-stage chemical production by correlated SACs. In this review, the research status and synthetic challenges in correlated single-atom catalysts (SACs) are showcased. Existing strategies, such as the regulation of nucleation kinetics, nanoscale confinement, defect-assisted metal trapping, precise control via ligand chemistry, and stepwise deposition, are highlighted. A complementary perspective on emerging methods is provided for high throughput screening and upscaling toward the next-stage catalyst production. image