Fundamentals of Activity and Stability in Heterogeneous Catalysis

Recommendations H eterogeneous catalysis plays a central role in addressing many of today's scientific and technological challenges, from sustainable chemical manufacturing and energy conversion to environmental remediation.Despite remarkable advances in catalyst design, achieving both high catalytic activity and long-term stability remains one of the defining challenges of the field.Addressing this challenge requires a fundamental understanding of catalytic processes across multiple length and time scales, supported by close integration between experimental characterization and computational simulation.This Special Issue originated from discussions at the ACS Physical Chemistry Summit, held in April 2024 at the University of Science and Technology of China in Hefei, China.The meeting brought together researchers from experimental and theoretical chemistry to exchange ideas on the fundamental principles governing catalytic activity, catalyst stability, and their intricate relationship.The lively discussions highlighted the importance of combining complementary approaches to reveal reaction mechanisms and guide the rational design of next-generation catalysts.Continuing these conversations, this Special Issue assembles more than 30 articles, including Perspectives, Viewpoints, Mini-Reviews, Letters, and original Research Articles that showcase recent advances in heterogeneous catalysis, computational methodologies, in situ characterization techniques, and other future research directions.A major theme emerging from this collection is the rational design of single-atom catalysts (SACs) and supported metal catalysts that simultaneously enhance catalytic performance and structural stability.SACs continue to attract significant attention because they maximize metal utilization while offering well-defined active sites for mechanistic investigations.Xu and co-workers demonstrate how introducing hemilabile coordination into heterogeneous SACs can overcome limitations imposed by conventional scaling relationships, providing a promising strategy for designing more efficient catalytic systems (DOI: 10.1021/acs.jpclett.5c00416).Shi and co-workers investigate transition metal (Mn, Fe, and Co) atoms anchored on N 4 -doped graphene and reveal a dual-path stabilization mechanism that enhances catalyst durability (DOI: 10.1021/acs.jpcc.5c08433).Wen, Li, and co-workers employ a grain-boundary engineering strategy to construct MoS 2 -supported SACs for electrocatalytic CO 2 reduction, illustrating how atomic-scale structural engineering can improve both activity and stability (DOI: 10.1021/acs.jp- clett.5c03749).Another prominent theme is the continued development of advanced computational methods for understanding catalytic