Influencing electrocatalytic processes through topographically disordered atomic sites

Catalysts saturated with highly reactive under-coordinated disordered atomic sites have been leveraged upon as high-performance electrode materials that are capable of alleviating activation energy barriers and promoting reaction kinetics as well as product selectivity across diverse electrocatalytic reactions. Surface discontinuities have significant influence on the catalytic behavior of electrode materials. However, a thorough understanding of these imperfections at the atomistic level is still far away and lacking. Herein, recent advances in the tailoring of nanomaterials from the aspect of introducing disordered atomic sites to attain superior catalytic performances are summarized, focusing on key reactions in electrocatalysis, including oxygen reduction reaction (ORR), oxygen evolution reaction (OER), hydrogen evolution reaction (HER), and carbon dioxide reduction reaction (CO2RR). Reaction mechanisms, insights from advanced characterization techniques, and theoretical perspectives are discussed, providing valuable atomistic-level understanding of topographically disordered materials for electrocatalysis. Finally, key challenges that lie ahead and future directions for further development of improved functional materials, bearing the tailored atomically disordered sites, are rationalized.