Similar rational design of catalysts is a paradigm shift of the old-fashioned trial and error discovery to the predictive mechanism-oriented development of catalytic systems with improved activity, selectivity and stability. This review article reviews the current state of catalyst design in many related aspects: active site engineering, at both the atomic and molecular scale, improved structure-activity relationship (SAR) studies through operando characterization methods, computational and machine learning methods of catalyst screening and optimization, and creating sustainable catalytic processes, with respect to the principles of green chemistry. We critically examine recent advances in single-atom catalysts (SACs), metal-organic frameworks (MOFs), defect-engineered materials, and bifunctional catalytic systems and how interdisciplinary integration of chemistry, materials science, and chemical engineering has spurred this development. Special attention is given to the emerging approaches based on the exploitation of designer-like methods, high-throughput experimentation, and data-driven approaches, to explore huge compositional and structural spaces. The review is concluded with a prospective outlook of the persisting challenges and opportunities such as catalyst design of electrochemical reduction of CO2, biomass valorization, and ambient-condition fixation of nitrogen.

Keywords catalyst design, structure-activity relationships, single-atom catalysts, computational catalysis, active site engineering, green catalysis, machine learning, operando characterization