催化剂筛选：火山型曲线成因理论解析及其在多相催化中的应用.pdfVIP

Chinese Journal of Catalysis 36 (2015) 1596–1605 催化学报 2015年 第36卷 第9期 | a v a i l a b l e a t w w w . s c i e n c e d i r e c t . c o m j o u r n a l h o m e p a g e : w w w . e l s e v i e r . c o m / l o c a t e / c h n j c Article (Special Issue for Excellent Research Work in Recognition of Scientists Who Are in Catalysis Field in China) Catalyst screening: Refinement of the origin of the volcano curve and its implication in heterogeneous catalysis Yu Mao a, Jianfu Chen a, Haifeng Wang a,*, P. Hu a,b a Key Laboratory for Advanced Materials, Research Institute of Industrial Catalysis and Centre for Computational Chemistry, East China University of Science and Technology, Shanghai 200237, China b School of Chemistry and Chemical Engineering, The Queen’s University of Belfast Belfast BT9 5AG, United Kingdom A R T I C L E I N F O A B S T R A C T Article history: Received 1 April 2015 Accepted 27 April 2015 Published 20 September 2015 Understanding the overall catalytic activity trend for rational catalyst design is one of the core goals in heterogeneous catalysis. In the past two decades, the development of density functional theory (DFT) and surface kinetics make it feasible to theoretically evaluate and predict the catalytic activity variation of catalysts within a descriptor-based framework. Thereinto, the concept of the volcano curve, which reveals the general activity trend, usually constitutes the basic foundation of catalyst screening. However, although it is a widely accepted concept in heterogeneous catalysis, its origin lacks a clear physical picture and definite interpretation. Herein, starting with a brief review of the development of the catalyst screening framework, we use a two-step kinetic model to refine and clarify the origin of the volcano curve with a full analytical analysis by integrating the surface kinet-ics and the results of first-principles calculations. It is mathematically demonstrated that the volca-no