何成西安交通大学教师主页管理系统 Enhanced catalytic CO oxidation by Cu 13-m Ni m (m=0, 1, 13) clusters at ambient temperatures with more active sites and distinct mechanistic pathways 中文主页

Enhanced catalytic CO oxidation by Cu 13-m Ni m (m=0, 1, 13) clusters at ambient temperatures with more active sites and distinct mechanistic pathways

论文名称：: Enhanced catalytic CO oxidation by Cu 13-m Ni m (m=0, 1, 13) clusters at ambient temperatures with more active sites and distinct mechanistic pathways

摘要：: Nowadays, developing highly efficient, stable and low cost catalysts is generally considered to be the key to solve the drastically increasing of carbon monoxide (CO) emission. In this paper, Cu 13-m Ni m (m= 0, 1, 13) bimetallic clusters have been proposed as new cluster catalysts, and their electronic, chemical properties and CO catalytic oxidation reaction are systematically calculated by DFT theoretical simulation. When an O 2 molecule is adsorbed on the active-site of Cu 13-m Ni m cluster, O 2 molecule decomposing reaction occurs firstly, rather than coad-sorption of O 2 and CO molecule, which is modified the traditional Langmuir - Hinshelwood (LH) mechanism. By analyzing the reaction energy barrier of each step on Cu 13-m Ni m clusters, the rate - determining step is de
termined as the oxidation reaction between aissociated oxygen atom and carbon monoxide, which is hindered
by a significant activation barrier. In addition, icrokinetics simulations predict that Cu 12 Ni cluster is extremely efficient in catalyzing CO oxidation. Our findings present a rational way for designing heterogeneous catalysts with abundant reactive sites.