title: Patched bimetallic surfaces are active catalysts for ammonia decomposition.
abstract: Ammonia decomposition is often used as an archetypical reaction for predicting new catalytic materials and understanding the very reason of why some reactions are sensitive on material's structure. Core-shell or surface-segregated bimetallic nanoparticles expose outstanding activity for many heterogeneously catalysed reactions but the reasons remain elusive owing to the difficulties in experimentally characterizing active sites. Here by performing multiscale simulations in ammonia decomposition on various nickel loadings on platinum (111), we show that the very high activity of core-shell structures requires patches of the guest metal to create and sustain dual active sites: nickel terraces catalyse N-H bond breaking and nickel edge sites drive atomic nitrogen association. The structure sensitivity on these active catalysts depends profoundly on reaction conditions due to kinetically competing relevant elementary reaction steps. We expose a remarkable difference in active sites between transient and steady-state studies and provide insights into optimal material design.
authors.affiliation: Department of Chemical and Biomolecular Engineering, Catalysis Center for Energy Innovation, University of Delaware, Newark, Delaware 19716, USA.|School of Physics, Beijing Institute of Technology, Beijing 100081, China.|Institute of Physics, Chinese Academy of Sciences, Beijing 100190, China.
authors.forename: Wei
authors.initials: W
authors.lastname: Guo
authors.affiliation: Department of Chemical and Biomolecular Engineering, Catalysis Center for Energy Innovation, University of Delaware, Newark, Delaware 19716, USA.
authors.forename: Dionisios G
authors.initials: DG
authors.lastname: Vlachos