title: Probing the effect of the Pt-Ni-Pt(111) bimetallic surface electronic structures on the ammonia decomposition reaction.
abstract: We report a detailed investigation of elementary catalytic decomposition of ammonia on the Pt-Ni-Pt(111) bimetallic surface using in situ near ambient pressure X-ray photoelectron spectroscopy. Under the near ambient pressure (0.6 mbar) reaction conditions, a different dehydrogenation pathway with a reduced activation energy barrier for recombinative nitrogen desorption on the Pt-Ni-Pt(111) bimetallic surface is observed. The unique surface catalytic activity is correlated with the downward shift of the Pt 5d band states induced by the Ni subsurface atoms via charge redistribution of the topmost Pt layer. Our results provide a practical understanding of the unique chemistry of bimetallic catalysts for facile ammonia decomposition under realistic reaction conditions.
authors.affiliation: Department of Chemistry, National University of Singapore, 3 Science Drive 3, 117543, Singapore, Singapore. jzhong@bnl.gov phycw@nus.edu.sg and Department of Physics, National University of Singapore, 2 Science Drive 3, 117542, Singapore, Singapore and Singapore-Peking University Research Centre (SPURc), 1 CREATE Way, #15-01, CREATE Tower, 138602, Singapore, Singapore.
authors.forename: Jian-Qiang
authors.initials: JQ
authors.lastname: Zhong
authors.affiliation: Department of Chemistry, National University of Singapore, 3 Science Drive 3, 117543, Singapore, Singapore. jzhong@bnl.gov phycw@nus.edu.sg and Singapore-Peking University Research Centre (SPURc), 1 CREATE Way, #15-01, CREATE Tower, 138602, Singapore, Singapore.
authors.forename: Xiong
authors.initials: X
authors.lastname: Zhou
authors.affiliation: Department of Physics, National University of Singapore, 2 Science Drive 3, 117542, Singapore, Singapore and Singapore-Peking University Research Centre (SPURc), 1 CREATE Way, #15-01, CREATE Tower, 138602, Singapore, Singapore.
authors.forename: Kaidi
authors.initials: K
authors.lastname: Yuan
authors.affiliation: Department of Chemistry and Physics, La Trobe Institute for Molecular Science, La Trobe University, Melbourne, Victoria 3086, Australia.
authors.forename: Christopher A
authors.initials: CA
authors.lastname: Wright
authors.affiliation: Department of Chemistry and Physics, La Trobe Institute for Molecular Science, La Trobe University, Melbourne, Victoria 3086, Australia and Australian Synchrotron, 800 Blackburn Road, Clayton, Victoria 3168, Australia.
authors.forename: Anton
authors.initials: A
authors.lastname: Tadich
authors.affiliation: Department of Chemistry and Physics, La Trobe Institute for Molecular Science, La Trobe University, Melbourne, Victoria 3086, Australia.
authors.forename: Dongchen
authors.initials: D
authors.lastname: Qi
authors.affiliation: Chinese Education Ministry Key Laboratory of Resource Chemistry, Shanghai Normal University, Shanghai, 200234, China.
authors.forename: He Xing
authors.initials: HX
authors.lastname: Li
authors.affiliation: Singapore-Peking University Research Centre (SPURc), 1 CREATE Way, #15-01, CREATE Tower, 138602, Singapore, Singapore and College of Chemistry and Molecular Engineering, Peking University, Beijing, 100871, China.
authors.forename: Kai
authors.initials: K
authors.lastname: Wu
authors.affiliation: Department of Chemistry, National University of Singapore, 3 Science Drive 3, 117543, Singapore, Singapore. jzhong@bnl.gov phycw@nus.edu.sg and Singapore-Peking University Research Centre (SPURc), 1 CREATE Way, #15-01, CREATE Tower, 138602, Singapore, Singapore and National University of Singapore (Suzhou) Research Institute, 377 Lin Quan Street, Suzhou Industrial Park, Jiangsu, 215123, China.
authors.forename: Guo Qin
authors.initials: GQ
authors.lastname: Xu
authors.affiliation: Department of Chemistry, National University of Singapore, 3 Science Drive 3, 117543, Singapore, Singapore. jzhong@bnl.gov phycw@nus.edu.sg and Department of Physics, National University of Singapore, 2 Science Drive 3, 117542, Singapore, Singapore and Singapore-Peking University Research Centre (SPURc), 1 CREATE Way, #15-01, CREATE Tower, 138602, Singapore, Singapore and National University of Singapore (Suzhou) Research Institute, 377 Lin Quan Street, Suzhou Industrial Park, Jiangsu, 215123, China.
authors.forename: Wei
authors.initials: W
authors.lastname: Chen