Probing the effect of the Pt-Ni-Pt(111) bimetallic surface electronic structures on the ammonia decomposition reaction

Jian-Qiang Zhong; Xiong Zhou; Kaidi Yuan; Christopher A Wright; Anton Tadich; Dongchen Qi; He Xing Li; Kai Wu; Guo Qin Xu; Wei Chen

doi:10.1039/c6nr08311k

Probing the effect of the Pt-Ni-Pt(111) bimetallic surface electronic structures on the ammonia decomposition reaction

Nanoscale. 2017 Jan 5;9(2):666-672. doi: 10.1039/c6nr08311k.

Authors

Jian-Qiang Zhong¹, Xiong Zhou², Kaidi Yuan³, Christopher A Wright⁴, Anton Tadich⁵, Dongchen Qi⁴, He Xing Li⁶, Kai Wu⁷, Guo Qin Xu⁸, Wei Chen⁹

Affiliations

¹ Department of Chemistry, National University of Singapore, 3 Science Drive 3, 117543, Singapore, Singapore. [email protected] [email protected] 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.
² Department of Chemistry, National University of Singapore, 3 Science Drive 3, 117543, Singapore, Singapore. [email protected] [email protected] and Singapore-Peking University Research Centre (SPURc), 1 CREATE Way, #15-01, CREATE Tower, 138602, Singapore, Singapore.
³ 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.
⁴ Department of Chemistry and Physics, La Trobe Institute for Molecular Science, La Trobe University, Melbourne, Victoria 3086, Australia.
⁵ 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.
⁶ Chinese Education Ministry Key Laboratory of Resource Chemistry, Shanghai Normal University, Shanghai, 200234, China.
⁷ 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.
⁸ Department of Chemistry, National University of Singapore, 3 Science Drive 3, 117543, Singapore, Singapore. [email protected] [email protected] 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.
⁹ Department of Chemistry, National University of Singapore, 3 Science Drive 3, 117543, Singapore, Singapore. [email protected] [email protected] 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.

PMID: 27942692
DOI: 10.1039/c6nr08311k

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.