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†

Jian-Qiang Zhong,‡*^abc Xiong Zhou,^ac Kaidi Yuan,^bc Christopher A. Wright,^d Anton Tadich,^de Dongchen Qi,^d He Xing Li,^f Kai Wu,^cg Guo Qin Xu^ach and Wei Chen*^abch

Author affiliations

* Corresponding authors

^a Department of Chemistry, National University of Singapore, 3 Science Drive 3, Singapore, Singapore
E-mail: jzhong@bnl.gov, phycw@nus.edu.sg

^b Department of Physics, National University of Singapore, 2 Science Drive 3, Singapore, Singapore

^c Singapore-Peking University Research Centre (SPURc), 1 CREATE Way, #15-01, CREATE Tower, Singapore, Singapore

^d Department of Chemistry and Physics, La Trobe Institute for Molecular Science, La Trobe University, Melbourne, Victoria, Australia

^e Australian Synchrotron, 800 Blackburn Road, Clayton, Victoria, Australia

^f Chinese Education Ministry Key Laboratory of Resource Chemistry, Shanghai Normal University, Shanghai, China

^g College of Chemistry and Molecular Engineering, Peking University, Beijing, China

^h National University of Singapore (Suzhou) Research Institute, 377 Lin Quan Street, Suzhou Industrial Park, Jiangsu, China

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.

Nanoscale

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

Abstract

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

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