Chinese Journal of Catalysis ›› 2016, Vol. 37 ›› Issue (10): 1738-1746.DOI: 10.1016/S1872-2067(16)62467-1

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Oxidation of formic acid on stepped Au(997) surface

Zong-Fang Wu, Zhi-Quan Jiang, Yue-Kang Jin, Feng Xiong, Guang-Hui Sun, Wei-Xin Huang   

  1. Hefei National Laboratory for Physical Sciences at the Microscale, CAS Key Laboratory of Materials for Energy Conversion, Department of Chemical Physics, University of Science and Technology of China, Hefei 230026, Anhui, China
  • Received:2016-04-11 Revised:2016-05-16 Online:2016-10-21 Published:2016-10-22
  • Contact: Wei-Xin Huang
  • Supported by:

    This work was supported by the National Basic Research Program of China (973 Program, 2013CB933104), the National Natural Science Foun-dation of China (21525313, 20973161, 21373192), the Fundamental Research Funds for the Central Universities (WK2060030017), and Collaborative Innovation Center of Suzhou Nano Science and Technology.

Abstract:

The adsorption and reaction of formic acid (HCOOH) on clean and atomic oxygen-covered Au(997) surfaces were studied by temperature-programmed desorption/reaction spectroscopy (TPRS) and X-ray photoelectron spectroscopy (XPS). At 105 K, HCOOH molecularly adsorbs on clean Au(997) and interacts more strongly with low-coordinated Au atoms at (111) step sites than with those at (111) terrace sites. On an atomic oxygen-covered Au(997) surface, HCOOH reacts with oxygen atoms to form HCOO and OH at 105 K. Upon subsequent heating, surface reactions occur among adsorbed HCOO, OH, and atomic oxygen and produce CO2, H2O, and HCOOH between 250 and 400 K. The Au(111) steps bind surface adsorbates more strongly than the Au(111) terraces and exhibit larger barriers for HCOO(a) oxidation reactions. The surface reactions also depend on the relative coverages of co-existing surface species. Our results elucidate the elementary surface reactions between formic acid and oxygen adatoms on Au surfaces and highlight the effects of the coordination number of the Au atoms on the Au catalysis.

Key words: Gold catalysis, Surface chemistry, Model catalyst, Geometric structure, Coordination number