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Citation: DUAN Yuan, CHEN Mingshu, WAN Huilin. Adsorption and Activation of O2 and CO on the Ni(111) Surface[J]. Acta Physico-Chimica Sinica, ;2018, 34(12): 1358-1365. doi: 10.3866/PKU.WHXB201803071 shu

Adsorption and Activation of O2 and CO on the Ni(111) Surface

  • State Key Laboratory of Physical Chemistry of Solid Surfaces, National Engineering Laboratory for Green Chemical Productions of Alcohols-Ethers-Esters, College of Chemistry and Chemical Engineering, Xiamen University, Xiamen 361005, Fujian Province, P. R. China

  • Corresponding author: CHEN Mingshu, chenms@xmu.edu.cn
  • Received Date: 4 February 2018
    Revised Date: 1 March 2018
    Accepted Date: 2 March 2018
    Available Online: 7 December 2018

    Fund Project: the National Natural Science Foundation of China 21073149The project was supported by the National Natural Science Foundation of China (21073149, 21573180, 91545204)the National Natural Science Foundation of China 91545204the National Natural Science Foundation of China 21573180

  • Ni-based catalysts have been widely used in many important industrial heterogeneous processes such as hydrogenation and steam reforming owing to their sufficiently high activity yet significantly lower cost than that of alternative precious-metal-based catalysts. However, nickel catalysts are susceptible to deactivation. Understanding the adsorption and activation behavior of small molecules on the model catalyst surface is important to optimize the catalytic performance. Although many studies have been carried out in recent years, the initial oxidation process of nickel surface is still not fully understood, and the influence of the adsorption sequence of CO and O2 and their co-adsorption is controversial. In this study, the surface oxygen species on Ni(111) and the co-adsorption of CO and O2 were explored using high-resolution electron energy loss spectroscopy (HREELS), Auger electron spectroscopy (AES), and low energy electron diffraction (LEED). HREELS can provide useful information about the surface structure, surface-adsorbed species, adsorption sites, and interactions between surface oxygen species and CO on the surface. The results showed that there were two kinds of oxygen species after the oxidation of Ni(111), and the energy loss peaks at 54–58 meV were ascribed to surface chemisorbed oxygen species, and the peak at 69 meV to surface nickel oxide. The chemisorbed oxygen at low coverage displayed a LEED pattern of (2×2), revealing the formation of an ordered surface structure. As the amount of oxygen increased, the energy loss peak at 54 meV shifted to 58 meV. At an O2 partial pressure of 1×10-8 Torr (1 Torr = 133.32 Pa), the AES ratio of O/Ni remained almost unchanged after dosing 48 L, which indicated that the surface nickel oxide was relatively stable. The surface chemisorbed oxygen species was less stable, which could change to surface nickel oxide after annealing in vacuum. CO adsorbed on Ni(111) at room temperature with tri-hollow and a-top sites. Upon annealing in vacuum, a-top CO weakened first and then disappeared completely at 520 K, whereas tri-hollow CO was much more stable. The pre-adsorption of CO could suppress O2 adsorption and oxidation of the Ni(111) surface. The presence of oxygen could then gradually remove and replace CO with O2. The surface oxygen species preferred the tri-hollow sites, resulting in more a-top adsorbed CO during the co-adsorption of CO and oxygen. The surface chemisorbed oxygen species were more active and could react with CO at room temperature; however, the surface nickel oxide was less active, and could only be reduced at a higher temperature and higher partial pressure of CO.
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