Citation: WANG Dan, DING Xunlei, LIAO Henglu, DAI Jiayu. Methane Activation on (Au/Ag)₁-Doped Vanadium Oxide Clusters[J]. Acta Physico-Chimica Sinica, ;2019, 35(9): 1005-1013. doi: 10.3866/PKU.WHXB201809006 shu

Methane Activation on (Au/Ag)₁-Doped Vanadium Oxide Clusters

WANG Dan ¹ ,
DING Xunlei ^2,, ,
LIAO Henglu ² ,
DAI Jiayu ^1,,

1.
Department of Physics, College of Arts and Sciences, National University of Defense Technology, Changsha 410073, P. R. China
2.
School of Mathematics and Physics, North China Electric Power University, Beijing 102206, P. R. China

Corresponding author: DING Xunlei, dingxl@ncepu.edu.cn DAI Jiayu, jydai@nudt.edu.cn
Received Date: 4 September 2018
Revised Date: 15 October 2018
Accepted Date: 15 October 2018
Available Online: 18 September 2018
Fund Project: the Science and Technology Project of Hunan Province, China 2017RS3038The project was supported by the National Natural Science Foundation of China (91545122, 11774429), the Science and Technology Project of Hunan Province, China (2017RS3038) and the Fundamental Research Funds for the Central Universities, China (JB2015RCY03)The project was supported by the National Natural Science Foundation of China 91545122The project was supported by the National Natural Science Foundation of China 11774429the Fundamental Research Funds for the Central Universities, China JB2015RCY03

The activation of methane (CH₄) is a key step in its conversion to more valuable products. The activation mechanisms of CH₄ on catalyst surfaces have been widely studied using gas-phase cluster models, which can be operated on systems with a precise number of atoms and determined structures. Herein, we have used MV₃O_y^q (M = Au/Ag, y = 6–8, q = 0 or ±1) clusters, in which a single Au or Ag atom was supported on vanadium oxide clusters, as simple models to mimic the properties of newly developed single-atom catalysts. The adsorption and activation of CH₄ on these MV₃O_y^q clusters were systematically studied via density functional theory calculations at the B3LYP/Def2-TZVP level, which provided insights into the geometric structures, adsorption energies, and charge distributions of the adsorption systems. Five Au-containing clusters, AuV₃O₆, AuV₃O₇, AuV₃O₈, AuV₃O₆⁺, and AuV₃O₇⁺, were able to activate CH₄, while other clusters, including all Ag-containing clusters, were inert. In the active clusters, all Au atoms were adsorbed on the O-atom sites of the supporting V₃O_y^q cluster and served as the active sites for CH₄ activation. The activation of CH₄ was characterized by the lengthened C―H bond (approximately 115 pm), short distances between CH₄ and Au (approximately 184 pm), relatively high adsorption energies of CH₄ (~0.590–1.145 eV), and significant electron transfer from CH₄ to the clusters (above 0.08e). In particular, AuV₃O₈, which is a neutral cluster with a close-shell electronic state, can activate CH₄ with a C―H bond length of 115 pm, Au―H bond length of 183 pm, the adsorption energy of CH₄ of 0.853 eV, and the charge on CH₄ of +0.088e. The charge state of the cluster has a significant effect on the activation ability: cationic clusters are the most active, followed by neutral clusters, while anionic clusters have the lowest activities toward CH₄. Consistently, the local charge on the M atom has a positive correction with the activation ability of MV₃O_y^q clusters with a certain M. However, as compared to Au-containing clusters, Ag-containing clusters have lower activities despite the higher local charges on Ag in each MV₃O_y^q cluster. The results indicate that the inclusion of D3 dispersion correction has a small effect on structures and energies. This study may serve as a foundation for further research on the activation of CH₄ on single-atom catalysts and provides useful information on rational designing of single-atom catalysts for CH₄ conversion at low temperatures.
- Methane activation,
- Metal oxide clusters,
- Noble metal,
- Single-atom catalysis,
- Density functional theory
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Methane Activation on (Au/Ag)₁-Doped Vanadium Oxide Clusters