Citation: YIN Yueqi, JIANG Mengxu, LIU Chunguang. DFT Study of POM-Supported Single Atom Catalyst (M₁/POM, M = Ni, Pd, Pt, Cu, Ag, Au, POM = [PW₁₂O₄₀]^3-) for Activation of Nitrogen Molecules[J]. Acta Physico-Chimica Sinica, ;2018, 34(3): 270-277. doi: 10.3866/PKU.WHXB201707071 shu

DFT Study of POM-Supported Single Atom Catalyst (M₁/POM, M = Ni, Pd, Pt, Cu, Ag, Au, POM = [PW₁₂O₄₀]^3-) for Activation of Nitrogen Molecules

Institute of Functional Material Chemistry, College of Chemical Engineering, Northeast Electric Power University, Jilin 132012, Jilin Province, P. R. China

Corresponding author: LIU Chunguang, liucg407@163.com
Received Date: 22 May 2017
Revised Date: 30 June 2017
Accepted Date: 30 June 2017
Available Online: 7 March 2017
Fund Project: The project was supported by the Natural Science Foundation of China (21373043)the Natural Science Foundation of China 21373043

Molecular geometries, electronic structure, and infrared spectroscopy of a series of polyoxometalate (POM)-supported single atom catalyst (SACs) (M₁/POM (M = Ni, Pd, Pt, Cu, Ag, Au, POM = [PW₁₂O₄₀]^3-) have been studied based on density factional theory (DFT) combined with natural bond orbital (NBO) analysis method. The results show that Pt₁/POM has a higher reactivity for activation of N₂ relevant to the others. The interaction between the isolated Pt atom and N₂ arises from an orbital mixture, which is formed by the d_xz and d_yz orbital of Pt atom and the π* anti-bond orbit of N₂ molecule. The electron transfer from Pt atom to the nitrogen molecule leads to a weakened N≡N bond. The N≡N bond distance increases when compared with the free N₂ molecule. All results indicate an effective activation of the nitrogen molecules. For DFT-derived IR spectra, the four characteristic peaks of Keggin-type POM split into five because of introduction of the isolated metal atom.
- Single atom catalyst,
- Artificial nitrogen fixation,
- Density functional theory,
- Electronic structure,
- Infrared spectroscopy
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通讯作者: 陈斌, bchen63@163.com

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沈阳化工大学材料科学与工程学院沈阳 110142

DFT Study of POM-Supported Single Atom Catalyst (M1/POM, M = Ni, Pd, Pt, Cu, Ag, Au, POM = [PW12O40]3-) for Activation of Nitrogen Molecules

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通讯作者: 陈斌, bchen63@163.com

DFT Study of POM-Supported Single Atom Catalyst (M₁/POM, M = Ni, Pd, Pt, Cu, Ag, Au, POM = [PW₁₂O₄₀]^3-) for Activation of Nitrogen Molecules