Keggin型多酸负载的单原子催化剂(M1/POM, M = Ni, Pd, Pt, Cu, Ag, Au, POM = [PW12O40]3-)活化氮气分子的密度泛函理论计算研究

doi:10.3866/PKU.WHXB201707071

Abstract

Abstract:

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.

Key words: Single atom catalyst, Artificial nitrogen fixation, Density functional theory, Electronic structure, Infrared spectroscopy

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Yueqi YIN,Mengxu JIANG,Chunguang LIU. 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 Phys. -Chim. Sin. 2018, 34(3), 270-277. doi: 10.3866/PKU.WHXB201707071

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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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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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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