物理化学学报2018，Vol.34Issue(3)：270-277,8.DOI:10.3866/PKU.WHXB201707071
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
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
摘要
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 dxz and dyz 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.关键词
单原子催化剂/人工固氮/密度泛函理论/电子结构/红外光谱Key words
Single atom catalyst/Artificial nitrogen fixation/Density functional theory/Electronic structure/Infrared spectroscopy分类
化学化工引用本文复制引用
尹玥琪,蒋梦绪,刘春光..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[J].物理化学学报,2018,34(3):270-277,8.基金项目
The project was supported by the Natural Science Foundation of China (21373043).国家自然科学基金(21373043)资助项目 （21373043）
