Study on catalytic properties of metal-supported ZIF-8 with computational chemistry

被引：0

作者：

Bo, Xiaofan ^{[1
]}

Wu, Pingyi ^{[2
]}

Liu, Dahuan ^{[1
]}

Yang, Qingyuan ^{[1
]}

Ma, Qintian ^{[1
]}

Lan, Ling ^{[2
]}

Wang, Shaohua ^{[3
]}

Zhang, Yi ^{[3
]}

Zhong, Chongli ^{[1
]}

机构：

[1] State Key Laboratory of Organic-Inorganic Composites, Beijing University of Chemical Technology

[2] Petrochemical Research Institute, PetroChina

[3] China Kunlun Contracting Engineering Corporation Liaoning Company, Liaoyang 111003, Liaoning

来源：

Huagong Xuebao/CIESC Journal | 2014年 / 65卷 / 05期

关键词：

Catalysis; Density functional theory; Metal particles; Metal-organic frameworks; Model; Nanoscale; Stability;

D O I：

10.3969/j.issn.0438-1157.2014.05.013

中图分类号：

学科分类号：

摘要：

Metal-organic frameworks (MOFs) are a new family of nanoporous functional materials that have shown potential applications in catalysis, due to their unique structural features. In this work, a combination of molecular simulation and density functional theory (DFT) calculation were employed to investigate the catalytic properties of metal-supported ZIF-8 with different metals (Pd, Ag, Pt and Au). First, the radial distribution function between these metal particles and the different atoms in ZIF-8 was analyzed from Monte Carlo (MC) and molecular dynamics (MD) simulations in order to determine the possible locations of the metal particles. Then, DFT calculations were performed at the generalized gradient corrected approximation (GGA) level with PW91 functional and the double numerical plus polarization (DNP) basis set. The binding energy was calculated to evaluate the relative stability of the metal particles (Pd, Ag, Pt and Au) in each site of the framework. The results showed that there were three types of interaction modes between the metals and the framework: carbon-metal-carbon (C-M-C), metal-carbon (M-C) and metal-bond (M-bond) modes, where the first type was the most stable one. For the same interaction type, the order of the stability of ZIF-8 with different metals was: Pd ≤ Ag ≤ Pt ≤ Au. At the same time, the catalytic activity of the metal-supported materials was also investigated using CO as probe molecule. The analysis of the Mulliken population and the electrostatic potential distributions of metals indicated that metal particles were the Lewis acid sites which were related to their capabilities of accepting an electron. The order of their catalytic activities was: Pd ≤ Pt ≤ Ag ≤ Au. The results obtained in this work may provide useful information for the catalytic application of MOFs loaded with metals. © All Rights Reserved.

引用

页码：1644 / 1651

页数：7

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