Catalyzed activation of CO2 by a Lewis-base site in W–Cu–BTC hybrid metal organic frameworks
- ️Liang Chen
* Corresponding authors
a
Ningbo Institute of Materials Technology and Engineering, Chinese Academy of Sciences, Ningbo, Zhejiang 315201, P. R. China
E-mail:
chenliang@nimte.ac.cn
b Department of Materials Science and Engineering, University of Michigan, Ann Arbor, Michigan 48109, USA
Abstract
A metal–organic framework (MOF)-based catalyst W–Cu–BTC is designed by hybridizing highly active W ions into Cu3(BTC)2(H2O)3 (also known as Cu–BTC or HKUST-1, BTC = 1,3,5-tricarboxylate benzene) frameworks based on density functional (DFT) calculations. We show that the hybrid W–Cu node plays a pivotal role in activating CO2 according to frontier molecular orbital theory. In contrast to the Lewis-acid nature of open metal sites in most MOFs, the exposed W ion in W–Cu–BTC is identified as a Lewis-base site, evidenced by the substantial electron donation from W ion to CO2. Kinetically, the linear CO2 molecule can be readily bent by forming a CO2–W complex after overcoming a negligible activation barrier of 0.09 eV. In addition, we present calculated infrared spectra (IR) and X-Ray spectra (XPS) for reference in future experimental studies.
Supplementary files
Article information
- https://doi.org/10.1039/C2SC20521A
- Edge Article
- 25 Apr 2012
- 26 Jun 2012
- 27 Jun 2012
DOI
Article type
Submitted
Accepted
First published
Chem. Sci., 2012,3, 2708-2715
Permissions
Catalyzed activation of CO2 by a Lewis-base site in W–Cu–BTC hybrid metal organic frameworks
Q. Zhang, L. Cao, B. Li and L. Chen, Chem. Sci., 2012, 3, 2708 DOI: 10.1039/C2SC20521A
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