Intermediate Binding Control Using Metal–Organic Frameworks Enhances Electrochemical CO2 Reduction
Type
ArticleAuthors
Nam, Dae-Hyun
Shekhah, Osama

Lee, Geonhui
Mallick, Arijit
Jiang, Hao

Li, Fengwang

Chen, Bin
Wicks, Joshua
Eddaoudi, Mohamed

Sargent, E.

KAUST Department
Advanced Membranes and Porous Materials Research CenterPhysical Science and Engineering (PSE) Division
Chemical Science Program
Date
2020-12-15Embargo End Date
2021-12-15Submitted Date
2020-10-11Permanent link to this record
http://hdl.handle.net/10754/666395
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Show full item recordAbstract
In the electrochemical CO2 reduction reaction (CO2RR), control over the binding of intermediates is key for tuning product selectivity and catalytic activity. Here we report the use of reticular chemistry to control the binding of CO2RR intermediates on metal catalysts encapsulated inside metal–organic frameworks (MOFs), thereby allowing us to improve CO2RR electrocatalysis. By varying systematically both the organic linker and the metal node in a face-centered cubic (fcu) MOF, we tune the adsorption of CO2, pore openness, and Lewis acidity of the MOFs. Using operando X-ray absorption spectroscopy (XAS) and in situ Raman spectroscopy, we reveal that the MOFs are stable under operating conditions and that this tuning plays the role of optimizing the *CO binding mode on the surface of Ag nanoparticles incorporated inside the MOFs with the increase of local CO2 concentration. As a result, we improve the CO selectivity from 74% for Ag/Zr-fcu-MOF-1,4-benzenedicarboxylic acid (BDC) to 94% for Ag/Zr-fcu-MOF-1,4-naphthalenedicarboxylic acid (NDC). The work offers a further avenue to utilize MOFs in the pursuit of materials design for CO2RR.Citation
Nam, D.-H., Shekhah, O., Lee, G., Mallick, A., Jiang, H., Li, F., … Sargent, E. H. (2020). Intermediate Binding Control Using Metal–Organic Frameworks Enhances Electrochemical CO2 Reduction. Journal of the American Chemical Society. doi:10.1021/jacs.0c10774Sponsors
This publication is based upon work supported by the King Abdullah University of Science and Technology (KAUST) Office of Sponsored Research (OSR) under Award No. OSR2018-CPF-3665-03. This research used synchrotron resources of the Advanced Photon Source (APS), an Office of Science User Facility operated for the US Department of Energy Office of Science by Argonne National Laboratory and was supported by the US Department of Energy under Contract No. DEAC02-06CH11357 and the Canadian Light Source and its funding partners. The authors thank Dr. T. P. Wu, Dr. Y. Z. Finfrock, Dr. G. Sterbinsky, and Dr. L. Ma for technical support at 9-BM beamline of APS. The authors acknowledge the use of facilities within CFI-funded Ontario Centre for the Characterization of Advanced Materials at the University of Toronto. This research was supported by the program of Carbon to X technology development for production of useful substances (2020M3H7A1098376), through the National Research Foundation of Korea (NRF), funded by the Korean government (Ministry of Science and ICT (MSIT)).Publisher
American Chemical Society (ACS)Additional Links
https://pubs.acs.org/doi/10.1021/jacs.0c10774ae974a485f413a2113503eed53cd6c53
10.1021/jacs.0c10774