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Molecular enhancement of heterogeneous CO₂ reduction

Nam, Dae-Hyun and De Luna, Phil and Rosas-Hernández, Alonso and Thevenon, Arnaud and Li, Fengwang and Agapie, Theodor and Peters, Jonas C. and Shekhah, Osama and Eddaoudi, Mohamed and Sargent, Edward H. (2020) Molecular enhancement of heterogeneous CO₂ reduction. Nature Materials, 19 (3). pp. 266-276. ISSN 1476-1122. https://resolver.caltech.edu/CaltechAUTHORS:20200302-110558568

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Abstract

The electrocatalytic carbon dioxide reduction reaction (CO₂RR) addresses the need for storage of renewable energy in valuable carbon-based fuels and feedstocks, yet challenges remain in the improvement of electrosynthesis pathways for highly selective hydrocarbon production. To improve catalysis further, it is of increasing interest to lever synergies between heterogeneous and homogeneous approaches. Organic molecules or metal complexes adjacent to heterogeneous active sites provide additional binding interactions that may tune the stability of intermediates, improving catalytic performance by increasing Faradaic efficiency (product selectivity), as well as decreasing overpotential. We offer a forward-looking perspective on molecularly enhanced heterogeneous catalysis for CO₂RR. We discuss four categories of molecularly enhanced strategies: molecular-additive-modified heterogeneous catalysts, immobilized organometallic complex catalysts, reticular catalysts and metal-free polymer catalysts. We introduce present-day challenges in molecular strategies and describe a vision for CO2RR electrocatalysis towards multi-carbon products. These strategies provide potential avenues to address the challenges of catalyst activity, selectivity and stability in the further development of CO₂RR.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1038/s41563-020-0610-2DOIArticle
https://rdcu.be/b2pu7PublisherFree ReadCube access
ORCID:
AuthorORCID
Nam, Dae-Hyun0000-0002-0871-1355
De Luna, Phil0000-0002-7729-8816
Rosas-Hernández, Alonso0000-0002-0812-5591
Thevenon, Arnaud0000-0002-5543-6595
Li, Fengwang0000-0003-1531-2966
Agapie, Theodor0000-0002-9692-7614
Peters, Jonas C.0000-0002-6610-4414
Shekhah, Osama0000-0003-1861-9226
Eddaoudi, Mohamed0000-0003-1916-9837
Sargent, Edward H.0000-0003-0396-6495
Additional Information:© 2020 Springer Nature Limited. Received 16 January 2019; Accepted 08 January 2020; Published 25 February 2020. This work was in part supported financially by the Natural Sciences and Engineering Research Council of Canada, the Ontario Research Fund: Research Excellence Program (ORF-RE-RE08-034), the Natural Resources Canada Clean Growth Program (CGP-17-0455) and CIFAR Bio-Inspired Solar Energy Program (FL-000719). This work was also supported by the Joint Center for Artificial Photosynthesis, a DOE Energy InnovationHub, supported through the Office of Science of the US Department of Energy under award no. DESC0004993, and was also based on work supported by the King Abdullah University of Science and Technology (KAUST) Office of Sponsored Research (OSR) under award no. OSR-2018-CPF-3665-03 and OSR-2019-CCF-1972.04. P.D.L. acknowledges the Natural Sciences and Engineering Research Council of Canada for support in the form of a Canada Graduate Scholarship and A.T. acknowledges the European Union’s Horizon 2020 research and innovation programme under the Marie Skłodowska-Curie Action H2020-MSCA-IF-2017 (793471). These authors contributed equally: Dae-Hyun Nam, Phil De Luna. The authors declare no competing interests.
Group:JCAP
Funders:
Funding AgencyGrant Number
Natural Sciences and Engineering Research Council of Canada (NSERC)UNSPECIFIED
Ontario Research FundORF-RE-RE08-034
Natural Resources CanadaCGP-17-0455
Canadian Institute for Advanced Research (CIFAR)FL-000719
Joint Center for Artificial Photosynthesis (JCAP)UNSPECIFIED
Department of Energy (DOE)DESC0004993
King Abdullah University of Science and Technology (KAUST)OSR-2018-CPF-3665-03
King Abdullah University of Science and Technology (KAUST)OSR-2019-CCF-1972.04
European Research Council (ERC)793471
Subject Keywords:Engineering; Materials science
Issue or Number:3
Record Number:CaltechAUTHORS:20200302-110558568
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20200302-110558568
Official Citation:Nam, D., De Luna, P., Rosas-Hernández, A. et al. Molecular enhancement of heterogeneous CO2 reduction. Nat. Mater. 19, 266–276 (2020). https://doi.org/10.1038/s41563-020-0610-2
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:101650
Collection:CaltechAUTHORS
Deposited By: Tony Diaz
Deposited On:02 Mar 2020 19:23
Last Modified:02 Mar 2020 19:23

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