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Heterogeneous molecular catalysts for electrocatalytic CO₂ reduction

Corbin, Nathan and Zeng, Joy and Williams, Kindle and Manthiram, Karthish (2019) Heterogeneous molecular catalysts for electrocatalytic CO₂ reduction. Nano Research, 12 (9). pp. 2093-2125. ISSN 1998-0124. doi:10.1007/s12274-019-2403-y. https://resolver.caltech.edu/CaltechAUTHORS:20220505-565274000

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Abstract

This review provides an overview of the literature regarding heterogeneous molecular catalysts for electrochemical CO₂ reduction (ECR). Fundamental aspects of the science, including aggregation, electrochemical rate laws, and electrode-catalyst electronic coupling, are discussed to provide a solid foundation on which to design experiments and interpret results. Mechanistic aspects of ECR are presented based on electrokinetic and spectroscopic measurements as well as density functional theory (DFT) calculations. Consensus is improving for electrokinetic measurements, but the redox state of the metal center under reaction conditions and DFT reaction pathways lack agreement in the literature. Concerning the tunable aspects of the molecular catalyst, the impacts of the metal center, ligand substituents, and electrode support on the activity and selectivity toward ECR are presented with an emphasis on those studies that controlled for aggregation and minimized mass-transport limitations. Extended three-dimensional (3D) structures such as polymers, metal-organic frameworks (MOFs), and covalent-organic frameworks (COFs) are discussed as highly tunable architectures that begin to mimic the catalytic pockets of enzyme active sites. To achieve the full potential of these catalysts, design principles must emerge based on a combination of deconvoluting measurements to extract intrinsic catalyst properties and more reliable theoretical calculations to predict reaction pathways.


Item Type:Article
Related URLs:
URLURL TypeDescription
https://doi.org/10.1007/s12274-019-2403-yDOIArticle
https://rdcu.be/cNra1PublisherFree ReadCube access
ORCID:
AuthorORCID
Corbin, Nathan0000-0001-6074-7948
Zeng, Joy0000-0002-3443-3504
Williams, Kindle0000-0001-9640-7849
Manthiram, Karthish0000-0001-9260-3391
Additional Information:© Tsinghua University Press and Springer-Verlag GmbH Germany, part of Springer Nature 2019. Received: 18 February 2019 / Revised: 29 March 2019 / Accepted: 3 April 2019. We gratefully acknowledge financial support from Cenovus Energy. N. C. was supported by a NSF Graduate Research Fellowship.
Funders:
Funding AgencyGrant Number
Cenovus EnergyUNSPECIFIED
NSF Graduate Research FellowshipUNSPECIFIED
Subject Keywords:CO₂ reduction, electrocatalysis, porphyrins, phthalocyanines, molecular complexes, heterogeneous catalysis
Issue or Number:9
DOI:10.1007/s12274-019-2403-y
Record Number:CaltechAUTHORS:20220505-565274000
Persistent URL:https://resolver.caltech.edu/CaltechAUTHORS:20220505-565274000
Official Citation:Corbin, N., Zeng, J., Williams, K. et al. Heterogeneous molecular catalysts for electrocatalytic CO2 reduction. Nano Res. 12, 2093–2125 (2019). https://doi.org/10.1007/s12274-019-2403-y
Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:114618
Collection:CaltechAUTHORS
Deposited By: George Porter
Deposited On:12 May 2022 20:21
Last Modified:12 May 2022 20:21

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