4.6 Review

Support-based modulation strategies in single-atom catalysts for electrochemical CO2 reduction: graphene and conjugated macrocyclic complexes

Journal

JOURNAL OF MATERIALS CHEMISTRY A
Volume 10, Issue 11, Pages 5699-5716

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/d1ta09069k

Keywords

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Funding

  1. National Natural Science Foundation of China [22033002, 21525311, 21973011, 22173018]

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This review provides an overview of recent progress in single-atom catalysts (SACs) for the electrochemical CO2 reduction reaction (CO2RR), focusing on the influence of catalyst supports such as graphene and conjugated macrocycle, as well as factors like heteroatom doping and bimetals on the activity and selectivity of the catalysts. Insights on the intrinsic connection between electronic structures and catalytic properties are summarized, along with discussions on the stability and dynamic structural changes of SACs under operating conditions. Challenges and perspectives for future development of efficient SACs based on graphene and conjugated macrocycle supports are also addressed.
The electrochemical CO2 reduction reaction (CO2RR) is a promising method to decrease the CO2 concentration in the atmosphere and produce high value-added chemicals simultaneously. Catalysts play a central role in the CO2RR system, and can determine the conversion efficiency and product species. Single-atom catalysts (SACs), a new class of catalysts, have been extensively employed in the CO2RR due to their high activities, selectivity and maximum atom utilization efficiency. In this review, an overview of the recent progress of SACs for the CO2RR is provided with respect to two types of catalyst supports including graphene (Gr)-based nanomaterials and conjugated macrocycle (CM)-based complexes. Specifically, we focus on significant influencing factors on the activity and selectivity of the modeled catalysts, such as heteroatom doping, ligand effects and bimetals. Insights on the intrinsic connection between electronic structures and catalytic properties are summarized. Moreover, the stability and the dynamic structural change of SACs under operating conditions are also discussed. Finally, some challenges and perspectives are raised for the future development of efficient SACs based on Gr and CM supports.

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