Molecular enhancement of heterogeneous CO2 reduction

Dae-Hyun Nam, Phil De Luna, Alonso Rosas-Hernández, Arnaud Thevenon, Fengwang Li, Theodor Agapie, Jonas C. Peters, Osama Shekhah, Mohamed Eddaoudi, E. Sargent

Research output: Contribution to journalArticlepeer-review

105 Scopus citations

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.
Original languageEnglish (US)
Pages (from-to)266-276
Number of pages11
JournalNature Materials
Volume19
Issue number3
DOIs
StatePublished - Feb 25 2020

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