Supramolecular Porphyrin Cages Assembled at Molecular-Materials Interfaces for Electrocatalytic CO Reduction.

ACS Cent Sci

Department of Chemistry, Department of Molecular and Cell Biology, and Howard Hughes Medical Institute, University of California, Berkeley, California 94720, United States.

Published: September 2017

AI Article Synopsis

  • The study highlights a method to convert carbon monoxide (CO) into valuable multi-carbon compounds, addressing energy and climate challenges.
  • Researchers developed a modular synthetic approach using supramolecular cages at molecular-materials interfaces for this electrochemical process.
  • The resulting heterobimetallic cavities achieved a high faradaic efficiency (FE = 83% with 57% to ethanol) and current density (1.34 mA/cm) at a specific potential, outperforming traditional copper surfaces in selectivity and activity.

Article Abstract

Conversion of carbon monoxide (CO), a major one-carbon product of carbon dioxide (CO) reduction, into value-added multicarbon species is a challenge to addressing global energy demands and climate change. Here we report a modular synthetic approach for aqueous electrochemical CO reduction to carbon-carbon coupled products via self-assembly of supramolecular cages at molecular-materials interfaces. Heterobimetallic cavities formed by face-to-face coordination of thiol-terminated metalloporphyrins to copper electrodes through varying organic struts convert CO to C2 products with high faradaic efficiency (FE = 83% total with 57% to ethanol) and current density (1.34 mA/cm) at a potential of -0.40 V vs RHE. The cage-functionalized electrodes offer an order of magnitude improvement in both selectivity and activity for electrocatalytic carbon fixation compared to parent copper surfaces or copper functionalized with porphyrins in an edge-on orientation.

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Source
http://www.ncbi.nlm.nih.gov/pmc/articles/PMC5620982PMC
http://dx.doi.org/10.1021/acscentsci.7b00316DOI Listing

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