Pendant Hydrogen-Bond Donors in Cobalt Catalysts Independently Enhance CO2 Reduction

Chapovetsky, Alon; Welborn, Matthew; Luna, John M.; Haiges, Ralf; Miller, Thomas F.; Marinescu, Smaranda C.

doi:10.1021/acscentsci.7b00607

Title: Pendant Hydrogen-Bond Donors in Cobalt Catalysts Independently Enhance CO₂ Reduction

Journal Article · 23 February 2018 · ACS Central Science

DOI: https://doi.org/10.1021/acscentsci.7b00607 · OSTI ID:1498679

Chapovetsky, Alon ^[1]; Welborn, Matthew ^[2]; Luna, John M. ^[3]; Haiges, Ralf ^[3];

^[2];

^[3]

Univ. of Southern California, Los Angeles, CA (United States); Department of Chemistry, University of Southern California, Los Angeles, California 90089, United States
California Inst. of Technology (CalTech), Pasadena, CA (United States)
Univ. of Southern California, Los Angeles, CA (United States)

The bioinspired incorporation of pendant proton donors into transition metal catalysts is a promising strategy for converting environmentally deleterious CO₂ to higher energy products. However, the mechanism of proton transfer in these systems is poorly understood. Herein, we present a series of cobalt complexes with varying pendant secondary and tertiary amines in the ligand framework with the aim of disentangling the roles of the first and second coordination spheres in CO₂ reduction catalysis. Electrochemical and kinetic studies indicate that the rate of catalysis shows a first-order dependence on acid, CO₂, and the number of pendant secondary amines, respectively. Density functional theory studies explain the experimentally observed trends and indicate that pendant secondary amines do not directly transfer protons to CO₂, but instead bind acid molecules from solution. Taken together, these results suggest a mechanism in which noncooperative pendant amines facilitate a hydrogen-bonding network that enables direct proton transfer from acid to the activated CO₂ substrate.

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Research Organization:: California Inst. of Technology (CalTech), Pasadena, CA (United States)

Sponsoring Organization:: USDOE Office of Science (SC)

Grant/Contract Number:: SC0004993

OSTI ID:: 1498679

Journal Information:: ACS Central Science, Journal Name: ACS Central Science Journal Issue: 3 Vol. 4; ISSN 2374-7943

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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CCDC 1590218: Experimental Crystal Structure Determination Chapovetsky, Alon; Welborn, Matthew; Luna, John M. https://doi.org/10.5517/ccdc.csd.cc1qcrc6 The current record is supplemented by this dataset	dataset	January 2018
CCDC 1590219: Experimental Crystal Structure Determination Chapovetsky, Alon; Welborn, Matthew; Luna, John M. https://doi.org/10.5517/ccdc.csd.cc1qcrd7 The current record is supplemented by this dataset	dataset	January 2018
CCDC 1590220: Experimental Crystal Structure Determination Chapovetsky, Alon; Welborn, Matthew; Luna, John M. https://doi.org/10.5517/ccdc.csd.cc1qcrf8 The current record is supplemented by this dataset	dataset	January 2018
CCDC 1590221: Experimental Crystal Structure Determination Chapovetsky, Alon; Welborn, Matthew; Luna, John M. https://doi.org/10.5517/ccdc.csd.cc1qcrg9 The current record is supplemented by this dataset	dataset	January 2018

Title: Pendant Hydrogen-Bond Donors in Cobalt Catalysts Independently Enhance CO2 Reduction

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