Push or Pull? Proton Responsive Ligand Effects in Rhenium Tricarbonyl CO 2 Reduction Catalysts

Manbeck, Gerald F.; Muckerman, James T.; Szalda, David J.; Himeda, Yuichiro; Fujita, Etsuko

doi:10.1021/jp511131x

Title: Push or Pull? Proton Responsive Ligand Effects in Rhenium Tricarbonyl CO ₂ Reduction Catalysts

Journal Article · Thu Feb 19 00:00:00 EST 2015 · Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry

DOI:https://doi.org/10.1021/jp511131x· OSTI ID:1182537

Manbeck, Gerald F. ^[1]; Muckerman, James T. ^[1]; Szalda, David J. ^[2]; Himeda, Yuichiro ^[3]; Fujita, Etsuko ^[1]

Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry
Brookhaven National Lab. (BNL), Upton, NY (United States). Dept. of Chemistry; City Univ. (CUNY), NY (United States). Buruch College. Dept. of Natural Science
National Inst. of Advanced Industrial Science and Technology (AIST), Tsukuba (Japan); Japan Science and Technology Agency (JST), Saitama (Japan)

Proton responsive ligands offer control of catalytic reactions through modulation of pH-dependent properties, second coordination sphere stabilization of transition states, or by providing a local proton source for multi-proton, multi-electron reactions. Two fac-[ReI(α-diimine)(CO)₃Cl] complexes with α-diimine = 4,4'- (or 6,6'-) dihydroxy-2,2'-bipyridine (4DHBP and 6DHBP) have been prepared and analyzed as electrocatalysts for reduction of carbon dioxide. Consecutive electrochemical reduction of these complexes yields species identical to those obtained by chemical deprotonation. An energetically feasible mechanism for reductive deprotonation is proposed in which the bpy anion is protonated followed by loss of H₂ and 2H⁺. Cyclic voltammetry reveals a two-electron, three-wave system owing to competing EEC and ECE pathways. The chemical step of the ECE pathway might be attributed to the reductive deprotonation. but cannot be distinguished from chloride dissociation. The rate obtained by digital simulation is approximately 8 s⁻¹. Under CO₂, these competing reactions generate a two-slope catalytic waveform with onset potential of –1.65 V vs Ag/AgCl. Reduction of CO₂ to CO by the [ReI (4DHBP–2H⁺)(CO)₃]⁻ suggests the interaction of CO₂ with the deprotonated species or a third reduction followed by catalysis. Conversely, the reduced form of [Re(6DHBP)(CO)₃Cl] converts CO₂ to CO with a single turnover.

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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES)

Grant/Contract Number:: SC00112704

OSTI ID:: 1182537

Report Number(s):: BNL-107638-2015-JA; R&D Project: CO026; KC0304030

Journal Information:: Journal of Physical Chemistry. B, Condensed Matter, Materials, Surfaces, Interfaces and Biophysical Chemistry, Vol. 119, Issue 24; ISSN 1520-6106

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Cited by: 81 works

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Proton responsive ligands
chemical deprotonation
chloride dissociation
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Title: Push or Pull? Proton Responsive Ligand Effects in Rhenium Tricarbonyl CO 2 Reduction Catalysts

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Title: Push or Pull? Proton Responsive Ligand Effects in Rhenium Tricarbonyl CO ₂ Reduction Catalysts