A Dicationic fac-Re(bpy)(CO)3Cl for CO2 Electroreduction at a Reduced Overpotential

Rotundo, Laura; Ahmad, Shahbaz; Cappuccino, Chiara; Polyansky, Dmitry E.; Ertem, Mehmed Z.; Manbeck, Gerald F.

doi:10.1021/acs.inorgchem.3c00624

Title: A Dicationic fac-Re(bpy)(CO)₃Cl for CO₂ Electroreduction at a Reduced Overpotential

Journal Article · 09 May 2023 · Inorganic Chemistry

DOI: https://doi.org/10.1021/acs.inorgchem.3c00624 · OSTI ID:1974193

^[1]; Ahmad, Shahbaz ^[1]; Cappuccino, Chiara ^[1];

^[1];

^[1]

Brookhaven National Lab. (BNL), Upton, NY (United States). Chemistry Div.

Here, a dicationic Re bipyridine-type complex, fac-Re(6,6'-(2-((trimethylammonio)-methyl)phenyl)-2,2'-bipyridine)(CO)₃Cl hexafluorophosphate (1²⁺), has been synthesized and its electrochemical behavior under Ar and CO₂ has been investigated. The presence of pendent tetra-alkylammonium cations induces an anodic shift in the electrocatalytic potential for CO₂ reduction relative to structurally similar model complexes. The electrochemical mechanisms in anhydrous CH₃CN and in the presence of weak acids (water or trifluoroethanol) have been analyzed using cyclic voltammetry assisted by infrared spectroelectrochemistry and theoretical calculations. The dication enables catalysis at a diminished potential through coulombic stabilization of the doubly reduced pentacoordinate species, its CO₂ adduct, the hydroxide anion, and the conjugate base formed during acid-assisted C-OH bond cleavage of the metallocarboxylic acid to the metallocarbonyl and H₂O. The major reduction product is CO, but in the presence of trifluoroethanol, formate is also produced with 14% Faradaic efficiency.

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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:: SC0012704; SC0021173

OSTI ID:: 1974193

Report Number(s):: BNL-224407-2023-JAAM

Journal Information:: Inorganic Chemistry, Vol. 62, Issue 20; ISSN 0020-1669

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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37 INORGANIC
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PHYSICAL AND ANALYTICAL CHEMISTRY
electrocatalysis
carbon dioxide reduction
mechanism
anions
catalysts
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redox reactions

Title: A Dicationic fac-Re(bpy)(CO)3Cl for CO2 Electroreduction at a Reduced Overpotential

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Title: A Dicationic fac-Re(bpy)(CO)₃Cl for CO₂ Electroreduction at a Reduced Overpotential