Methane Generation from CO2 with a Molecular Rhenium Catalyst

Nganga, John K.; Wolf, Lucienna M.; Mullick, Kankana; Reinheimer, Eric; Saucedo, Cesar; Wilson, Megan E.; Grice, Kyle A.; Ertem, Mehmed Z.; Angeles-Boza, Alfredo M.

doi:10.1021/acs.inorgchem.0c02579

Title: Methane Generation from CO₂ with a Molecular Rhenium Catalyst

Journal Article · Mon Feb 22 00:00:00 EST 2021 · Inorganic Chemistry

DOI:https://doi.org/10.1021/acs.inorgchem.0c02579· OSTI ID:1784495

Nganga, John K. ^[1]; Wolf, Lucienna M. ^[2]; Mullick, Kankana ^[1]; Reinheimer, Eric ^[3]; Saucedo, Cesar ^[2]; Wilson, Megan E. ^[2];

^[2];

^[4];

^[5]

Univ. of Connecticut, Storrs, CT (United States)
DePaul Univ., Chicago, IL (United States)
Rigaku, The Woodlands, TX (United States)
Brookhaven National Lab. (BNL), Upton, NY (United States)
Univ. of Connecticut, Storrs, CT (United States); Univ. of Connecticut, Storrs, CT (United States). Inst. of Materials Science

The atomic-level tunability of molecular structures is a compelling reason to develop homogeneous catalysts for challenging reactions such as the electrochemical reduction of carbon dioxide to valuable C₁–C_n products. Of particular interest is methane, the largest component of natural gas. Herein, we report a series of three isomeric rhenium tricarbonyl complexes coordinated by the asymmetric diimine ligands 2-(isoquinolin-1-yl)-4,5-dihydrooxazole (quin-1-oxa), 2-(quinolin-2-yl)-4,5-dihydrooxazole (quin-2-oxa), and 2-(isoquinolin-3-yl)-4,5-dihydrooxazole (quin-3-oxa) that catalyze the reduction of CO₂ to carbon monoxide and methane, albeit the latter with a low efficiency. To our knowledge, these complexes are the first examples of rhenium(I) catalysts capable of converting carbon dioxide into methane. Re(quin-1-oxa)(CO)₃Cl (1), Re(quin-2-oxa)(CO)₃Cl (2), and Re(quin-3-oxa)(CO)₃Cl (3) were characterized and studied using a variety of electrochemical and spectroscopic techniques. In bulk electrolysis experiments, the three complexes reduce CO₂ to CO and CH₄. When the controlled-potential electrolysis experiments are performed at -2.5 V (vs Fc^+/0) and in the presence of the Brønsted acid 2,2,2-trifluoroethanol, methane is produced with turnover numbers that range from 1.3 to 1.8. Isotope labeling experiments using ¹³CO₂ atmosphere produce ¹³CH₄ (m/z = 17) confirming that methane originates from CO₂ reduction. Theoretical calculations are performed to investigate the mechanistic aspects of the 8e^–/8H⁺ reduction of CO₂ to CH₄. Overall, a ligand-assisted pathway is proposed to be an efficient pathway in the formation of CH₄. Delocalization of the electron density on the (iso)quinoline moiety upon reduction stabilizes the key carbonyl intermediate leading to additional reactivity of this ligand. These results should aid the development of more robust catalytic systems that produce CH₄ from CO₂.

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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); National Science Foundation (NSF)

Grant/Contract Number:: SC0012704; CHE-1652606; 1411219

OSTI ID:: 1784495

Report Number(s):: BNL-221391-2021-JAAM

Journal Information:: Inorganic Chemistry, Vol. 60, Issue 6; ISSN 0020-1669

Publisher:: American Chemical Society (ACS)Copyright Statement

Country of Publication:: United States

Language:: English

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Title: Methane Generation from CO2 with a Molecular Rhenium Catalyst

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Title: Methane Generation from CO₂ with a Molecular Rhenium Catalyst