Probing Electrolyte Influence on CO2 Reduction in Aprotic Solvents

Gomes, Reginaldo J.; Birch, Chris; Cencer, Morgan M.; Li, Chenyang; Son, Seoung-Bum; Bloom, Ira D.; Assary, Rajeev S.; Amanchukwu, Chibueze V.

doi:10.1021/acs.jpcc.2c03321

Title: Probing Electrolyte Influence on CO₂ Reduction in Aprotic Solvents

Journal Article · 04 August 2022 · Journal of Physical Chemistry. C

DOI: https://doi.org/10.1021/acs.jpcc.2c03321 · OSTI ID:1923257

Gomes, Reginaldo J. ^[1]; Birch, Chris ^[1];

^[2];

^[1]

University of Chicago, IL (United States)
Argonne National Lab. (ANL), Lemont, IL (United States)

Selective CO₂ capture and electrochemical conversion are important tools in the fight against climate change. Industrially, CO₂ is captured using a variety of aprotic solvents due to their high CO₂ solubility. However, most research efforts on electrochemical CO₂ conversion use aqueous media and are plagued by competing hydrogen evolution reaction (HER) from water breakdown. Fortunately, aprotic solvents can circumvent HER, making it important to develop strategies that enable integrated CO₂ capture and conversion. However, the influence of ion solvation and solvent selection within nonaqueous electrolytes for efficient and selective CO₂ reduction is unclear. In this work, we show that the bulk solvation behavior within the nonaqueous electrolyte can control the CO2 reduction reaction and product distribution occurring at the catalyst-electrolyte interface. We study different tetrabutylammonium (TBA) salts in two electrolyte systems with glyme ethers (e.g., 1,2 dimethoxyethane or DME) and dimethyl sulfoxide (DMSO) as a low and high dielectric constant medium, respectively. Using spectroscopic tools, we quantify the fraction of ion pairs that forms within the electrolyte. Also, we show how ion pair formation is prevalent in DME and is dependent on the anion type. More importantly, we show that as ion pair formation decreases within the electrolyte, CO₂ current densities increase, and a higher CO Faradaic efficiency is observed at low overpotentials. Meanwhile, in an electrolyte medium where the ion pair fraction does not change with the anion type (such as in DMSO), a smaller influence of solvation is observed on CO₂ current densities and product distribution. By directly coupling bulk solvation to interfacial reactions and product distribution, we showcase the importance and utility of controlling the reaction microenvironment in tuning the electrocatalytic reaction pathways. Insights gained from this work will enable novel electrolyte designs for efficient and selective CO₂ conversion to desired fuels and chemicals.

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Research Organization:: Argonne National Laboratory (ANL), Lemont, IL (United States)

Sponsoring Organization:: Neubauer Family Assistant Professors program; USDOE Office of Energy Efficiency and Renewable Energy (EERE), Transportation Office. Bioenergy Technologies Office; University of Chicago

Grant/Contract Number:: AC02-06CH11357

OSTI ID:: 1923257

Journal Information:: Journal of Physical Chemistry. C, Journal Name: Journal of Physical Chemistry. C Journal Issue: 32 Vol. 126; ISSN 1932-7447

Publisher:: American Chemical SocietyCopyright Statement

Country of Publication:: United States

Language:: English

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Title: Probing Electrolyte Influence on CO₂ Reduction in Aprotic Solvents