Evaluation of Aliphatic Alcohols for CO2 Capture Using the Characteristic Carbonate Frequency

Delibas, Berk; Cotton, Dani; Sudhakaran, Keerthy P.; Dawlaty, Jahan M.

doi:10.1002/cssc.202402288

Evaluation of Aliphatic Alcohols for CO₂ Capture Using the Characteristic Carbonate Frequency

Journal Article · Wed Dec 04 23:00:00 EST 2024 · ChemSusChem

DOI:https://doi.org/10.1002/cssc.202402288· OSTI ID:2997910

Delibas, Berk ^[1]; Cotton, Dani ^[1]; Sudhakaran, Keerthy P. ^[1]; ^[1]

University of Southern California, Los Angeles, CA (United States)

Control over CO₂ capture and utilization are important scientific and technological challenges. Although a variety of amine absorbents are used for capture, releasing the captured CO₂ is often difficult and limits their recyclability. Therefore, it is crucial to control the strength of the CO₂ bond with the absorbent. Furthermore, it is desirable to use a method that can conveniently report the strength of this bond. This motivates exploring adducts of CO₂ with alcohols in the presence of a base, using vibrational spectroscopy to report on the bond strength. Although reactions of alcohols with CO₂ to form alkyl carbonates are known, a systematic study of these adducts has not been conducted. Here we show formation of alkyl carbonates by a series of alcohols spanning the pK_a range 9.5 to 16.8. We show experimental and computational results for the frequency of the characteristic asymmetric stretch of the carbonate and demonstrate that it correlates inversely with the pK_a of the alcohol. Based on computations of the bond lengths and previous work, we propose that this frequency also correlates inversely with the adduct strength. As a result, this work extends the scope of CO₂ capture reagents and inspires further research in tuning alcohols as reversible absorbents.

View Accepted Manuscript (DOE)

Research Organization:: University of Illinois, Champaign, IL (United States)

Sponsoring Organization:: USDOE; National Science Foundation (NSF)

Grant/Contract Number:: SC0022173

OSTI ID:: 2997910

Journal Information:: ChemSusChem, Journal Name: ChemSusChem Journal Issue: 8 Vol. 18; ISSN 1864-5631; ISSN 1864-564X

Publisher:: WileyCopyright Statement

Country of Publication:: United States

Language:: English

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Evaluation of Aliphatic Alcohols for CO2 Capture Using the Characteristic Carbonate Frequency

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Evaluation of Aliphatic Alcohols for CO₂ Capture Using the Characteristic Carbonate Frequency