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Phosphine Modulation for Enhanced CO₂ Capture: Quantum Mechanics Predictions of New Materials

Musgrave, Charles B., III and Prokofjevs, Aleksandrs and Goddard III, William A. (2022) Phosphine Modulation for Enhanced CO₂ Capture: Quantum Mechanics Predictions of New Materials. Journal of Physical Chemistry Letters, 13 (48). pp. 11183-11190. ISSN 1948-7185. doi:10.1021/acs.jpclett.2c03145.

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It is imperative to develop efficient CO₂ capture and activation technologies to combat the rising levels of deleterious greenhouse gases in the atmosphere. Using Quantum Mechanics methods (Density Functional Theory), we propose and evaluate several metal-free and metal-containing phosphines that provide strong CO₂ binding under ambient conditions. Depending on the electron donating capacity of the phosphine and the ability of the P-bound ligands to hydrogen bond to the CO₂, we find that the CO₂ binding can be as strong as −18.6 kcal/mol downhill, which should be quite adequate for ambient conditions. We explore some modifications of the phosphine to improve CO₂ binding, and we elucidate which chemical descriptors correlate directly with CO₂ binding energy. Specifically, we find that charge accumulation on the CO₂ unit of the CO₂-bound adduct has the greatest correlation with CO₂ binding affinity. Finally, we probe the mechanism for CO₂ reduction to CO and methanol in aqueous media.

Item Type:Article
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URLURL TypeDescription
Musgrave, Charles B., III0000-0002-3432-0817
Goddard III, William A.0000-0003-0097-5716
Alternate Title:Phosphine Modulation for Enhanced CO2 Capture: Quantum Mechanics Predictions of New Materials
Additional Information:C.B.M. and W.A.G. acknowledge support from the Liquid Sunlight Alliance, which is supported by the U.S. Department of Energy, Office of Science, Office of Basic Energy Sciences, Fuels from Sunlight Hub under Award No. DE-SC0021266.
Group:Liquid Sunlight Alliance
Funding AgencyGrant Number
Department of Energy (DOE)DE-SC0021266
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Issue or Number:48
Record Number:CaltechAUTHORS:20221216-550380000.5
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Usage Policy:No commercial reproduction, distribution, display or performance rights in this work are provided.
ID Code:118394
Deposited By: Research Services Depository
Deposited On:17 Dec 2022 15:08
Last Modified:22 Dec 2022 20:41

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