Synthesis and Evaluation of Electroactive CO<sub>2</sub> Carriers

Bell, William L.; Miedaner, Alex; Smart, James C.; DuBois, Daniel L.; Verostko, Charles E.

doi:10.4271/881078

Cited by 18 publications

(48 citation statements)

References 9 publications

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“…Since then, a number of systems have been developed for transporting chemical species by redox-active carriers that are activated at one electrode, to bind with the target species, and deactivated at the opposite electrode, to release the target and regenerate the carrier. 15,16 Systems that have been proposed for the concentration of CO 2 through this approach have been based on a number of different carrier molecules, such as quinones, [17][18][19][20] 4,4 0 -bipyridine, 21 and thiolates. 22,23 Quinones are of particular interest to this work for their superior electrochemical performance, serving as redox-active carriers for CO 2 in electrochemically mediated separation processes.…”

Section: Introductionmentioning

confidence: 99%

Faradaic electro-swing reactive adsorption for CO₂ capture

Voskian

Hatton

2019

Energy Environ. Sci.

213

263

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Section: Introductionmentioning

confidence: 99%

Faradaic electro-swing reactive adsorption for CO₂ capture

Voskian

Hatton

2019

Energy Environ. Sci.

213

263

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“…Several classes of redox-active carriers have been investigated for eCCC applications including bipyridines, [7][8][9] thiols, 10 and quinones. [11][12][13][14][15][16][17][18] However, eCCC systems generally degrade from aerobic input streams because the reduced carriers react with oxygen (O2) resulting in unproductive carrier oxidation and the generation of superoxide, which can cause destructive radical reactions with the carrier, solvent, or electrolyte (red reaction in Scheme 1). 19,20 Since oxygen is present in flue gas and atmospheric CO2 sources, practical eCCC methods must overcome this limitation.…”

mentioning

confidence: 99%

Oxygen Stable Electrochemical CO2 Capture and Concentration through Alcohol Additives

Yang

Barlow

2021

Preprint

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Current methods for CO2 capture and concentration (CCC) are energy intensive due to their reliance on thermal cycles, which are intrinsically Carnot limited in efficiency. In contrast, electrochemically driven CCC (eCCC) can operate at much higher theoretical efficiencies. However, most reported systems are sensitive to O2, precluding their practical use. In order to achieve O2 stable eCCC, we pursued the development of molecular redox carriers with reduction potentials positive of the O2/O2- redox couple. Prior efforts to chemically modify redox carriers to operate at milder potentials resulted in a loss in CO2 binding. To overcome these limitations, we used common alcohols additives to anodically shift the reduction potential of a quinone redox carrier, 2,3,5,6-tetrachloro-p-benzoquinone (TCQ), by up to 350 mV, conferring O2 stability. Intermolecular hydrogen-bonding interactions to the dianion and CO2-bound forms of TCQ were correlated to alcohol pKa to identify ethanol as the optimal additive, as it imparts beneficial changes to both the reduction potential and CO2 binding constant, the two key properties for eCCC redox carriers. We demonstrate a full cycle of eCCC in aerobic simulated flue gas using TCQ and ethanol, two commercially available compounds. Based on the system properties, an estimated minimum of 21 kJ/mol is required to concentrate CO2 from 10% to 100%, or twice as efficient as state-of-the-art thermal amine capture systems and other reported redox carrier-based systems. Furthermore, this approach of using hydrogen-bond donor additives is general and can be used to tailor the redox properties of other quinones/alcohol combinations for specific CO2 capture applications.

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“…The redox mechanism facilitates the pumping of CO 2 from the cathode to the anode side as the carrier compound gets reduced at the cathode and oxidized at the anode. DuBois and coworkers ( Bell et al., 1988 ) in 1988 examined electroactive species in quest of regenerable CO 2 removal systems for the National Aeronautics and Space Administration's long space missions. Simpson et al.…”

Section: Electrochemically Mediated Co 2 Separationmentioning

confidence: 99%

Perspective and challenges in electrochemical approaches for reactive CO2 separations

Gurkan

Klemm

et al. 2021

iScience

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Summary The desire toward decarbonization and renewable energy has sparked research interests in reactive CO 2 separations, such as direct air capture that utilize electricity as opposed to conventional thermal and pressure swing processes, which are energy-intensive, cost-prohibitive, and fossil-fuel dependent. Although the electrochemical approaches in CO 2 capture that support negative emissions technologies are promising in terms of modularity, smaller footprint, mild reaction conditions, and possibility to integrate into conversion processes, their practice depends on the wider availability of renewable electricity. This perspective discusses key advances made in electrolytes and electrodes with redox-active moieties that reversibly capture CO 2 or facilitate its transport from a CO 2 -rich side to a CO 2 -lean side within the last decade. In support of the discovery of new heterogeneous electrode materials and electrolytes with redox carriers, the role of computational chemistry is also discussed.

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Synthesis and Evaluation of Electroactive CO₂ Carriers

Cited by 18 publications

References 9 publications

Faradaic electro-swing reactive adsorption for CO₂ capture

Faradaic electro-swing reactive adsorption for CO₂ capture

Oxygen Stable Electrochemical CO2 Capture and Concentration through Alcohol Additives

Perspective and challenges in electrochemical approaches for reactive CO2 separations

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Synthesis and Evaluation of Electroactive CO2 Carriers

Cited by 18 publications

References 9 publications

Faradaic electro-swing reactive adsorption for CO2 capture

Faradaic electro-swing reactive adsorption for CO2 capture

Oxygen Stable Electrochemical CO2 Capture and Concentration through Alcohol Additives

Perspective and challenges in electrochemical approaches for reactive CO2 separations

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Synthesis and Evaluation of Electroactive CO₂ Carriers

Faradaic electro-swing reactive adsorption for CO₂ capture

Faradaic electro-swing reactive adsorption for CO₂ capture