Molecular design of redox carriers for electrochemical CO<sub>2</sub> capture and concentration

Barlow, Jeffrey M.; Clarke, Lauren E.; Zhang, Zisheng; Bím, Daniel; Ripley, Katelyn M.; Zito, Alessandra; Brushett, Fikile R.; Alexandrova, Anastassia N.; Yang, Jenny Y.

doi:10.1039/d2cs00367h

Cited by 31 publications

(33 citation statements)

References 67 publications

(136 reference statements)

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“…Without sophisticated modeling, the energy consumption for the production of HCl and NaOH based on the chloralkali process (brine electrolysis) can be translated for the regeneration cost, approximately 4–18 kWh/m 3 desalinated water at 3–15 g/L salinity based on the energy consumption of the chloralkali process . Therefore, further developments in desalination in continuous flow reactors and their combination with CO 2 capture and sequestration processes are foreseeable by coupling with electrochemical pH swing for efficient column regeneration. , This is to improve the efficiency of the regeneration step, which is the only step that requires an energy input. Further developments in advanced polymers, resins, and porous materials with high amine loadings that allow facile diffusion of ions and their exchange are expected to overcome the current limitations associated with the slow “CO 2 -treatment” step, in order to utilize ambient CO 2 sources, for example, from flue gas or even directly from air.…”

Section: Discussionmentioning

confidence: 99%

Carbon Dioxide-Mediated Desalination

et al. 2023

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Conventional desalination membrane technologies, although offer portable drinking water, are still energy-intensive processes. This paper proposes a potentially new approach for performing water desalination and purification by utilizing the reversible interaction of carbon dioxide (CO 2 ) with nucleophilic amines� reminiscent of the Solvay process. Based on our model studies with small molecules, CO 2 -responsive amphiphilic insoluble diamines were prepared, characterized, and applied in the formation of soda and ammonium chloride upon exposure to ambient CO 2 (1 atm), thus removing chloride ions from model and real seawater. This ion-exchange process and separation of chloride from the aqueous phase are spontaneous in the presence of CO 2 without the need for external energy sources. We demonstrate a flow system to envisage energy-efficient CO 2 -mediated desalination and simultaneous carbon capture and sequestration.

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Section: Discussionmentioning

confidence: 99%

Carbon Dioxide-Mediated Desalination

et al. 2023

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“…Therefore, we expect competition in solution between the formation of cation−(solvent) n −anion and cation−(solvent) n −reduced quinone ion pairs. With lithium-based supporting salts as examples, 7 Li chemical shift is sensitive to the solvation environment; a downfield shift indicates weaker interaction between Li + and its solvation shell (solvent and anion), thereby decreasing the cation's shielding. 35−37 As shown in Figure S10b, a downfield trend was observed in the order of TFSI − < OTf − < ClO 4 − (chemical shifts referenced to a LiCl in D 2 O internal standard in a coaxial configuration), which follows a positive correlation with k bimolecular .…”

Section: Effect Of Supporting Electrolyte Anions On Co 2 Complexation...mentioning

confidence: 99%

“…In EMCC processes, CO 2 capture and release are driven by gradients in electrical potential, which can be sourced from renewable energy. Compared to temperature-swing methods, EMCC can be operated isothermally, does not face the Carnot efficiency limit, and offers great design flexibility and modularity to adjust to various industrial scales. − …”

Section: Introductionmentioning

confidence: 99%

Assessing the Kinetics of Quinone–CO₂ Adduct Formation for Electrochemically Mediated Carbon Capture

Zheng

Musgrave

et al. 2023

ACS Sustainable Chem. Eng.

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Carbon capture driven by renewable electricity represents a promising approach to mitigate carbon dioxide (CO 2 ) emissions and combat climate change. Electrochemically mediated carbon capture can be achieved by developing redox-active Lewis bases, with quinones being the most representative chemistry. In aprotic electrolytes, a subset of quinoid species can selectively uptake CO 2 from a dilute feed upon electro-reduction via a nucleophilic addition reaction and release a concentrated CO 2 product stream upon oxidation. However, there is a lack of quantitative understanding of the reaction kinetics landscape of redox-active CO 2 sorbents, especially considering the complex nature of the multi-component electrolyte media they must be deployed in. To bridge this knowledge gap, we investigate the bimolecular reaction rate constant between CO 2 and radical anions of various quinones in a range of electrolytes using an electroanalytical technique. Combined with molecular dynamics and density functional theory calculations, we provide insights into the complex interplay between quinone chemistry, supporting salt composition, and electrolyte solvents on the intrinsic CO 2 adduct formation kinetics. To summarize some key observations, we found that the reaction rate is affected by both the identity and concentration of the cationic and anionic species in the supporting electrolyte, the presence of hydrogen-bonding additives may accelerate the kinetics, and orthoisomers of quinones have a faster reaction rate than para-isomers. We believe the work can help guide the rational design of electrochemical microenvironments for enhanced electrochemically mediated carbon capture performance.

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“…Electrochemical carbon capture and concentration (eCCC) offers a promising alternative to thermochemical processes as it circumvents the limitations of temperature-driven capture and release. [39][40][41][42][43] More specifically, electrochemical carbon capture systems are not bounded by Carnot efficiencies, and can theoretically approach operation at the thermodynamic minimum energy requirement (i.e., 100% energetic efficiencies). 41 As such, in electrochemical systems, the minimum cell potential (𝐸 cell ) is related to the minimum separation work (represented by the change in Gibbs free energy).…”

Section: δ𝐺 = −𝑅𝑇 Ln (mentioning

confidence: 99%

“…Beyond having adequate CO2 binding affinities while maintaining a minimal potential difference between binding and release steps, additional desirable characteristics of capture molecules include: rapid electron transfer kinetics, high solubility, stability of the carrier species towards other compounds present in a given feed gas composition (e.g., oxygen, water vapor), among others. 42,43,125 Overall, several different classes of molecules have been identified and assessed as capture molecule candidates.…”

Section: Introductionmentioning

confidence: 99%

Electrochemical Carbon Dioxide Capture and Concentration

Zito

Clarke

Barlow

et al. 2022

Preprint

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Electrochemical carbon capture and concentration (eCCC) offers a promising alternative to thermochemical processes as it circumvents the limitations of temperature-driven capture and release. This review will begin by discussing the history of eCCC, describing early work in the field and the motivation for pursuing such a process. We will then transition towards discussing more recent approaches, with a heavier emphasis on methods that employ redox mediators to facilitate CO2 capture and release. These methods rely more on optimization through chemical design and include pH-mediated systems, electrochemically-mediated amine regeneration, and direct capture with redox-active molecules. For each approach, we provide a general overview of the system, discuss redox mediator chemistries that have been studied in literature, and highlight requirements for future generations of redox mediators. We also describe previous demonstrations of each method and current cell/system designs that have been used at the lab-scale. To conclude, we summarize achievements in the field, current challenges, and opportunities for improving these technologies. Overall, this review is a comprehensive survey of the eCCC field and evaluates the chemical, theoretical, and electrochemical engineering aspects of this approach. We hope this work can be used to assist the community in the development of modern economical eCCC technologies that can be utilized in large-scale CCS processes.

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Molecular design of redox carriers for electrochemical CO₂ capture and concentration

Abstract: Developing improved methods for CO2 capture and concentration (CCC) is essential to mitigating the impact of our current emissions and can lead to net carbon negative technologies.

Cited by 31 publications

References 67 publications

Carbon Dioxide-Mediated Desalination

Carbon Dioxide-Mediated Desalination

Assessing the Kinetics of Quinone–CO₂ Adduct Formation for Electrochemically Mediated Carbon Capture

Electrochemical Carbon Dioxide Capture and Concentration

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Molecular design of redox carriers for electrochemical CO2 capture and concentration

Abstract: Developing improved methods for CO2 capture and concentration (CCC) is essential to mitigating the impact of our current emissions and can lead to net carbon negative technologies.

Cited by 31 publications

References 67 publications

Carbon Dioxide-Mediated Desalination

Carbon Dioxide-Mediated Desalination

Assessing the Kinetics of Quinone–CO2 Adduct Formation for Electrochemically Mediated Carbon Capture

Electrochemical Carbon Dioxide Capture and Concentration

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Product

Resources

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Molecular design of redox carriers for electrochemical CO₂ capture and concentration

Assessing the Kinetics of Quinone–CO₂ Adduct Formation for Electrochemically Mediated Carbon Capture