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Record W4387668418 · doi:10.26434/chemrxiv-2023-nfg6z

Electrochemically induced CO2 capture enabled by aqueous quinone flow chemistry

2023· preprint· en· W4387668418 on OpenAlexfundno aff
Yan Jing, Kiana Amini, Dawei Xi, Shijian Jin, Abdulrahman Alfaraidi, Emily F. Kerr, Roy G. Gordon, Michael J. Aziz

Bibliographic record

VenueChemRxiv · 2023
Typepreprint
Languageen
FieldEnergy
TopicCO2 Reduction Techniques and Catalysts
Canadian institutionsnot available
FundersPacific Northwest National LaboratoryNatural Sciences and Engineering Research Council of CanadaU.S. Department of Energy
KeywordsHydroquinoneQuinoneChemistryAqueous solutionRedoxAnthraquinoneDeprotonationBar (unit)ElectrochemistryInorganic chemistryOrganic chemistryElectrodePhysical chemistryIon

Abstract

fetched live from OpenAlex

Climate change caused by the accumulation of anthropogenic CO2 emissions motivates the development and deployment of cost-effective, scalable, and energetically efficient techniques to capture CO2 from point or diffuse sources. Electrochemically-driven CO2 capture processes utilizing redox-active organics in aqueous flow chemistry show promise for nonflammability, continuous-flow engineering, and the possibility of being driven at high current density by inexpensive, clean electricity. We show that the deprotonated hydroquinone-CO2 adducts, whose insolubility limits the utility of the quinone-hydroquinone redox couple, become soluble when alkylammonium cations are introduced. Consequently, we introduce alkylammonium groups to anthraquinone via covalent bonds, making the resulting bis[3-(trimethylammonio)propyl]-anthraquinones (BTMAPAQs) soluble. We report the first aqueous quinone flow chemistry-enabled electrochemical CO2 capture process, which occurs at ambient temperature and pressure, and show that it proceeds via both a pH-swing and a nucleophilicity-swing mechanism. 1,5-BTMAPAQ reaches the theoretical capture capacity of two CO2 molecules per quinone from 1-bar CO2-N2 mixtures for which the CO2 partial pressure is as low as 0.05 bar, or the applied current density is as high as 100 mA/cm2, or the organic concentration is as high as 0.4 M. The energetic cost ranges from 48 to 140 kJ/molCO2. In a crude simulated flue gas composed of 3% O2, 10% CO2, and 87% N2, 1,5-BTMAPAQ electrolyte reversibly captured and released 50% of the theoretical capacity during an exposure of over 4 hr. It outperforms its isomeric counterparts 1,4-, and 1,8-BTMAPAQ in capture capacity and O2 tolerance, demonstrating a substituent position effect on the reactivity of isomers with CO2 and O2. The results provide fundamental insight into electrochemical CO2 capture with aqueous quinone flow chemistry and suggest that oxygen tolerance of reduced quinones may be significantly advanced through molecular engineering.

Fetched live from OpenAlex and de-inverted. Abstracts are not stored in this database: the inverted indexes are 8.6 GB of the frame’s 9.3 GB of text, and the host has 13 GB free.

How this classification was reachedexpand

Full frame distilled prediction

Teacher imitation

Not calibrated prevalence, not ground truth. Human validation pending. Learned from the 10,348 direct Codex labels and 10,348 direct Gemma labels. Candidate is the union of thresholded teacher heads; consensus is their intersection. These outputs are machine_predicted_unvalidated and are not human labels or direct frontier model labels.

metaresearch head score (Codex)0.000
metaresearch head score (Gemma)0.000
Version: codex-gemma-dda1882f352aValidation status: machine_predicted_unvalidated
Candidate categoriesMeta-epidemiology (narrow), Research integrity, Insufficient payload (model declined to judge)
Consensus categoriesnone
DomainCandidate signal: none · Consensus signal: none
Study designCandidate signal: Bench or experimental · Consensus signal: Bench or experimental
GenreCandidate signal: Empirical · Consensus signal: Empirical
Teacher disagreement score0.062
Threshold uncertainty score1.000

Codex and Gemma teacher scores by category

CategoryCodexGemma
Metaresearch0.0000.000
Meta-epidemiology (narrow)0.0010.001
Meta-epidemiology (broad)0.0010.000
Bibliometrics0.0000.000
Science and technology studies0.0000.000
Scholarly communication0.0000.000
Open science0.0010.001
Research integrity0.0020.002
Insufficient payload (model declined to judge)0.0010.000

Machine scores (provisional)

The two teacher heads of the student model, read on this work. A score orders the frame for review; it never asserts a category, and the validation status ships verbatim with every row.

Baseline scores from an immature model (maturity gate not passed, 7 training rounds). Scores rank; they never assert a category.

Opus teacher head0.013
GPT teacher head0.235
Teacher spread0.222 · how far apart the two teachers sit on this one work
Validation statusscore_only:v0-immature-baseline · verbatim from the scoring run: score_only means the number may rank works, and no category label ships from it

Classification

machine, unvalidated

Machine predicted; a candidate call from one teacher head, not a consensus.

Study designBench or experimental
Domainnot available
GenreEmpirical

How this classification was reached, model by model and score by score, is at the end of the page under "How this classification was reached".

Quick stats

Citations6
Published2023
Admission routes1
Has abstractyes

Explore more

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