Yan Jing, Kiana Amini, Dawei Xi, Shijian Jin, Abdulrahman M. Alfaraidi, Emily F. Kerr, Roy G. Gordon, Michael J. Aziz
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引用次数: 0
Abstract
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 a high current density by inexpensive, clean electricity. We show that deprotonated hydroquinone–CO2 adducts, whose insolubility limits the utility of the quinone–hydroquinone redox couple, become soluble when alkylammonium cations are introduced. Consequently, we introduced 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/release process, which occurs at ambient temperature and pressure, and show that it proceeds via both pH-swing and nucleophilicity-swing mechanisms. 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/mol CO2. 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 h. 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 the oxygen tolerance of reduced quinones may be significantly advanced through molecular engineering.
ACS Energy Letters Energy-Renewable Energy, Sustainability and the Environment
CiteScore
31.20
自引率
5.00%
发文量
469
审稿时长
1 months
期刊介绍:
ACS Energy Letters is a monthly journal that publishes papers reporting new scientific advances in energy research. The journal focuses on topics that are of interest to scientists working in the fundamental and applied sciences. Rapid publication is a central criterion for acceptance, and the journal is known for its quick publication times, with an average of 4-6 weeks from submission to web publication in As Soon As Publishable format.
ACS Energy Letters is ranked as the number one journal in the Web of Science Electrochemistry category. It also ranks within the top 10 journals for Physical Chemistry, Energy & Fuels, and Nanoscience & Nanotechnology.
The journal offers several types of articles, including Letters, Energy Express, Perspectives, Reviews, Editorials, Viewpoints and Energy Focus. Additionally, authors have the option to submit videos that summarize or support the information presented in a Perspective or Review article, which can be highlighted on the journal's website. ACS Energy Letters is abstracted and indexed in Chemical Abstracts Service/SciFinder, EBSCO-summon, PubMed, Web of Science, Scopus and Portico.