气候变化领域集成服务门户(CCPortal): Direct and continuous generation of pure acetic acid solutions via electrocatalytic carbon monoxide reduction

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DOI	10.1073/pnas.2010868118
	Direct and continuous generation of pure acetic acid solutions via electrocatalytic carbon monoxide reduction
	Zhu P.; Xia C.; Liu C.-Y.; Jiang K.; Gao G.; Zhang X.; Xia Y.; Lei Y.; Alshareef H.N.; Senftle T.P.; Wang H.
发表日期	2021
ISSN	00278424
卷号	118 期号:2
英文摘要	Electrochemical CO2 or CO reduction to high-value C2+ liquid fuels is desirable, but its practical application is challenged by impurities from cogenerated liquid products and solutes in liquid electrolytes, which necessitates cost- and energy-intensive downstream separation processes. By coupling rational designs in a Cu catalyst and porous solid electrolyte (PSE) reactor, here we demonstrate a direct and continuous generation of pure acetic acid solutions via electrochemical CO reduction. With optimized edge-to-surface ratio, the Cu nanocube catalyst presents an unprecedented acetate performance in neutral pH with other liquid products greatly suppressed, delivering a maximal acetate Faradaic efficiency of 43%, partial current of 200 mA·cm−2, ultrahigh relative purity of up to 98 wt%, and excellent stability of over 150 h continuous operation. Density functional theory simulations reveal the role of stepped sites along the cube edge in promoting the acetate pathway. Additionally, a PSE layer, other than a conventional liquid electrolyte, was designed to separate cathode and anode for efficient ion conductions, while not introducing any impurity ions into generated liquid fuels. Pure acetic acid solutions, with concentrations up to 2 wt% (0.33 M), can be continuously produced by employing the acetate-selective Cu catalyst in our PSE reactor. © 2021 National Academy of Sciences. All rights reserved.
英文关键词	CO reduction; CO2 reduction; Pure acetic acid; Solid electrolyte
语种	英语
scopus关键词	acetic acid; electrolyte; nanocube; porous solid electrolyte; unclassified drug; anion exchange; anion exchange membrane; Article; catalysis; chemical parameters; chemical phenomena; chemical reaction; concentration (parameter); conductance; controlled study; density functional theory; edge to surface ratio; electrocatalytic carbon monoxide reduction; electrochemical analysis; electron diffraction; Faradaic efficiency; hydrogen evolution reaction; ion conduction; molecular dynamics; pH; priority journal; process optimization; purification; scanning electron microscopy; selective area electron diffraction; simulation
来源期刊	Proceedings of the National Academy of Sciences of the United States of America
文献类型	期刊论文
条目标识符	http://gcip.llas.ac.cn/handle/2XKMVOVA/181046
作者单位	Department of Chemical and Biomolecular Engineering, Rice University, Houston, TX 77005, United States; Smalley-Curl Institute, Rice University, Houston, TX 77005, United States; School of Mechanical Engineering, Shanghai Jiao Tong University, Shanghai, 200240, China; Department of Materials Science and Nano-Engineering, Rice University, Houston, TX 77005, United States; Materials Science and Engineering, King Abdullah University of Science and Technology, Thuwal, 23955-6900, Saudi Arabia; Department of Chemistry, Rice University, Houston, TX 77005, United States; Canadian Institute for Advanced Research (CIFAR) Azrieli Global Scholar, MaRS Centre, Toronto, ON M5G 1M1, Canada
推荐引用方式 GB/T 7714	Zhu P.,Xia C.,Liu C.-Y.,et al. Direct and continuous generation of pure acetic acid solutions via electrocatalytic carbon monoxide reduction[J],2021,118(2).
APA	Zhu P..,Xia C..,Liu C.-Y..,Jiang K..,Gao G..,...&Wang H..(2021).Direct and continuous generation of pure acetic acid solutions via electrocatalytic carbon monoxide reduction.Proceedings of the National Academy of Sciences of the United States of America,118(2).
MLA	Zhu P.,et al."Direct and continuous generation of pure acetic acid solutions via electrocatalytic carbon monoxide reduction".Proceedings of the National Academy of Sciences of the United States of America 118.2(2021).