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dc.contributor.authorZhu, Peng
dc.contributor.authorXia, Chuan
dc.contributor.authorLiu, Chun-Yen
dc.contributor.authorJiang, Kun
dc.contributor.authorGao, Guanhui
dc.contributor.authorZhang, Xiao
dc.contributor.authorXia, Yang
dc.contributor.authorLei, Yongjiu
dc.contributor.authorAlshareef, Husam N
dc.contributor.authorSenftle, Thomas P
dc.contributor.authorWang, Haotian
dc.date.accessioned2021-01-03T13:26:12Z
dc.date.available2021-01-03T13:26:12Z
dc.date.issued2020-12-30
dc.identifier.citationZhu, P., Xia, C., Liu, C.-Y., Jiang, K., Gao, G., Zhang, X., … Wang, H. (2020). Direct and continuous generation of pure acetic acid solutions via electrocatalytic carbon monoxide reduction. Proceedings of the National Academy of Sciences, 118(2), e2010868118. doi:10.1073/pnas.2010868118
dc.identifier.issn0027-8424
dc.identifier.pmid33380454
dc.identifier.doi10.1073/pnas.2010868118
dc.identifier.urihttp://hdl.handle.net/10754/666799
dc.description.abstractElectrochemical 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.
dc.description.sponsorshipThis work was supported by NSF Grant 2029442 and Rice University. H.W. is a Canadian Institute for Advanced Research (CIFAR) Azrieli Global Scholar in the Bio-Inspired Solar Energy Program. C.X. acknowledges support from a J. Evans Attwell-Welch postdoctoral fellowship provided by the Smalley-Curl Institute. This work was performed in part at the Shared Equipment Authority at Rice University. The authors acknowledge the use of Electron Microscopy Center (EMC) at Rice University. Y.L. and H.N.A. acknowledge the support from King Abdullah University of Science and Technology. T.P.S. and C.-Y.L. acknowledge startup funding from Rice University.
dc.publisherProceedings of the National Academy of Sciences
dc.relation.urlhttp://www.pnas.org/lookup/doi/10.1073/pnas.2010868118
dc.rightsArchived with thanks to Proceedings of the National Academy of Sciences of the United States of America
dc.titleDirect and continuous generation of pure acetic acid solutions via electrocatalytic carbon monoxide reduction.
dc.typeArticle
dc.contributor.departmentMaterial Science and Engineering Program
dc.contributor.departmentPhysical Science and Engineering (PSE) Division
dc.identifier.journalProceedings of the National Academy of Sciences
dc.rights.embargodate2021-07-01
dc.eprint.versionPost-print
dc.contributor.institutionDepartment of Chemical and Biomolecular Engineering, Rice University, Houston, TX 77005.
dc.contributor.institutionSmalley-Curl Institute, Rice University, Houston, TX 77005.
dc.contributor.institutionSchool of Mechanical Engineering, Shanghai Jiao Tong University, Shanghai 200240, China.
dc.contributor.institutionDepartment of Materials Science and Nano-Engineering, Rice University, Houston, TX 77005.
dc.contributor.institutionDepartment of Chemistry, Rice University, Houston, TX 77005.
dc.contributor.institutionCanadian Institute for Advanced Research (CIFAR) Azrieli Global Scholar, MaRS Centre, Toronto, ON M5G 1M1, Canada.
dc.identifier.volume118
dc.identifier.issue2
dc.identifier.pagese2010868118
kaust.personLei, Yongjiu
kaust.personSenftle, Thomas P
dc.relation.issupplementedbygithub:tsenftle/CO_Acetate
display.relations<b>Is Supplemented By:</b><br/> <ul><li><i>[Software]</i> <br/> Title: tsenftle/CO_Acetate: Distributed as part of the publication "Direct and Continuous Generation of Pure Acetic Acid Solutions via Electrocatalytic Carbon Monoxide Reduction". Publication Date: 2020-04-02. github: <a href="https://github.com/tsenftle/CO_Acetate" >tsenftle/CO_Acetate</a> Handle: <a href="http://hdl.handle.net/10754/667867" >10754/667867</a></a></li></ul>
dc.date.published-online2020-12-30
dc.date.published-print2021-01-12


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