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One reaction that can be performed with high selectivity and durability is the electrochemical conversion of CO<jats:sub>2<\/jats:sub> to formic acid and in\u2010situ esterification with methanol to produce methyl formate. However, the translation to a high\u2010performance flow electrolyzer is far from trivial, as the non\u2010aqueous catholyte leads to reactor challenges including flooding the gas diffusion electrode. Here, a two\u2010membrane flow electrolyzer with both anion and cation exchange membranes was used with flowing methanol catholyte and aqueous anolyte. This design prevented methanol from flooding the cathode, which was a pervasive limiting issue for electrolyzers with a single membrane. Methyl formate production at 42.9\u2009% faradaic efficiency was achieved with pure methanol in a flow electrolyzer with stable performance beyond 80\u2005min. However, low\u2010water\u2010content catholyte compositions also led to increased cell resistance and lower operating current densities. Thus, with the present ionomer materials there is a tradeoff between methyl formate selectivity and current density depending on water concentration, highlighting a need for new ionomers tailored for desirable non\u2010aqueous solvents such as methanol.<\/jats:p>","DOI":"10.1002\/cssc.202301337","type":"journal-article","created":{"date-parts":[[2023,11,6]],"date-time":"2023-11-06T16:23:31Z","timestamp":1699287811000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":5,"title":["Two\u2010Membrane Dual Non\u2010Aqueous\/Aqueous Electrolyte Flow Cell Operation for Electrochemical Conversion of CO<sub>2<\/sub> to Methyl Formate"],"prefix":"10.1002","volume":"17","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-2061-4646","authenticated-orcid":false,"given":"Manu","family":"Gautam","sequence":"first","affiliation":[{"name":"Conn Center for Renewable Energy Research University of Louisville  Louisville Kentucky 40292 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0368-1150","authenticated-orcid":false,"given":"Francois","family":"Nkurunziza","sequence":"additional","affiliation":[{"name":"Conn Center for Renewable Energy Research University of Louisville  Louisville Kentucky 40292 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8062-9252","authenticated-orcid":false,"given":"Matthew C.","family":"Mulvehill","sequence":"additional","affiliation":[{"name":"Conn Center for Renewable Energy Research University of Louisville  Louisville Kentucky 40292 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8049-1748","authenticated-orcid":false,"given":"Sandesh S.","family":"Uttarwar","sequence":"additional","affiliation":[{"name":"Conn Center for Renewable Energy Research University of Louisville  Louisville Kentucky 40292 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8638-2465","authenticated-orcid":false,"given":"Dillon T.","family":"Hofsommer","sequence":"additional","affiliation":[{"name":"Department of Chemistry University of Louisville  2320 South Brook Street 40292 Louisville Kentucky USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-4889-2645","authenticated-orcid":false,"given":"Craig A.","family":"Grapperhaus","sequence":"additional","affiliation":[{"name":"Department of Chemistry University of Louisville  2320 South Brook Street 40292 Louisville Kentucky USA"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-2987-0865","authenticated-orcid":false,"given":"Joshua M.","family":"Spurgeon","sequence":"additional","affiliation":[{"name":"Conn Center for Renewable Energy Research University of Louisville  Louisville Kentucky 40292 USA"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2023,11,17]]},"reference":[{"key":"e_1_2_8_1_1","unstructured":"\u00a0"},{"key":"e_1_2_8_2_2","doi-asserted-by":"publisher","DOI":"10.1126\/science.aav3506"},{"key":"e_1_2_8_3_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.coche.2013.03.005"},{"key":"e_1_2_8_4_2","doi-asserted-by":"publisher","DOI":"10.1039\/C3CS60323G"},{"key":"e_1_2_8_5_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.cattod.2016.02.006"},{"key":"e_1_2_8_6_1","unstructured":"\u00a0"},{"key":"e_1_2_8_7_2","doi-asserted-by":"publisher","DOI":"10.1039\/C1CP22700A"},{"key":"e_1_2_8_8_2","doi-asserted-by":"publisher","DOI":"10.1016\/j.checat.2022.04.012"},{"key":"e_1_2_8_9_2","doi-asserted-by":"publisher","DOI":"10.1021\/cs500522g"},{"key":"e_1_2_8_10_2","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201601282"},{"key":"e_1_2_8_11_2","volume":"28","author":"Fan L.","year":"2018","journal-title":"Adv. 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