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These emissions not only contribute to carbon footprints but also hinder the upgrading of C<jats:sub>2<\/jats:sub>H<jats:sub>2<\/jats:sub>. Herein, a two\u2010step electrochemical and thermochemical cascade system that directly converts CO\u2082\u2010contaminated crude acetylene into C<jats:sub>6+<\/jats:sub> esters is proposed. In the first step, CO\u2082 from crude acetylene is captured by hydroxide to form bicarbonate, which is subsequently released in situ at the cathode under electrolysis. Using a Ni single\u2010atom catalyst, CO is efficiently generated with a Faradaic efficiency of 97.8 \u00b1 0.84% at 100\u00a0mA\u00a0cm<jats:sup>\u22122<\/jats:sup>. The generated CO then reacts with acetylene in the second step, where a Pd\u2010based catalyst enables the production of dimethyl butenedioate at 7.83 \u00b1 0.31\u00a0mmol\u00a0L<jats:sup>\u22121<\/jats:sup>\u00a0h<jats:sup>\u22121<\/jats:sup> and selective dimethyl maleate synthesis (&gt;65% selectivity). Furthermore, replacing methanol with ethanol or butanol in the carbonylation step allows for tunable synthesis of diethyl or dibutyl butenedioate, demonstrating broad applicability. Techno\u2010economic analysis indicates a 46.9% cost reduction compared to the traditional reverse water\u2010gas shift system, attributed to lower energy demands and eliminated separation steps. This work provides a green strategy for valorizing low\u2010value acetylene streams while mitigating CO\u2082 emissions.<\/jats:p>","DOI":"10.1002\/smll.202504360","type":"journal-article","created":{"date-parts":[[2025,4,28]],"date-time":"2025-04-28T05:51:12Z","timestamp":1745819472000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Electrochemical\u2010Thermochemical Cascade System for the Sustainable Conversion of Crude Acetylene to C<sub>6+<\/sub> Esters"],"prefix":"10.1002","author":[{"given":"Wei","family":"Jiang","sequence":"first","affiliation":[{"name":"Key Laboratory of Precision and Intelligent Chemistry\/School of Chemistry and Materials Science University of Science and Technology of China  Hefei Anhui 230026 China"},{"name":"Deep Space Exploration Laboratory University of Science and Technology of China  Hefei 230026 China"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Dayin","family":"He","sequence":"additional","affiliation":[{"name":"Key Laboratory of Precision and Intelligent Chemistry\/School of Chemistry and Materials Science University of Science and Technology of China  Hefei Anhui 230026 China"},{"name":"Deep Space Exploration Laboratory University of Science and Technology of China  Hefei 230026 China"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Xianhui","family":"Ma","sequence":"additional","affiliation":[{"name":"Key Laboratory of Precision and Intelligent Chemistry\/School of Chemistry and Materials Science University of Science and Technology of China  Hefei Anhui 230026 China"},{"name":"Deep Space Exploration Laboratory University of Science and Technology of China  Hefei 230026 China"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Huang","family":"Zhou","sequence":"additional","affiliation":[{"name":"Key Laboratory of Precision and Intelligent Chemistry\/School of Chemistry and Materials Science University of Science and Technology of China  Hefei Anhui 230026 China"},{"name":"Deep Space Exploration Laboratory University of Science and Technology of China  Hefei 230026 China"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9524-2843","authenticated-orcid":false,"given":"Yuen","family":"Wu","sequence":"additional","affiliation":[{"name":"Key Laboratory of Precision and Intelligent Chemistry\/School of Chemistry and Materials Science University of Science and Technology of China  Hefei Anhui 230026 China"},{"name":"Deep Space Exploration Laboratory University of Science and Technology of China  Hefei 230026 China"}],"role":[{"role":"author","vocabulary":"crossref"}]}],"member":"311","published-online":{"date-parts":[[2025,4,27]]},"reference":[{"key":"e_1_2_8_1_1","doi-asserted-by":"crossref","first-page":"1761","DOI":"10.1021\/cr400357r","volume":"114","author":"Trotu\u015f I.\u2010T.","year":"2013","journal-title":"Chem. 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