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This study introduces a novel electrofermentation (EF) platform integrating polycarbazole\u2010based porous organic polymer (\n                    <jats:bold>VJ\u2010POP<\/jats:bold>\n                    )\u2010coated electrodes to enhance selective acetic acid (AA) biosynthesis by\n                    <jats:italic>Bacillus subtilis<\/jats:italic>\n                    . Impressive high surface area and tailored porosity facilitate efficient CO\u2082 capture, modulate intracellular metabolic fluxes, and improve electron transfer, thereby driving product specificity. In the bioreactor equipped with\n                    <jats:bold>VJ\u2010POP<\/jats:bold>\n                    , AA production reached 2.11\u00a0g L\n                    <jats:sup>\u22121<\/jats:sup>\n                    with a yield of 0.48\u00a0g g\n                    <jats:sup>\u22121<\/jats:sup>\n                    , achieving 71% of the theoretical maximum without genetic modifications. The process also resulted in enriched biohydrogen content (52%) in the biogas (H\n                    <jats:sub>2\u00a0<\/jats:sub>\n                    +\u00a0CO\n                    <jats:sub>2<\/jats:sub>\n                    ) composition, highlighting the synergistic effect of\n                    <jats:bold>VJ\u2010POP<\/jats:bold>\n                    on CO\u2082 sequestration and microbial metabolism. Gene expression analysis revealed significant upregulation of\n                    <jats:italic>ackA<\/jats:italic>\n                    (acetate kinase) and\n                    <jats:italic>pdhA<\/jats:italic>\n                    (pyruvate dehydrogenase), while\n                    <jats:italic>buk<\/jats:italic>\n                    (butyrate kinase) was downregulated, ensuring metabolic selectivity toward AA. Cyclic voltammetry and impedance analysis unambiguously confirmed an interesting phenomenon of enhanced electron transfer and reduced charge\u2010transfer resistance in\n                    <jats:bold>VJ\u2010POP\u2010<\/jats:bold>\n                    assisted systems. Computational analysis using density functional theory (DFT) revealed stronger binding energy for CO\n                    <jats:sub>2<\/jats:sub>\n                    (\u221217.4\u00a0kJ mol\n                    <jats:sup>\u22121<\/jats:sup>\n                    ) compared to H\n                    <jats:sub>2<\/jats:sub>\n                    (\u22122.5\u00a0kJ mol\n                    <jats:sup>\u22121<\/jats:sup>\n                    ), driven by a mix of van der Waals and weak electrostatic interactions for CO\n                    <jats:sub>2<\/jats:sub>\n                    versus solely weak van der Waals\u2010based physisorption for H\n                    <jats:sub>2<\/jats:sub>\n                    . This pioneering approach with unique investigation results presents a scalable and sustainable biocatalytic framework for CO\u2082 valorization, bridging material science and microbial electrochemical systems for selective AA and enhanced biohydrogen production.\n                  <\/jats:p>","DOI":"10.1002\/anie.202508070","type":"journal-article","created":{"date-parts":[[2025,6,3]],"date-time":"2025-06-03T03:53:18Z","timestamp":1748922798000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":6,"title":["Intracellular CO\n                    <sub>2<\/sub>\n                    Capture Triggered Outperforming Biocatalytic Production of Selective Acetic Acid and Biohydrogen Housing in Porous\u2010Organic\u2010Nanofiber"],"prefix":"10.1002","volume":"64","author":[{"given":"Nitumani","family":"Das","sequence":"first","affiliation":[{"name":"Department of Catalysis &amp; Fine Chemicals CSIR\u2010Indian Institute of Chemical Technology (CSIR\u2010IICT)  Uppal Road Hyderabad 500007 India"},{"name":"Academy of Scientific and Innovative Research (AcSIR)  Ghaziabad 201002 India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Triya","family":"Mukherjee","sequence":"additional","affiliation":[{"name":"Bioengineering and Environmental Sciences Lab Department of Energy and Environmental Engineering CSIR\u2010Indian Institute of Chemical Technology (CSIR\u2010IICT)  Hyderabad 500007 India"},{"name":"Academy of Scientific and Innovative Research (AcSIR)  Ghaziabad 201002 India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Chitra","family":"Sarkar","sequence":"additional","affiliation":[{"name":"Department of Catalysis &amp; Fine Chemicals CSIR\u2010Indian Institute of Chemical Technology (CSIR\u2010IICT)  Uppal Road Hyderabad 500007 India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ratul","family":"Paul","sequence":"additional","affiliation":[{"name":"Department of Catalysis &amp; Fine Chemicals CSIR\u2010Indian Institute of Chemical Technology (CSIR\u2010IICT)  Uppal Road Hyderabad 500007 India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Duy Quang","family":"Dao","sequence":"additional","affiliation":[{"name":"Institute of Research and Development Duy Tan University  Da Nang 550000 Vietnam"},{"name":"School of Engineering and Technology Duy Tan University  Da Nang 550000 Vietnam"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"S. Venkata","family":"Mohan","sequence":"additional","affiliation":[{"name":"Bioengineering and Environmental Sciences Lab Department of Energy and Environmental Engineering CSIR\u2010Indian Institute of Chemical Technology (CSIR\u2010IICT)  Hyderabad 500007 India"},{"name":"Academy of Scientific and Innovative Research (AcSIR)  Ghaziabad 201002 India"},{"name":"CSIR\u2010National Environmental Engineering Research Institute (CSIR\u2010NEERI)  Nagpur 440020 India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7813-2108","authenticated-orcid":false,"given":"John","family":"Mondal","sequence":"additional","affiliation":[{"name":"Department of Catalysis &amp; Fine Chemicals CSIR\u2010Indian Institute of Chemical Technology (CSIR\u2010IICT)  Uppal Road Hyderabad 500007 India"},{"name":"Academy of Scientific and Innovative Research (AcSIR)  Ghaziabad 201002 India"},{"name":"Organic &amp; Medicinal Chemistry Division CSIR\u2010Indian Institute of Chemical Biology (CSIR\u2010IICB)  4\u2010Raja S. 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