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Herein, we report a direct electron transfer (DET)-type gas diffusion electrode (GDE) utilizing formate dehydrogenase 1 (FoDH1) from Methylorubrum extorquens AM1 for efficient CO2-to-formate conversion across a broad range of low CO2 levels. The electrode surface was modified with pyrene derivatives using multiwalled carbon nanotubes (MWCNTs) to tailor the enzyme\u2013electrode interface, enabling favorable enzyme orientation for rapid electron transfer. A 1-pyrenemethylamine (PyNH2)-modified GDE with FoDH1 exhibited a current density of \u22121.2 mA cm\u20132 at a reduction potential of \u22120.9 V, which was twice that of the pristine electrode, and generated formate with a Faradaic efficiency of 82 \u00b1 5%, outperforming previously reported GDE systems. Kinetic analyses under controlled CO2 conditions (0.04\u2013100%) revealed a notably low apparent Michaelis constant (KM,app) of 2.6 \u00b1 0.3%, which is less than one-third of that of the solution system, indicating high CO2 affinity. This enhancement is attributed to the direct supply of gaseous CO2 to the catalytic layer, avoiding equilibrium limitations in the electrolyte solution. These results lead to a promising tool for enzymatic CO2 reduction using emission gases from industrial sources and provide key design principles for practical CO2-recycling technologies.<\/jats:p>","DOI":"10.1021\/acsomega.6c02909","type":"journal-article","created":{"date-parts":[[2026,8,4]],"date-time":"2026-08-04T14:34:43Z","timestamp":1785854083000},"page":"47701-47710","source":"Crossref","is-referenced-by-count":2,"title":["Direct Electron Transfer-Type Gas Diffusion Electrode\nfor Efficient CO2-to-Formate Bioconversion across\nBroad and Low CO2 Levels"],"prefix":"10.1021","volume":"11","author":[{"given":"Ami","family":"Kobayashi","sequence":"first","affiliation":[{"name":"Kyoto University , , Sakyo, ,","place":["Kyoto, Japan, 606-8502"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3863-993X","authenticated-orcid":true,"given":"Taiki","family":"Adachi","sequence":"additional","affiliation":[{"name":"Kyoto University , , Sakyo, ,","place":["Kyoto, Japan, 606-8502"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Konatsu","family":"Ichikawa","sequence":"additional","affiliation":[{"name":"Kyoto University , , Sakyo, ,","place":["Kyoto, Japan, 606-8502"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuki","family":"Kitazumi","sequence":"additional","affiliation":[{"name":"Kyoto University , , Sakyo, ,","place":["Kyoto, Japan, 606-8502"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Osamu","family":"Shirai","sequence":"additional","affiliation":[{"name":"Kyoto University , , Sakyo, ,","place":["Kyoto, Japan, 606-8502"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9767-4922","authenticated-orcid":true,"given":"Keisei","family":"Sowa","sequence":"additional","affiliation":[{"name":"Kyoto University , , Sakyo, ,","place":["Kyoto, Japan, 606-8502"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,3]]},"reference":[{"key":"2026081810492447200_cit1","unstructured":"Lindsey, R.\n          \n          Climate Change: Atmospheric\nCarbon Dioxide; NOAA Climate.gov2025, accessed Nov 19, 2025. https:\/\/www.climate.gov\/news-features\/understanding-climate\/climate-change-atmospheric-carbon-dioxide."},{"key":"2026081810492447200_cit2","unstructured":"National Oceanic and Atmospheric Administration.\n          .  During a Year of Extremes,\nCarbon Dioxide Levels Surge Faster Than Ever; National Oceanic and Atmospheric Administration2024, accessed Nov 19, 2025. https:\/\/www.noaa.gov\/news-release\/during-year-of-extremes-carbon-dioxide-levels-surge-faster-than-ever."},{"key":"2026081810492447200_cit3","unstructured":"Ritchie, H.; Rosado, P.; Roser, M.\n          CO2 and Greenhouse Gas\nEmissions; Our World in Data, 2023, accessed Nov 19, 2025. https:\/\/ourworldindata.org\/co2-and-greenhouse-gas-emissions."},{"key":"2026081810492447200_cit4","doi-asserted-by":"publisher","first-page":"143203","DOI":"10.1016\/j.scitotenv.2020.143203","article-title":"Progress\nin Carbon Capture Technologies","volume":"761","author":"Wilberforce","year":"2021","journal-title":"Sci. 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