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Alkaline hydrothermal vents (AHVs) may have facilitated energy transfer and carbon fixation at life\u2019s emergence. Specifically, pH separation across vent walls could have been the forerunner to pH separation across cell membranes, with inorganic barriers containing [Ni-]FeS minerals as precursors of metalloenzymes in potentially ancient biological reductive acetyl-CoA Wood\u2013Ljungdahl (WL) and other metabolic pathways. We previously demonstrated pH-gradient-dependent reduction of CO2 to formate by H2 in AHV interface conditions. Here, we address the same problem of CO2 reduction using a macroscale reactor with minerals synthesized via protocols meant to mimic the natural processes of hydrothermal chimney formation. This reactor also allowed us to probe more variables and explore longer experimentation time frames. These results elucidate how different aspects of the hydrothermal\u2013vent interface (e.g., different minerals and\/or temperature gradients) affect the observed CO2 electrochemical reduction as well as the flow of electrons under passive vs induced currents and potentials. Using experimental simulations and electrochemistry techniques, we detected two key steps of the WL pathway (CO2 to formic acid and the formation of acetic acid). We explored effects of Ni incorporation in the mineral catalyst, as well as temperature and the effects of these variables on the production of formate. Currents as small as 10 nanoamps to 10 microamps were enough to efficiently carry out CO2 reduction. In this work, we electrochemically explore energy protometabolism in vent\u2013ocean interfaces, specifically focusing on [Ni-]FeS minerals as precursors of metalloenzymes.<\/jats:p>","DOI":"10.1021\/jacs.5c01948","type":"journal-article","created":{"date-parts":[[2025,7,29]],"date-time":"2025-07-29T23:39:06Z","timestamp":1753832346000},"page":"28674-28683","source":"Crossref","is-referenced-by-count":4,"title":["Carbon Reduction Powered\nby Natural Electrochemical\nGradients under Submarine Hydrothermal Vent Conditions"],"prefix":"10.1021","volume":"147","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-1501-7687","authenticated-orcid":true,"given":"T.","family":"Altair","sequence":"first","affiliation":[{"name":"College of the Atlantic , ,","place":["Bar Harbor, Maine, United States, 04609"]},{"name":"University of Sao Paulo , ,","place":["Sao Carlos, Brazil, 13560-970"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0002-7889-0202","authenticated-orcid":true,"given":"E.","family":"Dragoti","sequence":"additional","affiliation":[{"name":"College of the Atlantic , ,","place":["Bar Harbor, Maine, United States, 04609"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"V.","family":"Sojo","sequence":"additional","affiliation":[{"name":"American Museum of Natural History , , , ,","place":["New York, New York, United States, 10024"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5411-0211","authenticated-orcid":true,"given":"Y.","family":"Li","sequence":"additional","affiliation":[{"name":"Institute of Science Tokyo , , ,","place":["Tokyo, Japan, 152-0033"]},{"name":"Center for Sustainable Resource Science RIKEN ,","place":["Wako, Japan, 351-0198"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"S.","family":"Skiffington","sequence":"additional","affiliation":[{"name":"Colby College , , , ,","place":["Waterville, Maine, United States, 04901"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"W.A.","family":"Sullivan","sequence":"additional","affiliation":[{"name":"Colby College , , , ,","place":["Waterville, Maine, United States, 04901"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-9195-6360","authenticated-orcid":true,"given":"G.T.","family":"Drozd","sequence":"additional","affiliation":[{"name":"Colby College , , , ,","place":["Waterville, Maine, United States, 04901"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-8199-7011","authenticated-orcid":true,"given":"S.E.","family":"McGlynn","sequence":"additional","affiliation":[{"name":"Institute of Science Tokyo , , ,","place":["Tokyo, Japan, 152-0033"]},{"name":"Center for Sustainable Resource Science RIKEN ,","place":["Wako, Japan, 351-0198"]},{"name":"Blue Marble Space Institute of Science , , ,","place":["Seattle, Washington, United States, 98104"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"D.","family":"Galante","sequence":"additional","affiliation":[{"name":"University of Sao Paulo , , ,","place":["Sao Paulo, Brazil, 05508-080"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6237-6068","authenticated-orcid":true,"given":"H.","family":"Varela","sequence":"additional","affiliation":[{"name":"University of Sao Paulo , ,","place":["Sao Carlos, Brazil, 13560-970"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"R.","family":"Hudson","sequence":"additional","affiliation":[{"name":"College of the Atlantic , ,","place":["Bar Harbor, Maine, United States, 04609"]},{"name":"Colby College , , , ,","place":["Waterville, Maine, United States, 04901"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2025,7,29]]},"reference":[{"issue":"3","key":"2026093015073253200_cit1","doi-asserted-by":"publisher","first-page":"231","DOI":"10.1007\/BF00160147","article-title":"A Hydrothermally\nPrecipitated Catalytic Iron Sulphide Membrane as a First Step toward\nLife","volume":"39","author":"Russell","year":"1994","journal-title":"J. Mol. Evol."},{"issue":"8","key":"2026093015073253200_cit2","doi-asserted-by":"publisher","first-page":"777","DOI":"10.3390\/life11080777","article-title":"Experimental Approaches\nfor Testing the Hypothesis of the Emergence of Life at Submarine Alkaline\nVents","volume":"11","author":"Altair","year":"2021","journal-title":"Life"},{"issue":"2","key":"2026093015073253200_cit3","doi-asserted-by":"publisher","first-page":"181","DOI":"10.1089\/ast.2015.1406","article-title":"The Origin of Life in Alkaline Hydrothermal Vents","volume":"16","author":"Sojo","year":"2016","journal-title":"Astrobiology"},{"issue":"4","key":"2026093015073253200_cit4","doi-asserted-by":"publisher","first-page":"271","DOI":"10.1002\/bies.200900131","article-title":"How Did LUCA Make a Living? 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Acta, Bioenerg."},{"issue":"3","key":"2026093015073253200_cit15","doi-asserted-by":"publisher","first-page":"35","DOI":"10.3390\/life8030035","article-title":"Green Rust:\nThe Simple Organizing \u2018Seed\u2019 of All Life?","volume":"8","author":"Russell","year":"2018","journal-title":"Life"},{"issue":"5714","key":"2026093015073253200_cit16","doi-asserted-by":"publisher","first-page":"1428","DOI":"10.1126\/science.1102556","article-title":"A Serpentinite-Hosted Ecosystem:\nThe Lost City Hydrothermal Field","volume":"307","author":"Kelley","year":"2005","journal-title":"Science"},{"issue":"1622","key":"2026093015073253200_cit17","doi-asserted-by":"publisher","first-page":"20120258","DOI":"10.1098\/rstb.2012.0258","article-title":"Beating the Acetyl Coenzyme A-Pathway to the Origin\nof Life","volume":"368","author":"Nitschke","year":"2013","journal-title":"Philos. Trans. R. Soc., B"},{"key":"2026093015073253200_cit18","doi-asserted-by":"publisher","first-page":"817","DOI":"10.3389\/fmicb.2020.00817","article-title":"Older Than\nGenes: The Acetyl CoA Pathway and Origins","volume":"11","author":"Martin","year":"2020","journal-title":"Front.\nMicrobiol"},{"issue":"35","key":"2026093015073253200_cit19","doi-asserted-by":"publisher","first-page":"7501","DOI":"10.1039\/C5CC02078F","article-title":"Bio-Inspired CO2 Conversion\nby Iron Sulfide Catalysts under Sustainable Conditions","volume":"51","author":"Roldan","year":"2015","journal-title":"Chem. Commun."},{"issue":"22","key":"2026093015073253200_cit20","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202218189","article-title":"Influence\nof Composition\nof Nickel-Iron Nanoparticles for Abiotic CO2 Conversion\nto Early Prebiotic Organics","volume":"62","author":"Beyazay","year":"2023","journal-title":"Angew. Chem. 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