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Here, we report an interface-engineered inorganic\u2013biological biohybrid, constructed by covalently anchoring iron single-atom catalysts (ISA) onto\n                    <jats:italic>Cupriavidus necator<\/jats:italic>\n                    (\n                    <jats:italic>C.N<\/jats:italic>\n                    @ISA) via click chemistry. The ISA anchored interface generates a localized H\n                    <jats:sub>2<\/jats:sub>\n                    -rich microenvironment, accelerates H\n                    <jats:sub>2<\/jats:sub>\n                    dissociation, while the synergy between ISA and polyethylene glycol-phenylboronate linker stabilizes the inorganic-biological hybrid interface and promotes electron\/proton transfer across microbial membrane. These coupled effects boost reduced form of nicotinamide adenine dinucleotide (NADH) regeneration and adenosine triphosphate (ATP) synthesis. In addition, ISA exhibits nanozyme-like activity, scavenging reactive oxygen species to protect cell viability. As a result,\n                    <jats:italic>C.N<\/jats:italic>\n                    @ISA achieves CO\n                    <jats:sub>2<\/jats:sub>\n                    -to-bioplastic poly-\n                    <jats:italic>\u03b2<\/jats:italic>\n                    -hydroxybutyrate production of 1058.8\u2009mg\u2009L\n                    <jats:sup>\u22121<\/jats:sup>\n                    with a Faradaic efficiency of 42.0%. Integrating theoretical calculations, electrochemical analysis, and transcriptomics confirms that ISA simultaneously enriches and activates H\n                    <jats:sub>2<\/jats:sub>\n                    while reinforcing intracellular metabolism, offering a generalizable strategy for carbon-negative biomanufacturing.\n                  <\/jats:p>","DOI":"10.1038\/s41467-026-76902-9","type":"journal-article","created":{"date-parts":[[2026,8,20]],"date-time":"2026-08-20T11:05:08Z","timestamp":1787223908000},"update-policy":"https:\/\/doi.org\/10.1007\/springer_crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Interface-engineered iron single-atom biohybrids for efficient CO2-to-bioplastic conversion"],"prefix":"10.1038","volume":"17","author":[{"given":"Sulin","family":"Ni","sequence":"first","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0007-7315-2039","authenticated-orcid":false,"given":"Dong","family":"Xia","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Can","family":"Chen","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Cheng","family":"Qiu","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Youzhi","family":"Li","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5136-9743","authenticated-orcid":false,"given":"Bin","family":"Yang","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9795-8503","authenticated-orcid":false,"given":"Yang","family":"Hou","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4471-5898","authenticated-orcid":false,"given":"Lecheng","family":"Lei","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7990-2856","authenticated-orcid":false,"given":"Zhengwei","family":"Mao","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-3685-381X","authenticated-orcid":false,"given":"Zhongjian","family":"Li","sequence":"additional","affiliation":[],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"297","published-online":{"date-parts":[[2026,8,20]]},"reference":[{"key":"76902_CR1","doi-asserted-by":"publisher","first-page":"9857","DOI":"10.1021\/jacs.3c02428","volume":"145","author":"JQ Feng","year":"2023","unstructured":"Feng, J. 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