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Here, we report a catalyst design integrating an ultrathin Turing\u2010type nanonet with a Pd\u2010based crystalline\/amorphous (C\/A) heterointerface, achieving a near\u2010complete C1\u2010pathway selectivity of 97.1% for alkaline EOR, which is the highest reported to date. Inspired by spatially decoupling C\u2500C cleavage and CO oxidation, we engineer two intimately integrated phases: strained interstitial\u2010carbon\u2010doped PdO (C\n                    <jats:sub>int<\/jats:sub>\n                    \u2010PdO) enriched with oxygen vacancies and defective amorphous PdC\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    (a\u2010PdC\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    ). This heterostructure is realized via a \u201ccarbon engineering\u201d strategy combining salt\u2010melt templating with secondary annealing. Atomic\u2010resolution studies confirm atomically sharp C\/A interfaces and the highly unsaturated a\u2010PdC\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    phase. In situ Fourier\u2010transform infrared spectroscopy (FTIR) directly visualizes CO\n                    <jats:sub>2<\/jats:sub>\n                    emergence at ultralow overpotentials, while high\u2010performance liquid chromatography (HPLC) verifies the near\u2010complete C1 pathway. Density functional theory (DFT) reveals a dual\u2010cooperative mechanism: C\n                    <jats:sub>int<\/jats:sub>\n                    \u2010PdO steers the EOR toward C1 pathway by facilitating CH\n                    <jats:sub>3<\/jats:sub>\n                    CO* dehydrogenation and subsequent C\u2500C cleavage via CH\n                    <jats:sub>2<\/jats:sub>\n                    CO*, thereby suppressing acetate formation; concurrently, a\u2010PdC\n                    <jats:italic>\n                      <jats:sub>x<\/jats:sub>\n                    <\/jats:italic>\n                    dramatically accelerates CO oxidation and may also contribute to C\u2500C cleavage via an alternative direct CH\n                    <jats:sub>3<\/jats:sub>\n                    CO* pathway. This work establishes carbon\u2010engineered C\/A heterointerfaces as a powerful platform for overcoming the EOR selectivity bottleneck.\n                  <\/jats:p>","DOI":"10.1002\/adma.74323","type":"journal-article","created":{"date-parts":[[2026,7,24]],"date-time":"2026-07-24T12:10:08Z","timestamp":1784895008000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Near\u2010100% C1\u2010Pathway Selective Ethanol Oxidation on Turing\u2010Type Pd\u2010Based Crystalline\/Amorphous Heterointerfaces"],"prefix":"10.1002","volume":"38","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-9262-5213","authenticated-orcid":false,"given":"Genlei","family":"Zhang","sequence":"first","affiliation":[{"name":"Anhui Province Key Laboratory of Value\u2010Added Catalytic Conversion and Reaction Engineering School of Chemistry and Chemical Engineering Hefei University of Technology  Hefei P. R. 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