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However, this strategy is limited by the instability of single-atom cocatalysts under reaction conditions and the sluggish migration of OL in conventional oxide supports. Here, we report a vacancy-engineered perovskite ferrite (LaFe1\u2013xO3) that simultaneously stabilizes atomic cocatalysts and accelerates OL dynamics for efficient photothermal DRM. Introducing Fe defects generates robust anchoring sites for atomic Ru cocatalysts (Ru1) while weakening the La\u2013O\u2013Fe framework to promote OL mobility. The optimized Ru1\/LaFe1\u2013xO3 catalyst enables light-driven DRM without external heating, achieving high syngas production (H2: 53.6 and CO: 66.1 mol gRu\u20131 h\u20131), a methane turnover frequency of 1.3 s\u20131, and stable operation over 180 h. Mechanistic studies reveal that vacancy-induced electron localization facilitates OL migration, while photoinduced metal-to-metal charge transfer enriches Fe sites with electrons and activates surface OL with holes. This cooperative process selectively oxidizes CH3* to CH3O*, suppressing deep dehydrogenation and coke formation. These findings propose defect engineering as a general strategy to couple atomic cocatalyst stabilization with OL activation for solar-driven catalytic transformations.<\/jats:p>","DOI":"10.1021\/jacs.6c05473","type":"journal-article","created":{"date-parts":[[2026,8,12]],"date-time":"2026-08-12T07:01:45Z","timestamp":1786518105000},"page":"35424-35432","source":"Crossref","is-referenced-by-count":3,"title":["Vacancy-Engineered\nPerovskite Ferrites Stabilize Atomic\nRu Sites and Activate Lattice Oxygen for Photothermal Methane Dry\nReforming"],"prefix":"10.1021","volume":"148","author":[{"given":"Jilong","family":"Li","sequence":"first","affiliation":[{"name":"Fuzhou University , , ,","place":["Fuzhou, P. R. China, 350116"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Ke","family":"Tang","sequence":"additional","affiliation":[{"name":"Fuzhou University , , ,","place":["Fuzhou, P. R. China, 350116"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yueling","family":"Chen","sequence":"additional","affiliation":[{"name":"Fuzhou University , , ,","place":["Fuzhou, P. R. China, 350116"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Bo","family":"Su","sequence":"additional","affiliation":[{"name":"Fuzhou University , , ,","place":["Fuzhou, P. R. China, 350116"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Xiahui","family":"Lin","sequence":"additional","affiliation":[{"name":"Fuzhou University , , ,","place":["Fuzhou, P. R. China, 350108"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2154-2223","authenticated-orcid":true,"given":"Xue Feng","family":"Lu","sequence":"additional","affiliation":[{"name":"Fuzhou University , , ,","place":["Fuzhou, P. R. China, 350116"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Kunlong","family":"Liu","sequence":"additional","affiliation":[{"name":"Fuzhou University , , ,","place":["Fuzhou, P. R. China, 350116"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Masakazu","family":"Anpo","sequence":"additional","affiliation":[{"name":"Fuzhou University , , ,","place":["Fuzhou, P. R. China, 350116"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2656-9169","authenticated-orcid":true,"given":"Sibo","family":"Wang","sequence":"additional","affiliation":[{"name":"Fuzhou University , , ,","place":["Fuzhou, P. R. China, 350116"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,12]]},"reference":[{"key":"2026090104494658900_cit1","doi-asserted-by":"publisher","first-page":"1606","DOI":"10.1016\/j.joule.2019.06.023","article-title":"Solar-Energy-Mediated\nMethane Conversion","volume":"3","author":"Song","year":"2019","journal-title":"Joule"},{"key":"2026090104494658900_cit2","doi-asserted-by":"publisher","first-page":"1030","DOI":"10.1038\/s41929-022-00870-8","article-title":"Enhanced CO2 Utilization\nin Dry Reforming\nof Methane Achieved through Nickel-Mediated Hydrogen Spillover in\nZeolite Crystals","volume":"5","author":"Zhu","year":"2022","journal-title":"Nat. Catal."},{"key":"2026090104494658900_cit3","doi-asserted-by":"publisher","first-page":"3193","DOI":"10.1039\/C8CS00502H","article-title":"New Horizon\nin C1 Chemistry:\nBreaking the Selectivity Limitation in Transformation of Syngas and\nHydrogenation of CO2 into Hydrocarbon Chemicals and Fuels","volume":"48","author":"Zhou","year":"2019","journal-title":"Chem. Soc. Rev."},{"key":"2026090104494658900_cit4","doi-asserted-by":"publisher","first-page":"12890","DOI":"10.1021\/jacs.5c01751","article-title":"Conversion of Syngas to Ethanol over\na RhFe Alloy Catalyst","volume":"147","author":"Zhou","year":"2025","journal-title":"J. Am. Chem. 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Mater."},{"key":"2026090104494658900_cit26","doi-asserted-by":"publisher","first-page":"148","DOI":"10.1038\/s41929-019-0419-z","article-title":"Photocatalytic Uphill\nConversion of Natural Gas Beyond the Limitation of Thermal Reaction\nSystems","volume":"3","author":"Shoji","year":"2020","journal-title":"Nat. Catal."},{"key":"2026090104494658900_cit27","doi-asserted-by":"publisher","first-page":"5208","DOI":"10.1021\/acscatal.6c00807","article-title":"Electron-Deficient\nRu\u03b4+ Sites Coupled with Lattice Oxygen at Ru\/BaTiO3 Interfaces Enable Efficient Photothermal Methane Dry Reforming","volume":"16","author":"Su","year":"2026","journal-title":"ACS Catal."},{"key":"2026090104494658900_cit28","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-026-68429-w","article-title":"Light-Driven Restructuring Generates Nanoisland NiIr Alloy for Efficient\nMethane Dry Reforming","volume":"17","author":"He","year":"2026","journal-title":"Nat. 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Mater."},{"key":"2026090104494658900_cit41","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202504015","article-title":"Dynamic Switching\nSpin State of Fe Single Atoms for Piezoelectric-Mediated Overall Nitrogen\nFixation Photosynthesis","volume":"37","author":"Yuan","year":"2025","journal-title":"Adv. Mater."},{"key":"2026090104494658900_cit42","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202303654","article-title":"Highly Efficient\nSolar-Driven\nDry Reforming of Methane on a Rh\/LaNiO3 Catalyst through\na Light-Induced Metal-to-Metal Charge Transfer Process","volume":"35","author":"Yao","year":"2023","journal-title":"Adv. Mater."},{"key":"2026090104494658900_cit43","doi-asserted-by":"publisher","DOI":"10.1016\/j.apcatb.2023.123054","article-title":"Enhanced Dry Reforming\nof CO2 and CH4 on Photothermal Catalyst Ru\/SrTiO3","volume":"338","author":"Tang","year":"2023","journal-title":"Appl. Catal. 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Soc."},{"key":"2026090104494658900_cit47","doi-asserted-by":"publisher","first-page":"617","DOI":"10.1038\/s41578-022-00422-3","article-title":"Methane Transformation by Photocatalysis","volume":"7","author":"Li","year":"2022","journal-title":"Nat. Rev. Mater."},{"key":"2026090104494658900_cit48","doi-asserted-by":"publisher","first-page":"1400","DOI":"10.1016\/j.scib.2024.02.020","article-title":"Rh\/InGaN1-xOx Nanoarchitecture\nfor Light-Driven Methane\nReforming with Carbon Dioxide toward Syngas","volume":"69","author":"Li","year":"2024","journal-title":"Sci. Bull."},{"key":"2026090104494658900_cit49","doi-asserted-by":"publisher","first-page":"4730","DOI":"10.1021\/acscatal.0c04826","article-title":"Insights into the Nonthermal Effects\nof Light in Dry Reforming of Methane to Enhance the H2\/CO\nRatio near Unity over Ni\/Ga2O3","volume":"11","author":"Rao","year":"2021","journal-title":"ACS Catal."},{"key":"2026090104494658900_cit50","doi-asserted-by":"publisher","first-page":"17566","DOI":"10.1021\/jacs.5c04676","article-title":"Coverage-Dependent\nSelective Conversion of Methane into Value-Added Ethane over Noble-Metal-Free\nNi1-CeO2 Photocatalyst","volume":"147","author":"Luo","year":"2025","journal-title":"J. Am. Chem. Soc."},{"key":"2026090104494658900_cit51","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202404658","article-title":"Best Practices for Experiments and\nReports in Photocatalytic Methane Conversion","volume":"63","author":"Jiang","year":"2024","journal-title":"Angew. Chem., Int. 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