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The challenge exists in the key *CO intermediate adsorption behavior, in which the typically top-bonded *CO favors CO release, resulting in dominant syngas (CO and H2) products. Herein, we demonstrate an intermediate adsorption tuning strategy via a Zn\u2013P\u2013Cd coordinated photocatalyst (denoted as P\u2013Cd4ZnS5), in which the diffuse 3p orbital of the coordinated P site enables close P\u2013O overlap with the oxygen end of *CO, thus leading to a parallel *CO configuration by simultaneously forming P\u2013O and Zn\u2013C bonds. Moreover, the stabilized parallel-type *CO subsequently undergoes hydrogenation at adjacent Cd sites to yield *CHO intermediates toward the CH4 reaction pathway. As a result, the optimized P\u2013Cd4ZnS5 achieves an efficient CO2-to-CH4 conversion under ambient light irradiation at 120 mW cm\u20132, including a high selectivity of \u223c93.8%, a CH4 production rate of \u223c366 \u03bcmol g\u20131 h\u20131, and a sustained stability of &amp;gt;120 h, substantially exceeding most of the previous reports. Our work proposes an attractive strategy to tune parallel-type *CO adsorption for steering photocatalytic CO2 reduction toward deep-reduction products with high efficiency, selectivity, and stability.<\/jats:p>","DOI":"10.1021\/acsnano.6c11178","type":"journal-article","created":{"date-parts":[[2026,8,10]],"date-time":"2026-08-10T22:02:13Z","timestamp":1786399333000},"page":"23544-23551","source":"Crossref","is-referenced-by-count":0,"title":["Parallel-Type *CO\nAdsorption Tuning Steers Efficient\nPhotocatalytic CO2 Methanation"],"prefix":"10.1021","volume":"20","author":[{"ORCID":"https:\/\/orcid.org\/0000-0001-9693-1667","authenticated-orcid":true,"given":"Quan","family":"Zhang","sequence":"first","affiliation":[{"name":"Jiangsu University , , ,","place":["Zhenjiang, China, 212013"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Haozhen","family":"Wang","sequence":"additional","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 200438"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yuan","family":"Zhang","sequence":"additional","affiliation":[{"name":"Jiangsu University , , ,","place":["Zhenjiang, China, 212013"]},{"name":"Suzhou Laboratory , ,","place":["Suzhou, China, 215000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Hui","family":"Xu","sequence":"additional","affiliation":[{"name":"Jiangsu University , , ,","place":["Zhenjiang, China, 212013"]},{"name":"Suzhou Laboratory , ,","place":["Suzhou, China, 215000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-1803-6955","authenticated-orcid":true,"given":"Gengfeng","family":"Zheng","sequence":"additional","affiliation":[{"name":"Fudan University , , ,","place":["Shanghai, China, 200438"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,10]]},"reference":[{"key":"2026083119004197600_cit1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-025-55891-1","article-title":"In-situ Restructuring of Ni-Based\nMetal Organic Frameworks for Photocatalytic CO2 Hydrogenation","volume":"16","author":"Gouda","year":"2025","journal-title":"Nat. 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