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However, photocatalytic N2 reduction (PNR) remains constrained by the high energy barrier for N2 activation and reduction. In this work, we report that the spin-polarized chiral mesostructured Bi2WO6 (CMB) can facilitate the formation of metastable triplet NOH (3NOH) intermediates, while simultaneously promoting the separation and transport of photogenerated charge carriers, thereby enhancing PNR performance. The CMB was fabricated via a hydrothermal method using tartaric acid as a symmetry-breaking agent. Under sacrificial-agent-free conditions, the NH3 yield of 1325.5 \u03bcmol gcat\u20131 h\u20131 was achieved, representing a 4.7-fold enhancement over the best values reported for Bi- and W-based catalysts. The pronounced accumulation of the *NOH intermediate, a key precursor to NH3, is speculated to originate from the 3NOH intermediate, driven by the spin polarization of CMB. This work reveals the critical role of spin polarization in regulating triplet reaction intermediates and charge-carrier dynamics during N2 reduction, providing an effective strategy for the design of advanced photocatalysts for sustainable NH3 synthesis.<\/jats:p>","DOI":"10.1021\/jacs.6c13135","type":"journal-article","created":{"date-parts":[[2026,10,12]],"date-time":"2026-10-12T16:36:36Z","timestamp":1791822996000},"page":"44567-44574","source":"Crossref","is-referenced-by-count":0,"title":["Spin\nPolarization Enhanced Photocatalytic N2 Reduction on Chiral\nMesostructured Bi2WO6"],"prefix":"10.1021","volume":"148","author":[{"given":"Jiamin","family":"Ma","sequence":"first","affiliation":[{"name":"Shanghai Jiao Tong University , , 800 Dongchuan Road , ,","place":["Shanghai, China, 200240"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Wanning","family":"Zhang","sequence":"additional","affiliation":[{"name":"Shanghai Jiao Tong University , , 800 Dongchuan Road , ,","place":["Shanghai, China, 200240"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6119-4895","authenticated-orcid":true,"given":"Lu","family":"Han","sequence":"additional","affiliation":[{"name":"Tongji University , , 1239 Siping Road , ,","place":["Shanghai, China, 200092"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7831-1552","authenticated-orcid":true,"given":"Shunai","family":"Che","sequence":"additional","affiliation":[{"name":"Shanghai Jiao Tong University , , 800 Dongchuan Road , ,","place":["Shanghai, China, 200240"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0009-0000-5019-1413","authenticated-orcid":true,"given":"Yuxi","family":"Fang","sequence":"additional","affiliation":[{"name":"Shanghai Jiao Tong University , , 800 Dongchuan Road , ,","place":["Shanghai, China, 200240"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,10,12]]},"reference":[{"key":"2026102111094894600_cit1","doi-asserted-by":"publisher","first-page":"1357","DOI":"10.1126\/science.adn0558","article-title":"Spin-mediated promotion of Co catalysts\nfor ammonia synthesis","volume":"383","author":"Zhang","year":"2024","journal-title":"Science"},{"key":"2026102111094894600_cit2","doi-asserted-by":"publisher","first-page":"612","DOI":"10.1038\/s44160-023-00321-7","article-title":"Prospects and\nchallenges of green ammonia synthesis","volume":"2","author":"Ye","year":"2023","journal-title":"Nat.\nSynth."},{"key":"2026102111094894600_cit3","doi-asserted-by":"publisher","first-page":"286","DOI":"10.1038\/s41557-022-01088-8","article-title":"Photocatalytic nitrogen\nfixation under an ambient atmosphere using a porous coordination polymer\nwith bridging dinitrogen anions","volume":"15","author":"Xiong","year":"2023","journal-title":"Nat. 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