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Replicating such an elegant blueprint, or its function and mechanism within artificial systems, remains challenging. This study demonstrates a photoinduced PCET process in a pyrene-based zirconium-oxo metal\u2013organic framework (MOF) NU-1000, operating in the singlet manifold, directly producing an NADH model analogue (HNH-H) along with a 2[pyrene\u2022+]\u2500[Zr-oxo node-O\u2013] pair, without any cocatalysts. Spectroscopic analyses\u2500including steady-state, time-resolved, and transient methods\u2500reveal that in a stepwise two 1e\u2013 reduction process, the proton transfer from node-bound hydroxyl and aqua ligands in polar dimethylformamide solvent is not directly involved in the rate-defining step, evidenced by a kinetic isotope effect (KIE) of 1 at a very low [HNH+]. However, with increasing difficulty in the successive deprotonation from the anionic node, an inverse KIE (0.75) was observed at higher [HNH+]. Density functional theory-based computation supports a pre-equilibrium proton transfer to the first 1e\u2013 reduced radical intermediate HNH\u2022, followed by the second electron transfer, consistent with an overall ET\u2013PTET mechanism for this endoergic process. In nonpolar solvents that do not support proton transfer, the HNH\u2022 intermediate instead undergoes irreversible dimerization. The reduced HNH-H shuttle was exploited in the photocatalytic multielectron PCET-based reduction of maleate to succinate, achieving \u223c30% consumption of maleate and \u223c12% conversion to succinate in aprotic media without any external hole scavengers and proton source, relying solely on node-bound protons in NU-1000. Under these conditions, the benchmark photocatalyst Ru(bpy)32+ was ineffective. Introduction of ethanol as a regenerator establishes a fully catalytic, recyclable system with NU-1000. These results highlight the potential of Zr-oxo MOFs as platforms for entirely artificial, bioinspired photosystem I analogues.<\/jats:p>","DOI":"10.1021\/jacs.6c02964","type":"journal-article","created":{"date-parts":[[2026,7,21]],"date-time":"2026-07-21T18:58:29Z","timestamp":1784660309000},"page":"31783-31793","source":"Crossref","is-referenced-by-count":0,"title":["Heterogeneous\nArtificial Photosystem I: Photoinduced\nProton-Coupled Electron Transfer in Zr\u2013Metal\u2013Organic\nFrameworks"],"prefix":"10.1021","volume":"148","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-8138-3618","authenticated-orcid":true,"given":"Bapan","family":"Saha","sequence":"first","affiliation":[{"name":"Southern Illinois University , , 1245 Lincoln Drive , , ,","place":["Carbondale, Illinois, United States, 62901"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Sreehari Surendran","family":"Rajasree","sequence":"additional","affiliation":[{"name":"Southern Illinois University , , 1245 Lincoln Drive , , ,","place":["Carbondale, Illinois, United States, 62901"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Prachi","family":"Dilwalia","sequence":"additional","affiliation":[{"name":"Southern Illinois University , , 1245 Lincoln Drive , , ,","place":["Carbondale, Illinois, United States, 62901"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Emma N.","family":"Phillips","sequence":"additional","affiliation":[{"name":"Southern Illinois University , , 1245 Lincoln Drive , , ,","place":["Carbondale, Illinois, United States, 62901"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-2674-1379","authenticated-orcid":true,"given":"David J.","family":"Gosztola","sequence":"additional","affiliation":[{"name":"Argonne National Laboratory , , 9700 S Cass Ave , , ,","place":["Lemont, Illinois, United States, 60439"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8343-5189","authenticated-orcid":true,"given":"H. Christopher","family":"Fry","sequence":"additional","affiliation":[{"name":"Argonne National Laboratory , , 9700 S Cass Ave , , ,","place":["Lemont, Illinois, United States, 60439"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Debmalya","family":"Ray","sequence":"additional","affiliation":[{"name":"Monmouth University , , West Long Branch , , ,","place":["New Jersey, New Jersey, United States, 07764"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-7998-4492","authenticated-orcid":true,"given":"Pravas","family":"Deria","sequence":"additional","affiliation":[{"name":"Southern Illinois University , , 1245 Lincoln Drive , , ,","place":["Carbondale, Illinois, United States, 62901"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,7,21]]},"reference":[{"key":"2026080511132644700_cit1","doi-asserted-by":"publisher","first-page":"763","DOI":"10.1038\/nchem.1145","article-title":"Lessons\nfrom Nature about Solar Light Harvesting","volume":"3","author":"Scholes","year":"2011","journal-title":"Nat.\nChem."},{"key":"2026080511132644700_cit2","doi-asserted-by":"publisher","first-page":"3293","DOI":"10.1103\/PhysRevE.59.3293","article-title":"Energy transfer\nbetween carotenoids\nand bacteriochlorophylls in light-harvesting complex II of purple\nbacteria","volume":"59","author":"Damjanovic\u0301","year":"1999","journal-title":"Phys. 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