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However, the development of donor and\/or acceptor engineering approaches that can simultaneously optimize the charge and energy transfer processes for abundant generation of O2\u2022\u2013 and 1O2 is a major challenge. Herein, a series of porphyrin (electron donor)- and naphthalene diimide (NDI, electron acceptor)-based isostructural mixed-ligand donor\u2013acceptor MOFs were designed and synthesized. Experiments and theoretical calculations revealed that by delicately tuning the electron-pushing capacity of the organic conjugated groups on the donor porphyrin units, the charge transfer kinetics from the donors to the acceptors as well as the energy transfer gifted by the donor porphyrins related to their singlet\u2013triplet energy gaps could be simultaneously optimized. As a result, Zr-NDI-H2DPBP(Pyr), wherein the porphyrin donor ligand with pyrene (Pyr) groups possesses the strongest electron-pushing capacity, exhibited the highest O2\u2022\u2013 and 1O2 generation activities, which can be utilized for efficient aerobic oxidation reactions, including dipolar [3 + 2] cycloaddition and the synthesis of quinoxaline derivatives. This work exemplifies a dual-function donor engineering approach for developing heterogeneous catalysts toward advanced artificial photosynthesis.<\/jats:p>","DOI":"10.1021\/acsami.6c13030","type":"journal-article","created":{"date-parts":[[2026,9,7]],"date-time":"2026-09-07T21:01:42Z","timestamp":1788814902000},"page":"49198-49212","source":"Crossref","is-referenced-by-count":0,"title":["Dual-Function Donor Engineering of a Metal\u2013Organic Framework for Efficient Photocatalytic Oxidative Synthesis"],"prefix":"10.1021","volume":"18","author":[{"given":"Peng-Cheng","family":"Zhao","sequence":"first","affiliation":[{"name":"Changsha University of Science & Technology , , ,","place":["Changsha, China, 410114"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Tian-Yuan","family":"Yang","sequence":"additional","affiliation":[{"name":"Changsha University of Science & Technology , , ,","place":["Changsha, China, 410114"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3109-3839","authenticated-orcid":true,"given":"Huapeng","family":"Sun","sequence":"additional","affiliation":[{"name":"Chenzhou Vocational Technical College , , , ,","place":["Chenzhou, Hunan, China, 423000"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yong-Tao","family":"Liu","sequence":"additional","affiliation":[{"name":"Changsha University of Science & Technology , , ,","place":["Changsha, China, 410114"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Shuang","family":"Pi","sequence":"additional","affiliation":[{"name":"Changsha University of Science & Technology , , ,","place":["Changsha, China, 410114"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-6038-4320","authenticated-orcid":true,"given":"Zijun","family":"Huang","sequence":"additional","affiliation":[{"name":"Hunan Institute of Engineering , , ,","place":["Xiangtan, P.R. China, 411104"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Zi-Sheng","family":"Chao","sequence":"additional","affiliation":[{"name":"Changsha University of Science & Technology , , ,","place":["Changsha, China, 410114"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3433-7464","authenticated-orcid":true,"given":"Hong-Guang","family":"Jin","sequence":"additional","affiliation":[{"name":"Changsha University of Science & Technology , , ,","place":["Changsha, China, 410114"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,9,7]]},"reference":[{"key":"2026092321452750500_cit1","doi-asserted-by":"publisher","first-page":"10034","DOI":"10.1002\/anie.201709766","article-title":"Visible-light photocatalysis: does it make a difference in organic synthesis?","volume":"57","author":"Marzo","year":"2018","journal-title":"Angew. Chem., Int. 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