{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,3,21]],"date-time":"2026-03-21T06:42:58Z","timestamp":1774075378743,"version":"3.50.1"},"reference-count":47,"publisher":"Wiley","issue":"4","license":[{"start":{"date-parts":[[2025,4,10]],"date-time":"2025-04-10T00:00:00Z","timestamp":1744243200000},"content-version":"vor","delay-in-days":0,"URL":"http:\/\/creativecommons.org\/licenses\/by\/4.0\/"}],"funder":[{"DOI":"10.13039\/501100001809","name":"National Natural Science Foundation of China","doi-asserted-by":"publisher","award":["22478261"],"award-info":[{"award-number":["22478261"]}],"id":[{"id":"10.13039\/501100001809","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100001809","name":"National Natural Science Foundation of China","doi-asserted-by":"publisher","award":["22178229"],"award-info":[{"award-number":["22178229"]}],"id":[{"id":"10.13039\/501100001809","id-type":"DOI","asserted-by":"publisher"}]}],"content-domain":{"domain":["onlinelibrary.wiley.com"],"crossmark-restriction":true},"short-container-title":["Exploration"],"published-print":{"date-parts":[[2025,8]]},"abstract":"<jats:title>ABSTRACT<\/jats:title><jats:p>The C\u2500H bond is the most abundant chemical bond in organic compounds. Therefore, the development of the more direct methods for C\u2500H bond cleavage and the elucidation of their mechanisms will provide an important theoretical basis for achieving more efficient C\u2500H functionalization and target molecule construction. In this study, the catalyst\u2010free photon\u2010induced direct homolysis of C<jats:sub>sp3<\/jats:sub>\u2500H bonds at room temperature was discovered for the first time. The applicable substrate scope of this phenomenon is very wide, expanding from the initial benzyl compounds to aliphatic alcohols, alkanes, olefins, polymers containing benzyl hydrogens, and even gaseous methane. Experiments and calculations have demonstrated that this process involves rapid vibrational relaxation on the femtosecond time scale, leading to the formation of hydrogen radical and carbon radical. Importantly, the direct homolysis of C<jats:sub>sp3<\/jats:sub>\u2500H bonds is independent of the presence of oxidants, highlighting its spontaneous nature. Additionally, the cleaved hydrogen radical exhibits diverse reactivity, including coupling reactions to produce hydrogen gas (H<jats:sub>2<\/jats:sub>), reduction of oxygen to generate hydrogen peroxide (H<jats:sub>2<\/jats:sub>O<jats:sub>2<\/jats:sub>), and reduction of carbon dioxide to formic acid (HCOOH). Notably, in the field of H<jats:sub>2<\/jats:sub>O<jats:sub>2<\/jats:sub> production, the absence of a catalyst allows for the bypassing of inherent drawbacks associated with photocatalysts, thereby presenting significant potential for practical application. Furthermore, the cleaved carbon radicals display enhanced reactivity, providing excellent opportunities for direct functionalization, thereby enabling efficient C\u2500H bond activation and molecular construction. Overall, this significant discovery offers a valuable new strategy for the production of bulk chemicals, organic synthesis, low\u2010carbon and hydrogen energy industries, as well as environmental treatment.<\/jats:p>","DOI":"10.1002\/exp.20240237","type":"journal-article","created":{"date-parts":[[2025,4,11]],"date-time":"2025-04-11T02:21:07Z","timestamp":1744338067000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":2,"title":["Room\u2010Temperature Direct Homolysis of C<sub>sp3<\/sub>\u2500H Bond via Catalyst\u2010Free Photoexcitation"],"prefix":"10.1002","volume":"5","author":[{"given":"Qi","family":"Miao","sequence":"first","affiliation":[{"name":"Low\u2010Carbon Technology and Chemical Reaction Engineering Laboratory School of Chemical Engineering Sichuan University Chengdu P.R. China"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Meng","family":"Liu","sequence":"additional","affiliation":[{"name":"Low\u2010Carbon Technology and Chemical Reaction Engineering Laboratory School of Chemical Engineering Sichuan University Chengdu P.R. China"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Jun","family":"Wang","sequence":"additional","affiliation":[{"name":"State Key Laboratory of Environmental\u2010Friendly Energy Materials School of Materials and Chemistry Southwest University of Science and Technology Mianyang China"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Pan","family":"Wu","sequence":"additional","affiliation":[{"name":"Low\u2010Carbon Technology and Chemical Reaction Engineering Laboratory School of Chemical Engineering Sichuan University Chengdu P.R. China"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Changjun","family":"Liu","sequence":"additional","affiliation":[{"name":"Low\u2010Carbon Technology and Chemical Reaction Engineering Laboratory School of Chemical Engineering Sichuan University Chengdu P.R. China"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"given":"Jian","family":"He","sequence":"additional","affiliation":[{"name":"Low\u2010Carbon Technology and Chemical Reaction Engineering Laboratory School of Chemical Engineering Sichuan University Chengdu P.R. China"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-1917-6738","authenticated-orcid":false,"given":"Giacomo Lo","family":"Zupone","sequence":"additional","affiliation":[{"name":"Department of Mechanics Mathematics and Management Polytechnic of Bari Bari Italy"}],"role":[{"role":"author","vocabulary":"crossref"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-5560-0885","authenticated-orcid":false,"given":"Wei","family":"Jiang","sequence":"additional","affiliation":[{"name":"Low\u2010Carbon Technology and Chemical Reaction Engineering Laboratory School of Chemical Engineering Sichuan University Chengdu P.R. China"}],"role":[{"role":"author","vocabulary":"crossref"}]}],"member":"311","published-online":{"date-parts":[[2025,4,10]]},"reference":[{"key":"e_1_2_7_2_1","doi-asserted-by":"publisher","DOI":"10.1126\/science.1114731"},{"key":"e_1_2_7_3_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.1c00263"},{"key":"e_1_2_7_4_1","doi-asserted-by":"publisher","DOI":"10.1038\/nchem.1607"},{"key":"e_1_2_7_5_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.chemrev.6b00620"},{"key":"e_1_2_7_6_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.orglett.5b00088"},{"key":"e_1_2_7_7_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201504603"},{"key":"e_1_2_7_8_1","doi-asserted-by":"publisher","DOI":"10.1039\/c2sc20712e"},{"key":"e_1_2_7_9_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.201406393"},{"key":"e_1_2_7_10_1","doi-asserted-by":"publisher","DOI":"10.1039\/D1CS00727K"},{"key":"e_1_2_7_11_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41570-022-00388-4"},{"key":"e_1_2_7_12_1","doi-asserted-by":"publisher","DOI":"10.1038\/s44160-022-00180-8"},{"key":"e_1_2_7_13_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.chempr.2021.04.009"},{"key":"e_1_2_7_14_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-021-24203-8"},{"key":"e_1_2_7_15_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja502639e"},{"key":"e_1_2_7_16_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja411596q"},{"key":"e_1_2_7_17_1","doi-asserted-by":"publisher","DOI":"10.1038\/nature14255"},{"key":"e_1_2_7_18_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.accounts.6b00272"},{"key":"e_1_2_7_19_1","doi-asserted-by":"publisher","DOI":"10.1002\/smll.201601545"},{"key":"e_1_2_7_20_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.biomac.8b00123"},{"key":"e_1_2_7_21_1","doi-asserted-by":"publisher","DOI":"10.1002\/marc.201800528"},{"key":"e_1_2_7_22_1","doi-asserted-by":"publisher","DOI":"10.1039\/C8QM00528A"},{"key":"e_1_2_7_23_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41557-024-01472-6"},{"key":"e_1_2_7_24_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja00132a008"},{"key":"e_1_2_7_25_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-017-01906-5"},{"key":"e_1_2_7_26_1","doi-asserted-by":"publisher","DOI":"10.1021\/ja803879k"},{"key":"e_1_2_7_27_1","doi-asserted-by":"publisher","DOI":"10.1021\/ol801488w"},{"key":"e_1_2_7_28_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.9b01060"},{"key":"e_1_2_7_29_1","doi-asserted-by":"publisher","DOI":"10.1039\/D2SC03590A"},{"key":"e_1_2_7_30_1","doi-asserted-by":"publisher","DOI":"10.1038\/s44160-022-00125-1"},{"key":"e_1_2_7_31_1","doi-asserted-by":"publisher","DOI":"10.1021\/acs.jpclett.1c02182"},{"key":"e_1_2_7_32_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.6b13223"},{"key":"e_1_2_7_33_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.rser.2023.113323"},{"key":"e_1_2_7_34_1","doi-asserted-by":"publisher","DOI":"10.1039\/D0TA05753C"},{"key":"e_1_2_7_35_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41929-021-00605-1"},{"key":"e_1_2_7_36_1","doi-asserted-by":"publisher","DOI":"10.1021\/acsami.1c02953"},{"key":"e_1_2_7_37_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202202328"},{"key":"e_1_2_7_38_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41563-019-0398-0"},{"key":"e_1_2_7_39_1","doi-asserted-by":"publisher","DOI":"10.1021\/jacs.1c04622"},{"key":"e_1_2_7_40_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.202203225"},{"key":"e_1_2_7_41_1","doi-asserted-by":"publisher","DOI":"10.1038\/s44160-023-00272-z"},{"key":"e_1_2_7_42_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41560-023-01218-7"},{"key":"e_1_2_7_43_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41467-023-40007-4"},{"key":"e_1_2_7_44_1","doi-asserted-by":"publisher","DOI":"10.1002\/advs.202103408"},{"key":"e_1_2_7_45_1","doi-asserted-by":"publisher","DOI":"10.1039\/D1CC02551A"},{"key":"e_1_2_7_46_1","doi-asserted-by":"publisher","DOI":"10.1002\/anie.202207410"},{"key":"e_1_2_7_47_1","doi-asserted-by":"publisher","DOI":"10.1021\/acscatal.3c00326"},{"key":"e_1_2_7_48_1","doi-asserted-by":"publisher","DOI":"10.1002\/EXP.20210063"}],"container-title":["Exploration"],"original-title":[],"language":"en","link":[{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/pdf\/10.1002\/EXP.20240237","content-type":"unspecified","content-version":"vor","intended-application":"similarity-checking"}],"deposited":{"date-parts":[[2025,8,26]],"date-time":"2025-08-26T10:32:02Z","timestamp":1756204322000},"score":1,"resource":{"primary":{"URL":"https:\/\/onlinelibrary.wiley.com\/doi\/10.1002\/EXP.20240237"}},"subtitle":[],"short-title":[],"issued":{"date-parts":[[2025,4,10]]},"references-count":47,"journal-issue":{"issue":"4","published-print":{"date-parts":[[2025,8]]}},"alternative-id":["10.1002\/EXP.20240237"],"URL":"https:\/\/doi.org\/10.1002\/exp.20240237","archive":["Portico"],"relation":{},"ISSN":["2766-8509","2766-2098"],"issn-type":[{"value":"2766-8509","type":"print"},{"value":"2766-2098","type":"electronic"}],"subject":[],"published":{"date-parts":[[2025,4,10]]},"assertion":[{"value":"2024-07-28","order":0,"name":"received","label":"Received","group":{"name":"publication_history","label":"Publication History"}},{"value":"2025-02-24","order":2,"name":"accepted","label":"Accepted","group":{"name":"publication_history","label":"Publication History"}},{"value":"2025-04-10","order":3,"name":"published","label":"Published","group":{"name":"publication_history","label":"Publication History"}}],"article-number":"e20240237"}}