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Herein, we report that the photoexcitation of LiNH\n                    <jats:sub>2<\/jats:sub>\n                    under UV illumination (0.8 W\u00b7cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    ) induces homolytic N\u2500H bond cleavage and produces a distinctive photo\u2010response with simultaneous evolution of H\n                    <jats:sub>2<\/jats:sub>\n                    , N\n                    <jats:sub>2<\/jats:sub>\n                    , and NH\n                    <jats:sub>3<\/jats:sub>\n                    . Coupling LiNH\n                    <jats:sub>2<\/jats:sub>\n                    with LiH enables UV\u2010driven hydrogen release with effective suppression of gaseous byproducts. Under high\u2010intensity full\u2010spectrum illumination (2.9\u00a0 W\u00b7cm\n                    <jats:sup>\u22122<\/jats:sup>\n                    ), the combined non\u2010thermal and photothermal effects allow complete dehydrogenation of LiNH\n                    <jats:sub>2<\/jats:sub>\n                    \u20102LiH (&gt;10.0\u00a0wt.%), and near\u2010full reversibility over 6 cycles (capacity retention\u00a0ca.\u00a099%). We further realized direct hydrogen release from LiNH\n                    <jats:sub>2<\/jats:sub>\n                    \u20102LiH under natural sunlight. This photo\u2010induced destabilization strategy provides a general route to activate strong bonds in amide\u2010hydride composites and offers a promising approach toward solid\u2010state hydrogen storage under mild conditions.\n                  <\/jats:p>","DOI":"10.1002\/anie.6076689","type":"journal-article","created":{"date-parts":[[2026,7,15]],"date-time":"2026-07-15T12:36:45Z","timestamp":1784119005000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Solar\u2010Driven Reversible Hydrogen Storage Over LiNH\n                    <sub>2<\/sub>\n                    \u20102LiH"],"prefix":"10.1002","volume":"65","author":[{"given":"Zibo","family":"Cheng","sequence":"first","affiliation":[{"name":"Dalian Institute of Chemical Physics Chinese Academy of Sciences  Dalian China"},{"name":"School of Chemistry and Materials Science University of Science and Technology of China  Hefei China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Yeqin","family":"Guan","sequence":"additional","affiliation":[{"name":"Dalian Institute of Chemical Physics Chinese Academy of Sciences  Dalian China"},{"name":"Center of Materials and Optoelectronics Engineering University of Chinese Academy of Sciences  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Le","family":"Xie","sequence":"additional","affiliation":[{"name":"Dalian Institute of Chemical Physics Chinese Academy of Sciences  Dalian China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Qijun","family":"Pei","sequence":"additional","affiliation":[{"name":"Dalian Institute of Chemical Physics Chinese Academy of Sciences  Dalian China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-5464-6649","authenticated-orcid":false,"given":"Hujun","family":"Cao","sequence":"additional","affiliation":[{"name":"Dalian Institute of Chemical Physics Chinese Academy of Sciences  Dalian China"},{"name":"Center of Materials and Optoelectronics Engineering University of Chinese Academy of Sciences  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-0625-0639","authenticated-orcid":false,"given":"Ping","family":"Chen","sequence":"additional","affiliation":[{"name":"Dalian Institute of Chemical Physics Chinese Academy of Sciences  Dalian China"},{"name":"School of Chemistry and Materials Science University of Science and Technology of China  Hefei China"},{"name":"Center of Materials and Optoelectronics Engineering University of Chinese Academy of Sciences  Beijing China"}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"311","published-online":{"date-parts":[[2026,7,15]]},"reference":[{"key":"e_1_2_8_2_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.joule.2020.02.008"},{"key":"e_1_2_8_3_1","doi-asserted-by":"publisher","DOI":"10.1038\/nenergy.2016.130"},{"key":"e_1_2_8_4_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41560\u2010018\u20100209\u2010x"},{"key":"e_1_2_8_5_1","doi-asserted-by":"publisher","DOI":"10.1039\/C8EE01157E"},{"key":"e_1_2_8_6_1","doi-asserted-by":"publisher","DOI":"10.1038\/s41560\u2010021\u201000940\u20104"},{"key":"e_1_2_8_7_1","doi-asserted-by":"publisher","DOI":"10.1038\/natrevmats.2016.59"},{"key":"e_1_2_8_8_1","doi-asserted-by":"publisher","DOI":"10.1016\/S1369\u20107021(08)70251\u20107"},{"key":"e_1_2_8_9_1","doi-asserted-by":"publisher","DOI":"10.1002\/cssc.201500231"},{"key":"e_1_2_8_10_1","doi-asserted-by":"publisher","DOI":"10.1039\/b921645f"},{"key":"e_1_2_8_11_1","doi-asserted-by":"publisher","DOI":"10.1016\/j.nanoen.2012.05.005"},{"key":"e_1_2_8_12_1","doi-asserted-by":"publisher","DOI":"10.1002\/ente.202200433"},{"key":"e_1_2_8_13_1","doi-asserted-by":"publisher","DOI":"10.1002\/adma.201902757"},{"key":"e_1_2_8_14_1","unstructured":"U. 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