{"status":"ok","message-type":"work","message-version":"1.0.0","message":{"indexed":{"date-parts":[[2026,9,28]],"date-time":"2026-09-28T13:00:34Z","timestamp":1790600434303,"version":"4.1.0"},"reference-count":54,"publisher":"American Chemical Society (ACS)","issue":"9","license":[{"start":{"date-parts":[[2026,8,17]],"date-time":"2026-08-17T00:00:00Z","timestamp":1786924800000},"content-version":"vor","delay-in-days":0,"URL":"https:\/\/creativecommons.org\/licenses\/by\/4.0\/"}],"funder":[{"DOI":"10.13039\/100019180","name":"HORIZON EUROPE European Research Council","doi-asserted-by":"publisher","award":["101041759"],"award-info":[{"award-number":["101041759"]}],"id":[{"id":"10.13039\/100019180","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100011033","name":"Agencia Estatal de Investigaci?n","doi-asserted-by":"publisher","award":["CEX2024 001469-S"],"award-info":[{"award-number":["CEX2024 001469-S"]}],"id":[{"id":"10.13039\/501100011033","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/501100011033","name":"Agencia Estatal de Investigaci?n","doi-asserted-by":"publisher","award":["PID2023-149497NA-I00"],"award-info":[{"award-number":["PID2023-149497NA-I00"]}],"id":[{"id":"10.13039\/501100011033","id-type":"DOI","asserted-by":"publisher"}]},{"DOI":"10.13039\/100018694","name":"HORIZON EUROPE Marie Sklodowska-Curie Actions","doi-asserted-by":"publisher","award":["101202441"],"award-info":[{"award-number":["101202441"]}],"id":[{"id":"10.13039\/100018694","id-type":"DOI","asserted-by":"publisher"}]}],"content-domain":{"domain":[],"crossmark-restriction":false},"short-container-title":[],"published-print":{"date-parts":[[2026,9,28]]},"abstract":"<jats:title>Abstract<\/jats:title>\n                  <jats:p>Mechanical force can often unlock chemical reactivity inaccessible under conventional conditions. However, understanding how molecular structure and environment govern mechanochemical reaction pathways in the solid state remains a significant challenge. In particular, establishing design principles to access heterolytic bond scission in nonpolar materials remains elusive. Here, we investigate a family of diarylmethane-based mechanophores embedded in polymer networks to elucidate how bond identity, substituent electronics, leaving-group stabilization, and matrix interactions collectively determine mechanochemical reactivity. By systematically varying the nature of the scissile bond (C\u2013O vs C\u2013C), the electronic properties of the diarylmethane core, and the presence or absence of hydrogen-bonding functionalities in the surrounding polymer matrix, we establish structure\u2013reactivity relationships that govern the formation of radical and ionic species under tensile load. Mechanophores containing C\u2013O bonds display environment-dependent behavior, with homolytic cleavage dominating in non-hydrogen-bonding matrices and heterolytic scission accessible only when both strongly donating substituents and hydrogen-bond donors are present. In contrast, mechanophores incorporating polarized C\u2013C bonds with strongly stabilizing leaving groups undergo heterolytic cleavage to yield diarylcarbenium ions, even in matrices lacking hydrogen-bonding functionality. These results establish design principles linking molecular structure and polymer environment to mechanochemical reactivity and demonstrate that ionic pathways can be accessed and stabilized in the solid state. More broadly, this work provides guidelines for designing mechanoresponsive materials with distinct reaction pathways and mechanochromic responses.<\/jats:p>","DOI":"10.1021\/jacsau.6c00989","type":"journal-article","created":{"date-parts":[[2026,8,17]],"date-time":"2026-08-17T14:02:07Z","timestamp":1786975327000},"page":"5307-5316","source":"Crossref","is-referenced-by-count":0,"title":["Designing Heterolytic and Homolytic Bond Scission\nin Diarylmethane Mechanophores"],"prefix":"10.1021","volume":"6","author":[{"given":"Gaia","family":"Egizzo","sequence":"first","affiliation":[{"name":"Institute of Chemical Research of Catalonia (ICIQ), The Barcelona Institute of Science and Technology (BIST) , Av. Pai\u0308sos Catalans 16 , ,","place":["Tarragona, Spain, 43007"]},{"name":"Universitat Rovira i Virgili (URV) , , ,","place":["Tarragona, Spain, 43007"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-9715-7992","authenticated-orcid":true,"given":"Eduardo","family":"Garci\u0301a-Padilla","sequence":"additional","affiliation":[{"name":"Institute of Chemical Research of Catalonia (ICIQ), The Barcelona Institute of Science and Technology (BIST) , Av. Pai\u0308sos Catalans 16 , ,","place":["Tarragona, Spain, 43007"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Federico","family":"Frateloreto","sequence":"additional","affiliation":[{"name":"Institute of Chemical Research of Catalonia (ICIQ), The Barcelona Institute of Science and Technology (BIST) , Av. Pai\u0308sos Catalans 16 , ,","place":["Tarragona, Spain, 43007"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0002-4165-3652","authenticated-orcid":true,"given":"Florent","family":"Monie","sequence":"additional","affiliation":[{"name":"Institute of Chemical Research of Catalonia (ICIQ), The Barcelona Institute of Science and Technology (BIST) , Av. Pai\u0308sos Catalans 16 , ,","place":["Tarragona, Spain, 43007"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Dnyaneshwar Ajinath","family":"Mache","sequence":"additional","affiliation":[{"name":"Institute of Chemical Research of Catalonia (ICIQ), The Barcelona Institute of Science and Technology (BIST) , Av. Pai\u0308sos Catalans 16 , ,","place":["Tarragona, Spain, 43007"]},{"name":"Universitat Rovira i Virgili (URV) , , ,","place":["Tarragona, Spain, 43007"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0001-8806-2019","authenticated-orcid":true,"given":"Feliu","family":"Maseras","sequence":"additional","affiliation":[{"name":"Institute of Chemical Research of Catalonia (ICIQ), The Barcelona Institute of Science and Technology (BIST) , Av. Pai\u0308sos Catalans 16 , ,","place":["Tarragona, Spain, 43007"]}],"role":[{"vocabulary":"crossref","role":"author"}]},{"ORCID":"https:\/\/orcid.org\/0000-0003-3435-8310","authenticated-orcid":true,"given":"Jose\u0301 Augusto","family":"Berrocal","sequence":"additional","affiliation":[{"name":"Institute of Chemical Research of Catalonia (ICIQ), The Barcelona Institute of Science and Technology (BIST) , Av. Pai\u0308sos Catalans 16 , ,","place":["Tarragona, Spain, 43007"]},{"name":"Catalan Institution for Research and Advanced Studies (ICREA) , Pg. Llui\u0301s Companys 23 , ,","place":["Barcelona, Spain, 08010"]}],"role":[{"vocabulary":"crossref","role":"author"}]}],"member":"316","published-online":{"date-parts":[[2026,8,17]]},"reference":[{"issue":"7243","key":"2026092808095120500_cit1","doi-asserted-by":"publisher","first-page":"68","DOI":"10.1038\/nature07970","article-title":"Force-Induced Activation\nof Covalent Bonds in Mechanoresponsive Polymeric Materials","volume":"459","author":"Davis","year":"2009","journal-title":"Nature"},{"issue":"18","key":"2026092808095120500_cit2","doi-asserted-by":"publisher","first-page":"7497","DOI":"10.1039\/c2cs35463b","article-title":"Polymer Mechanochemistry: Techniques to Generate Molecular\nForce via Elongational Flows","volume":"42","author":"May","year":"2013","journal-title":"Chem. Soc. 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