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The reaction proceeds efficiently under mild (50\u2009\u00b0C), aerobic, and heterogeneous conditions, using zinc as the terminal reductant, (dtbbpy)NiBr\n                    <jats:sub>2<\/jats:sub>\n                    (2\u2009mol%) as catalyst, and MePh\n                    <jats:sub>3<\/jats:sub>\n                    PBr (10\u2009mol%) as additive, delivering a broad range of diarylmethanes in up to 95% yield with wide functional\u2010group tolerance and gram\u2010scale applicability within 3\u2009h. Mechanistic and electrochemical studies support a radical\/polar crossover pathway in which benzyl radicals, generated off\u2010cycle from benzyl chlorides, are selectively funneled into productive cross\u2010coupling through a predominantly Ni(I)\/Ni(II)\/Ni(III) catalytic manifold rather than diverted into homodimerization. The phosphonium salt appears to modulate nickel speciation, stabilize reduced Ni intermediates, and promote interfacial electron transfer between insoluble substrates and the fraction of nickel catalyst dissolved in the DES. The halide\u2010rich DES environment likely enhances the reducing power of Zn through Zn\n                    <jats:sup>2+<\/jats:sup>\n                    chloride complexation and improved zinc surface activation. Overall, this study establishes DESs as noninnocent media for XEC, providing a sustainable platform beyond conventional volatile organic compound (VOC)\u2010based solvent systems.\n                  <\/jats:p>","DOI":"10.1002\/cssc.70970","type":"journal-article","created":{"date-parts":[[2026,8,20]],"date-time":"2026-08-20T14:03:22Z","timestamp":1787234602000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":0,"title":["Noninnocent Deep Eutectic Solvents Enable Selective, Sustainable Nickel\u2010Catalyzed Cross\u2010Electrophile Couplings to Diarylmethanes"],"prefix":"10.1002","volume":"19","author":[{"ORCID":"https:\/\/orcid.org\/0000-0002-7112-9106","authenticated-orcid":false,"given":"Andrea Nicola","family":"Paparella","sequence":"first","affiliation":[{"name":"Dipartimento di Farmacia\u2013Scienze del Farmaco Universit\u00e0 degli Studi di Bari Aldo Moro Consorzio CINMPIS  Bari 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