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The reaction of thiophenol\/4\u2010chlorothiophenol\/4\u2010methylthiophenol\/4\u2010methoxythiophenol with 2\u2010bromo\u2010<jats:italic>N<\/jats:italic>\u2010quinolin\u20108\u2010yl\u2010acetamide in presence of sodium hydroxide in ethanol at 80\u2009\u00b0C gave [C<jats:sub>9<\/jats:sub>H<jats:sub>6<\/jats:sub>N\u2010NH\u2212C(O)\u2212CH<jats:sub>2<\/jats:sub>\u2010S\u2212Ar] [Ar=C<jats:sub>6<\/jats:sub>H<jats:sub>5<\/jats:sub> (<jats:bold>L1<\/jats:bold>); C<jats:sub>6<\/jats:sub>H<jats:sub>4<\/jats:sub>Cl\u20104 <jats:bold>(L2<\/jats:bold>); C<jats:sub>6<\/jats:sub>H<jats:sub>4<\/jats:sub>Me\u20104 <jats:bold>(L3<\/jats:bold>) and C<jats:sub>6<\/jats:sub>H<jats:sub>4<\/jats:sub>\u2010OMe\u20104 <jats:bold>(L4<\/jats:bold>)], respectively. The corresponding reaction of <jats:bold>L1<\/jats:bold>\u2010<jats:bold>L4<\/jats:bold> with Ni(OAc)<jats:sub>2<\/jats:sub> in methanol at 80\u2009\u00b0C for 3\u2005hours resulted in octahedral nickel complexes [(<jats:bold>L1<\/jats:bold>\u2010H)<jats:sub>2<\/jats:sub>Ni] (<jats:bold>C1<\/jats:bold>), [(<jats:bold>L2<\/jats:bold>\u2010H)<jats:sub>2<\/jats:sub>Ni] (<jats:bold>C2<\/jats:bold>), [(<jats:bold>L3<\/jats:bold>\u2010H)<jats:sub>2<\/jats:sub>Ni] (<jats:bold>C3<\/jats:bold>), and [(<jats:bold>L4<\/jats:bold>\u2010H)<jats:sub>2<\/jats:sub>Ni] (<jats:bold>C4<\/jats:bold>), respectively. All compounds have been characterized by micro and spectroscopic analysis. The molecular structure of complexes <jats:bold>C1<\/jats:bold>\u2013<jats:bold>C3<\/jats:bold> has also been determined by single crystal X\u2010ray diffraction data. The utility of complexes <jats:bold>C1<\/jats:bold>\u2013<jats:bold>C4<\/jats:bold> were evaluated for the <jats:italic>N<\/jats:italic>\u2010alkylation of aniline with benzyl alcohols, and for 1,2\u2010disubstituted benzimidazoles synthesis. The obtained results indicate that complex <jats:bold>C1<\/jats:bold> showed better catalytic activity in both <jats:italic>N<\/jats:italic>\u2010alkylation of amines with benzyl alcohols [catalyst loading: 2.0\u2005mol\u2009%; Yield up to 92\u2009%], and for 1,2\u2010disubstituted benzimidazoles derivatives [catalyst loading: 2.0\u2005mol\u2009%; Yield up to 94\u2009%)]. The mechanistic studies suggested that the reaction works through hydrogen borrowing from benzyl alcohol and its subsequent utilization for <jats:italic>in\u2005situ<\/jats:italic> reduction of imine. The experimentally observed catalytic reactivity patterns of complexes <jats:bold>C1<\/jats:bold>\u2013<jats:bold>C4<\/jats:bold> have found in good agreement with the HOMO\u2010LUMO energy gaps obtained by DFT analysis of corresponding complexes.<\/jats:p>","DOI":"10.1002\/asia.202400557","type":"journal-article","created":{"date-parts":[[2024,7,12]],"date-time":"2024-07-12T03:14:58Z","timestamp":1720754098000},"update-policy":"https:\/\/doi.org\/10.1002\/crossmark_policy","source":"Crossref","is-referenced-by-count":5,"title":["Nickel Complexes Bearing Quinoline Derived NNS Donor Ligands as Catalytic Activators for <i>N<\/i>\u2010Alkylation of Anilines with Alcohols"],"prefix":"10.1002","volume":"19","author":[{"given":"Deepika","family":"Tanwar","sequence":"first","affiliation":[{"name":"Catalysis and Bioinorganic Research Lab Department of Chemistry Deshbandhu College University of Delhi  New Delhi 110019 India"},{"name":"Department of Chemistry University of Delhi  New Delhi 110007 India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Suman","family":"Mahala","sequence":"additional","affiliation":[{"name":"ISC Laboratory Department of Chemistry School of Chemical Sciences and Pharmacy Central University of Rajasthan  NH-8, Bandarsindri Ajmer, Rajasthan 305817 India"}],"role":[{"vocabulary":"crossref","role":"author"}]},{"given":"Deepali","family":"Ahluwalia","sequence":"additional","affiliation":[{"name":"Department of Chemistry S. 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