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This protocol demonstrates the synthesis of branched carbonyl compounds, <jats:italic>\u03b1<\/jats:italic>,<jats:italic>\u03b1<\/jats:italic>\u2010disubstituted ketones, and <jats:italic>\u03b1<\/jats:italic>\u2010substituted chalcones <jats:italic>via<\/jats:italic> borrowing hydrogen strategy and acceptorless dehydrogenative coupling, respectively. A wide range of aryl\u2010based secondary alcohols are coupled with various primary alcohols in this tandem dehydrogenation\/hydrogenation reaction. The nickel catalyst, along with KO<jats:sup><jats:italic>t<\/jats:italic><\/jats:sup>Bu or K<jats:sub>2<\/jats:sub>CO<jats:sub>3<\/jats:sub>, governed the selectivity for the formation of branched saturated ketones or chalcones. 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