Abstract
Allylic alcohols are the essential building blocks widely used in diverse streams of organic inventions for pharmaceuticals, fragrances, agrochemicals and polymers. Currently, allylic alcohols are industrially produced from petroleum-based feedstocks via atom uneconomic processes. More sustainable synthesis route for allylic alcohols is limited. Herein, a methodology for the direct and highly selective production of allylic alcohols has been accomplished by controlled dehydrogenative α-methylenation of alcohols with methanol. This transformation is enabled by interfacial Lewis acid-basic pair on tailor-made ZnO/4Mg1ZrOx mixed oxide. High selectivity (83∼92%) of allylic alcohols is the consequence of alcohols acceptorless dehydrogenation to liberation of H2 and Meerwein-Ponndorf-Verley type hydrogen transfer onto C = O bonds of unsaturated aldehydes. Furthermore, the prepared ZnO/4Mg1ZrOx mixed oxide shows good stability after 200 h time on stream test. These observations could additionally allow us to design multifunctional solid acid-basic catalysts for the transformations of renewable oxygenates into value-added chemicals.
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