首页|Regulating the oxidation state of Pd to enhance the selective hydrogenation for 5-hydroxymethylfurfural
Regulating the oxidation state of Pd to enhance the selective hydrogenation for 5-hydroxymethylfurfural
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The highly selective hydrogenation of 5-hydroxymethylfurfural to 2,5-dihydroxymethylfuran is an impor-tant reaction in the field of biomass hydrogenation,because it is a bridge between biomass resources and chemical industry.Here,we precisely constructed carbon nitride supported Pd-based catalysts by a simple impregnation-reduction method.By changing the reduction temperature,catalysts with different oxidation state could be precisely constructed.Moreover,the important correlation between the ratio of Pd0/Pd2+and catalytic activity is revealed during the selective hydrogenation of HMF.The Pd/g-C3N4-300 catalyst with a Pd0/Pd2+ratio of 3/2 showed the highest catalytic activity,which could get 96.9%5-hydroxymethylfurfural conversion and 90.3%2,5-dihydroxymethylfuran selectivity.Further density functional theory calculation revealed that the synergistic effect between Pd0 and Pd2+in Pd/g-C3N4-300 system could boost the adsorption of the substrate and the dissociation of hydrogen.In this work,we highlight the important correlation between metal oxidation state and catalytic activity,which provides valuable insights for the rational design of precious metal catalysts for hydrogenation reactions.
Pd/g-C3N4Selective hydrogenation5-hydroxymethylfurfural2,5-dihydroxymethylfuranOxidation state
State Key Laboratory of Organic-Inorganic Composites and College of Chemical Engineering Beijing University of Chemical Technology,Beijing 100029,China
National Key Research and Development Program of China