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Influence of Re–M interactions in Re–M/C bimetallic catalysts prepared by a microwave-assisted thermolytic method on aqueous-phase hydrogenation of succinic acid
Catalysis Science & Technology ( IF 5 ) Pub Date : 2017-09-18 00:00:00 , DOI: 10.1039/c7cy01039g
Xin Di 1, 2, 3, 4 , Chuang Li 1, 2, 3, 4 , Gwendoline Lafaye 5, 6, 7, 8 , Catherine Especel 5, 6, 7, 8 , Florence Epron 5, 6, 7, 8 , Changhai Liang 1, 2, 3, 4
Affiliation  

Carbon-supported Re–M (M = Pt and Rh) bimetallic catalysts with controlled size and composition were synthesized by using a microwave-assisted thermolytic method and evaluated in the aqueous phase hydrogenation of succinic acid. The Re–M interaction contributes to the inhibition of aggregation of particles and to the improvement in the catalytic activity for succinic acid hydrogenation through decreasing the activation energy. The Re–M interaction favors the ring opening of γ-butyrolactone, an intermediate product, to 1,4-butanediol instead of the hydrogenation and dehydration to tetrahydrofuran observed over a Re/C catalyst. The kinetic study proves that the Re–M interaction can increase the relative formation rate of 1,4-butanediol more than that of tetrahydrofuran, while the strength of the Re–M interaction has a limited influence on the product selectivity. It was shown that the Re–Rh interaction can reduce the direct hydrogenolysis of succinic acid, but it cannot avoid the hydrogenolysis of 1,4-butanediol, thus limiting the selectivity to this product. According to the kinetic mechanism, ring opening of γ-butyrolactone is favored at low temperature while direct hydrogenation to tetrahydrofuran is favored at high temperature.

中文翻译:

微波辅助热解法制备的Re-M / C双金属催化剂中Re-M相互作用对琥珀酸水相加氢的影响

采用微波辅助热解法合成了尺寸和组成均受控的碳载Re-M(M = Pt和Rh)双金属催化剂,并在琥珀酸的水相加氢中进行了评估。Re-M相互作用通过降低活化能,有助于抑制颗粒的聚集并改善琥珀酸加氢的催化活性。Re-M相互作用有利于中间产物γ-丁内酯开环成1,4-丁二醇,而不是在Re / C催化剂上氢化和脱水成四氢呋喃。动力学研究证明,Re-M相互作用比四氢呋喃可增加1,4-丁二醇的相对形成速率,Re-M相互作用的强度对产物的选择性影响有限。结果表明,Re-Rh相互作用可以减少琥珀酸的直接氢解,但不能避免1,4-丁二醇的氢解,因此限制了该产物的选择性。根据动力学机理,在低温下有利于γ-丁内酯的开环,而在高温下有利于直接氢化成四氢呋喃。
更新日期:2017-11-14
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