Aqueous-phase hydrodeoxygenation of carboxylic acids to alcohols or alkanes over supported Ru catalysts

Aqueous-phase hydrodeoxygenation of carboxylic acids to alcohols or alkanes over supported Ru catalysts
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负载型 Ru 催化剂上羧酸水相加氢脱氧生成醇或烷烃

DOI:
10.1016/j.molcata.2011.10.015
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发表时间:
2011-12
期刊:
Journal of Molecular Catalysis A: Chemical
影响因子:
--
通讯作者:
Li, Yongwang
Li, Yongwang
中科院分区:
其他
文献类型:
--
作者:
Chen, Lungang;Zhu, Yulei;Zheng, Hongyan;Zhang, Chenghua;Zhang, Bin;Li, Yongwang

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针对 Ru/C、Ru/ZrO2 和 Ru/Al2O3 催化剂上羧酸的水相加氢脱氧 (APHDO),通过收集反应动力学数据和 DRIFTS 测量,研究了 CO 加氢和 C-C 键断裂反应。 C-C 键断裂在高温和高金属负载量下得到改善。酸性载体与Ru金属结合有利于羧基的CO加氢。通过DRIFTS方法研究了催化剂上酰基脱羰引起的C-C键断裂。 APHDO和DRIFTS结果表明C-C键断裂的顺序为Ru/C>Ru/ZrO2>Ru/Al2O3。通过多种方法(H2-TPR、NH3-TPD、CO-FTIR 和丙酸 DRIFTS)对催化剂进行了表征。结论是,载体对反应路线的影响可能归因于催化剂的这些因素,即表面酸性、金属-载体相互作用和Ru物质的电子态。
For the aqueous-phase hydrodeoxygenation (APHDO) of carboxylic acids over the Ru/C, Ru/ZrO2and Ru/Al2O3catalysts, the CO hydrogenation and C–C bond cleavage reactions were studied by collecting reaction kinetics data and the measures of DRIFTS. The C–C bond cleavage was improved at high temperature and with high metal loadings. The acidic supports in combination with Ru metal can favor the CO hydrogenation of carboxyl. The C–C bond cleavage derived from the decarbonylation of acyl on the catalyst was studied by the measures of DRIFTS. The APHDO and DRIFTS results demonstrated that the C–C bond cleavage was favored in the order of Ru/C>Ru/ZrO2>Ru/Al2O3. The catalysts were characterized by multiple methods (H2-TPR, NH3-TPD, CO-FTIR and DRIFTS of propanoic acid). It is concluded that the effect of support on the reaction routes may be attributed to these factors of catalysts, i.e., surface acidity, metal–support interaction and electronic state of Ru species.
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