陈伦刚,刘勇,龙金星,张兴华,张琦,王铁军,马隆龙.丙酸水相加氢反应中Ru负载量对C-C键断裂的影响[J].分子催化,2014,(1):29-38 |
丙酸水相加氢反应中Ru负载量对C-C键断裂的影响 |
The Effect of Ru Loading on the Cleavage of C-C Bond for Propanoic Acid Aqueous-phase Hydrogeantion |
投稿时间:2013-10-20 修订日期:2013-12-17 |
DOI: |
中文关键词: 丙酸 红外光谱 水相 加氢 酰基 脱羰反应 |
英文关键词:Propanoic acid IR Aqueous phase hydrogenation Acyl Decarbonylation |
基金项目:国家自然科学基金(51306189);广东省自然科学基金(S2013040016417)和广东省中国科学院全面战略合作项目(2012B090400042) |
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中文摘要: |
考察了(1.0、4.0、6.0 wt.%)Ru/ZrO2催化剂的丙酸水相加氢性能。采用N2物理吸附、CO脉冲化学吸附、H2程序升温还原(H2-TPR)、CO和丙酸吸附傅里叶变换红外光谱(FTIR)研究了Ru/ZrO2催化剂的物理化学性质。CO-FTIR表明,Ru负载量增加,催化剂表面Ru粒子的富电子程度增加,更接近金属Ru的本征特性。丙酸FTIR表明,丙酸分子在Ru/ZrO2催化剂表面经解离吸附主要形成丙酰基和丙酸盐物种。随Ru含量增加,丙酰基更容易发生脱羰反应,导致C-C键断裂。 |
英文摘要: |
The propanoic acid aqueous phase hydrogenation was investigated over the Ru/ZrO2 catalysts with 1.0, 4.0 and 6.0 wt.% Ru loadings. The physicochemical properties of catalysts were characterized by N2 physisorption, CO pulse chemisorption, temperature programmed reduction of H2, Fourier transform infrared spectra (FTIR) of CO and propanoic acid adsorption. The CO-FTIR exhibited that the Ru sites in abundant electron increased, and become close to the intrinsic properties of the metal Ru with the increase of the Ru loading over the Ru/ZrO2 catalyst. The FTIR of propanoic acid adsorption indicated that the molecular propanoic acid mainly formed the propanoyl and propionate species on the Ru/ZrO2 catalyst surface by dissociation adsorption. However, the propanoyl species were more readily to rupture the C-C bond by decarbonylation on the Ru sites with the increase of Ru loading. |
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