| 盖媛媛,李建法,孙瑞霞,张因.Ni/SiO2-Al2O3催化乙酰丙酸加氢制γ-戊内酯[J].分子催化,2018,32(5):415-424 |
| Ni/SiO2-Al2O3催化乙酰丙酸加氢制γ-戊内酯 |
| Hydrogenation of Levulinic Acid to γ-valerolactone Catalyzed by Ni/SiO2-Al2O3 |
| 投稿时间：2018-08-11 修订日期：2018-09-10 |
| DOI： |
| 中文关键词: 乙酰丙酸 加氢 γ-戊内酯 Ni/SiO2-Al2O3催化剂 SiO2-Al2O3载体 协同作用 |
| 英文关键词:levulinic acid hydrogenation γ-valerolactone Ni/SiO2-Al2O3 catalyst SiO2-Al2O3 support synergistic effect |
| 基金项目:国家自然科学基金（21503124），陕西省教育厅专项科研计划项目（16JK2256），榆林市科技计划项目（2016CXY-16-5）和榆林市科技计划项目（2016CXY-26）资助项目 |
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| 中文摘要: |
| 采用溶胶-凝胶法制备了一系列不同Al2O3含量的SiO2-Al2O3复合氧化物，以该系列复合氧化物为载体，采用等体积浸渍法制备了Ni负载量15%（重量百分比）的催化剂，用于催化乙酰丙酸加氢制γ-戊内酯.采用N2物理吸附、X射线衍射（XRD）、H2程序升温还原（H2-TPR）、H2程序升温脱附（H2-TPD）、NH3程序升温脱附（NH3-TPD）和吡啶吸附红外（Py-IR）等手段对催化剂进行了表征.结果表明，不同载体催化剂的活性组分分散度及表面酸性质存在明显差异，显著影响了催化剂吸附、活化H2与C=O键的能力，进而影响了催化剂的乙酰丙酸加氢活性.其中，Ni/SiO2-Al2O3催化剂上的L酸中心能够促进C=O键的吸附、活化，与金属Ni上的H2吸附活性位协同作用，大大提高了乙酰丙酸加氢活性.因此，具有最多L酸中心和丰富H2吸附活性位的Ni/SiO2-8Al2O3催化剂表现出最高的乙酰丙酸加氢活性，在180℃、4 MPa氢气压力下，乙酰丙酸转化率达到90.5%，目标产物γ-戊内酯选择性为100%. |
| 英文摘要: |
| A series of SiO2-Al2O3 composite oxides with different Al2O3 content were prepared by sol-gel method. Ni/SiO2-Al2O3 catalysts with 15% Ni loading were then prepared via impregnation method and were applied to the selective hydrogenation of levulinic acid. The catalysts were characterized by N2 physisorption, X-ray diffraction (XRD), H2 temperature-programmed reduction (H2-TPR), H2 temperature-programmed desorption (H2-TPD), NH3 temperature-programmed desorption (NH3-TPD) and IR spectra of pyridine adsorption (Py-IR). The results showed that the adsorption and activation capability for H2 and C=O were effectively influenced by supports. Especially, the adsorption and activation of C=O bonds were enhanced by the L acid sites on Ni/SiO2-Al2O3 catalysts. As a result, the activity for levulinic acid hydrogenation was significantly affected by synergistic effect of L acid sites and active Ni sites. Ni/SiO2-8Al2O3 catalyst with the most L acid centersand abundant H2 adsorption sites showed the highest catalytic activity for levulinic acid hydrogenation. The conversion of levulinic acid reached 90.5% and the selectivity for target product γ-valerolactone was 100%, under 180℃ and 4 MPa hydrogen pressure. |
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