| 沈美玉,王晓月,孙德,赵凤伟,杜长海.La修饰的Co-B非晶态催化剂用于乳酸乙酯选择性加氢制1,2-丙二醇[J].分子催化,2016,30(1):1-9 |
| La修饰的Co-B非晶态催化剂用于乳酸乙酯选择性加氢制1,2-丙二醇 |
| Selective Hydrogenation of Ethyl Lactate to 1,2-propanediol over the La-doped Co-B Amorphous Catalyst |
| 投稿时间：2015-12-04 修订日期：2016-01-11 |
| DOI： |
| 中文关键词: 非晶态合金 助剂La 催化加氢 乳酸乙酯 Co-La-B 1,2-丙二醇 |
| 英文关键词:amorphous alloy La-additives catalytic hydrogenation ethyl lactate Co-La-B 1,2-propanediol |
| 基金项目:吉林省科技厅自然科学基金(201215117)资助项目 |
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| 中文摘要: |
| 用化学还原法制备了La修饰的Co-B非晶态合金催化剂(Co-La-B)，并考察了其在乳酸乙酯液相加氢制1,2-丙二醇(1,2-PDO)反应中的催化性能. 通过X射线粉末衍射(XRD)、透射电子显微镜(TEM)、物理吸附(BET)、差示扫描量热(DSC)、电感耦合等离子发射光谱(ICP-OES)、X射线光电子能谱(XPS)、催化剂活性比表面积（Sco）、氢程序升温脱附（H2-TPD）等手段对催化剂进行表征，研究了稀土助剂La对Co-B催化剂催化性能的影响. 结果表明，活性组分Co以元素态和氧化态两种形式存在于Co-La-B非晶态合金催化剂中，催化剂中存在B向Co的电子转移，富电子的Co用于活化氢，氧化态形式存在的La3 促进了B向Co的电子转移; 适量的La能提高催化剂的热稳定性，显著减小催化剂粒径，使催化剂形成更加单一的Co吸附活性位，有利于吸附活化的氢促进加氢反应进行. 在氢气压力6 MPa，反应温度433 K，反应时间9 h条件下，0.5 % Co-La-B催化剂表现出最优的催化加氢性能，乳酸乙酯的转化率达到99.7 %，1,2-丙二醇的选择性达到98.5 %. |
| 英文摘要: |
| The La-doped Co-B amorphous alloy catalyst (Co-La-B) was prepared by the chemical reduction method for liquid phase hydrogenation of ethyl lactate to 1,2-propanediol (1,2-PDO). The Co-La-B catalysts were characterized using X-ray diffraction (XRD), transmission electron microscopy(TEM), physical adsorption (BET)，differential scanning calorimetry (DSC), inductively coupled plasma atomic emission spectrometry (ICP-AES), X-ray photoelectron spectroscopy (XPS), the active surface area (SCo) and H2 temperature-programmed desorption (H2-TPD). The effects of the La content on the hydrogenation of ethyl lactate were investigated. At a suitable La content, the Co-La-B amorphous alloy catalyst exhibited higher activity and selectivity than the Co-B catalyst in the hydrogenation. With the increase of La, the activity first increased and then decreased. The optimum theoretical La content was 0.5 % (mole ratio), at which the conversion of ethyl lactate could reach 99.7 % and the selectivity of 1,2-propanediol could reach 98.5 %. The promoting effect of the La-dopant could be attributed to the dispersing effect that resulted in the higher thermal stability and appropriate particle size, unique Co active sites and electron transfer effect between Co and B. |
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