| 刘琳丽,李海涛,王长真,武瑞芳,徐亚琳,赵永祥.负载Ni催化剂上1,4-丁炔二醇加氢反应的载体效应研究[J].分子催化,2018,32(2):99-106 |
| 负载Ni催化剂上1,4-丁炔二醇加氢反应的载体效应研究 |
| Effect of Supports on the Hydrogenation of 1, 4-Butynediol over Supported Ni Catalyst |
| 投稿时间：2017-12-28 修订日期：2018-02-10 |
| DOI： |
| 中文关键词: 1,4-丁炔二醇 加氢 Ni/Al2O3 Ni/SiO2 Ni/ZrO2 |
| 英文关键词:1,4-butynediol hydrogenation Ni/Al2O3 Ni/SiO2 Ni/ZrO2 |
| 基金项目:国家自然青年科学基金（21503124）；国家自然科学基金面上项目（21673132）. |
| 作者 | 单位 | E-mail | | 刘琳丽 | 山西大学 化学化工学院, 精细化学品教育部工程研究中心, 山西 太原 030006 | | | 李海涛 | 山西大学 化学化工学院, 精细化学品教育部工程研究中心, 山西 太原 030006 | htli@sxu.edu.cn | | 王长真 | 山西大学 化学化工学院, 精细化学品教育部工程研究中心, 山西 太原 030006 | | | 武瑞芳 | 山西大学 化学化工学院, 精细化学品教育部工程研究中心, 山西 太原 030006 | | | 徐亚琳 | 山西大学 化学化工学院, 精细化学品教育部工程研究中心, 山西 太原 030006 | | | 赵永祥 | 山西大学 化学化工学院, 精细化学品教育部工程研究中心, 山西 太原 030006 | yxzhao@sxu.edu.cn |
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| 中文摘要: |
| 制备了Ni负载量为15%的3种催化剂Ni/Al2O3、Ni/SiO2、Ni/ZrO2，考察了其在1，4-丁炔二醇加氢反应中的催化性能，结合XRD、H2-TPR、H2-TPD、N2物理吸附等表征，研究了载体性质对催化剂1，4-丁炔二醇加氢性能的影响.结果表明，Ni/SiO2催化剂上，由于Ni与SiO2间弱的相互作用，Ni物种主要以大晶粒形式存在，产生大量弱吸附H2物种，有利于低温下1，4-丁炔二醇加氢，在温度50℃，氢气压力1 MPa时，反应2 h可实现1，4-丁炔二醇的完全转化，1，4-丁烯二醇和1，4-丁二醇选择性分别达到68.1%与18.2%.Ni/Al2O3中Ni与载体间具有强相互作用，主要存在Ni-Al2O3界面或溢流到Al2O3载体表面的强吸附H2物种，而Ni表面的弱吸附H2物种较少，催化加氢活性明显降低.Ni/ZrO2中由于还原过程中ZrO2的迁移包裹作用，Ni表面低温吸附H2物种最少，活性最低，1，4-丁炔二醇转化率仅为8.1%，主产物为1，4-丁烯二醇. |
| 英文摘要: |
| Ni/Al2O3, Ni/SiO2 and Ni/ZrO2 catalysts with 15% Ni loadings were prepared by impregnation method using Al2O3, SiO2 and ZrO2 as supports, and Ni(NO3)·6H2O as Ni source. The catalytic performance of these catalysts was investigated in the hydrogenation of 1,4-butynediol. By relating catalytic results to the results of XRD, H2-TPR, H2-TPD and N2 physical adsorption, the effects of support properties on hydrogenation performance of catalyst were studied. It was found that Ni species on Ni/SiO2 existed mainly in the form of large grains due to the weak interaction between Ni and SiO2, resulting in a large number of weakly adsorbed H2 species which was beneficial to the hydrogenation of 1,4-butynediol at low temperatures. The 1,4-butynediol was completely converted, and the selectivity of 1,4-butenediol and 1,4-butanediol reached 68.1% and 18.2%, respectively, at the reaction temperature of 50℃, hydrogen pressure of 1.0 MPa and a reaction time of 2 h. As to Ni/Al2O3. Ni has strong interaction with the carrier, leading to increased number of hydrogen species adsorbed strongly on the Ni-Al2O3 interface or on carrier surface and little weakly adsorbed H2 species on Ni surface. As a result, the catalytic hydrogenation activity is significantly reduced. As to Ni/ZrO2, due to the migration and encapsulation effects of ZrO2 in the reduction process, the adsorption of H2 on Ni was prohibited which resulted in the poorest catalytic activity of Ni/ZrO2. The conversion of 1,4-butynediol was only 8.1%, and the main product was 1,4-butenediol. |
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