| 刘琪,李福伟,孙鹏,高广,席永杰,赵泽伦,黄志威.沉淀剂对Ni-Ce催化剂催化四氢糠醇选择性加氢开环性能的影响[J].分子催化,2025,39(1):14-22 |
| 沉淀剂对Ni-Ce催化剂催化四氢糠醇选择性加氢开环性能的影响 |
| Effect of Precipitators on Selective Hydrogenation Ring-opening of Tetrahydrofurfuryl Alcohol over Ni-Ce Catalysts |
| 投稿时间：2024-10-23 修订日期：2024-12-25 |
| DOI：10.16084/j.issn1001-3555.2025.01.002 |
| 中文关键词: Ni-Ce催化剂 C—O键氢解 四氢糠醇 1,5-戊二醇 |
| 英文关键词:Ni-Ce catalyst C—O bond hydrogenolysis tetrahydrofurfuryl alcohol 1,5-pentanediol |
| 基金项目:国家自然科学基金(22272187, 22102196, 22102193)、甘肃省科技重大专项(22ZD6GA003, 23ZDFA016)、甘肃省科技计划基础研究创新群体项目(23JRRA568)和中国科学院“西部之光”西部青年学者项目[The National Natural Science Foundation of China (22272187, 22102196, 22102193), the Major Project of Gansu Province (22ZD6GA003, 23ZDFA016), the Basic Research Creative Groups Project of the Science and Technology Plan of Gansu Province (23JRRA568) and the CAS “Light of West China” Program]. |
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| 中文摘要: |
| 生物基呋喃化合物制备高值含羟基聚酯单体是绿色化学领域的研究热点, 其中非贵金属催化剂对C—O键断裂的选择性和稳定性仍亟待提高. 本文分别以草酸钠(Na2C2O4)、碳酸钠(Na2CO3)、氢氧化钠(NaOH)和草酸(H2C2O4)为沉淀剂, 采用共沉淀法制备了一系列Ni-Ce催化剂, 考察了其在四氢糠醇(THFA)氢解开环制1,5-戊二醇反应中的催化性能. 利用SEM、XRD、BET、准原位XPS、Raman等表征手段, 研究了沉淀剂对催化剂结构的影响, 探究了催化剂结构与氢解性能之间的关系. 结果表明, 以H2C2O4为沉淀剂的催化剂由于具有较小的粒径尺寸和较高浓度的Ni-VO-Ce物种, 明显优于其他催化剂的催化性能. 在170 ℃, 4 MPa H2, 反应20 h条件下, 该催化剂在THFA氢解反应中对1,5-戊二醇的选择性和收率分别为92.8%和90.4%. 该催化剂表现出良好的稳定性, 循环套用5次未见明显失活. |
| 英文摘要: |
| The transformation of biomass-based furan compounds to high-valued hydroxy-containing polyester monomer has attracted attention in the fields of green chemistry, and the catalytic selectivity and stability of non-noble metal catalysts in the selective scission of C—O bond needs to be improved. In this work, Ni-Ce catalysts are prepared by co-precipitation method using sodium oxalate (Na2C2O4), sodium carbonate (Na2CO3), sodium hydroxide (NaOH), and oxalic acid (H2C2O4) as precipitators, respectively. The structure of catalysts is characterized by SEM, XRD, BET, quasi in-situ XPS and Raman. The effects of different precipitants on catalytic performance of Ni-Ce catalysts in the transformation of tetrahydrofurfuryl alcohol (THFA) to 1,5-pentanediol are investigated, and the structure-activity relationship is preliminarily discussed. The Ni-Ce-H2C2O4 catalyst shows higher catalytic activity (the selectivity and yield of 1,5-pentanediol up to 92.8% and 90.4%, respectively) at 170 ℃ under 4 MPa H2 for 20 h, which can be attributed to its smaller particle size and higher concentration of Ni-VO-Ce species. Furthermore, the catalyst shows good stability and can be recycled 5 times. |
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