李海涛,郝全爱,王志鹏,班丽君,孟平凡,牛珠珠,高春光,徐亚琳,赵永祥.不同沉淀剂制备CuO-ZnO催化剂甲醛乙炔化反应性能[J].分子催化,2019,33(2):124-131 |
不同沉淀剂制备CuO-ZnO催化剂甲醛乙炔化反应性能 |
Study on Catalytic Performance of CuO-ZnO Catalyst Prepared by Different Precipitants |
投稿时间:2019-01-16 修订日期:2019-02-19 |
DOI: |
中文关键词: CuO-ZnO 甲醛乙炔化 1,4-丁炔二醇 沉淀剂 |
英文关键词:CuO-ZnO formaldehyde acetylation 1,4-butynediol precipitants |
基金项目:国家自然科学基金(U1710221,21503124);山西省国际合作项目(201603D421025,201703D421034) |
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中文摘要: |
分别以NaOH、Na2CO3、NaHCO3为沉淀剂,采用共沉淀法制备了Cu:Zn摩尔比为2:1的CuO-ZnO催化剂,利用氢气程序升温还原(H2-TPR)、热重(TG)、X射线衍射(XRD)及拉曼光谱(Raman)等技术对催化剂进行了表征,结合甲醛乙炔化活性评价,研究了沉淀剂对催化剂结构及催化性能的影响.结果表明,不同沉淀剂对催化剂中活性组分分散度有较大影响,进而在甲醛乙炔化合成1,4-丁炔二醇反应中表现出不同的催化活性.以Na2CO3为沉淀剂制备的催化剂中形成CuO-ZnO固溶体,提高了CuO的分散度及Cu+在还原性气氛下的稳定性,经活化后可生成较多的活性物种炔化亚铜,表现出最佳的炔化反应活性与1,4-丁炔二醇选择性. |
英文摘要: |
CuO-ZnO catalyst with Cu:Zn molar ratio of 2:1 was prepared by coprecipitation method using NaOH, Na2CO3 and NaHCO3 as precipitants. The catalysts were characterized by thermogravimetry (TG), hydrogen-programmed reduction (H2-TPR), X-ray diffraction (XRD) and Raman spectroscopy (Raman). Combined with the evaluation of formaldehyde acetylation activity, the effect of precipitation agent on the structure and cataly-tic performance of the catalyst were studied. The results show that different precipitants have a great influence on the dispersion of active components in the catalyst, and then show different catalytic activities in the reaction of formaldehyde acetylation to 1,4-butynediol. In the CZ(Na2CO3) catalyst, the active species CuO and ZnO form a CuO-ZnO solid solution, which improves the dispersion of CuO and the stability of Cu+ under reducing atmosphere. After activation, more active central species acetylene cuprous can be formed. The optimum alkyneization activity is selective with 1,4-butynediol. |
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