化工进展 ›› 2023, Vol. 42 ›› Issue (1): 289-296.DOI: 10.16085/j.issn.1000-6613.2022-0584

• 工业催化 • 上一篇    下一篇

Al掺杂的Cu/SBA-15催化剂用于己二酸二甲酯加氢合成1,6-己二醇

刘书林(), 杨娜, 张龙飞, 孙永利, 姜斌, 肖晓明, 澹台晓伟, 张吕鸿()   

  1. 天津大学化工学院,天津 300072
  • 收稿日期:2022-04-07 修回日期:2022-05-26 出版日期:2023-01-25 发布日期:2023-02-20
  • 通讯作者: 张吕鸿
  • 作者简介:刘书林(1996—),男,硕士研究生,研究方向为酯加氢催化剂的性能。E-mail:2019207435@tju.edu.cn

Al-doped Cu/SBA-15 catalysts for the hydrogenation of dimethyl adipate to 1,6-hexanediol

LIU Shulin(), YANG Na, ZHANG Longfei, SUN Yongli, JIANG Bin, XIAO Xiaoming, TANTAI Xiaowei, ZHANG Lyuhong()   

  1. School of Chemical Engineering and Technology, Tianjin University, Tianjin 300072, China
  • Received:2022-04-07 Revised:2022-05-26 Online:2023-01-25 Published:2023-02-20
  • Contact: ZHANG Lyuhong

摘要:

作为一种重要的有机合成原料,1,6-己二醇(HDO)的工业化生产主要通过己二酸二甲酯(DMA)加氢反应来实现,而理性设计开发相应的Cu基催化剂是提高HDO产率的关键。本文采用Al掺杂的介孔分子筛SBA-15为载体制备得到了一系列CuAl x /SBA-15催化剂,探究了使用该催化剂用于DMA加氢反应合成HDO的催化性能和催化机理,并对反应条件进行了优化。研究结果表明:CuAl5/SBA-15催化剂能够增加催化剂的路易斯酸酸量,提高Cu+/Cu0的比例,从而提升DMA加氢反应的选择性,同时Al的掺杂也能减少Cu活性组分的团聚,从而增强催化剂的稳定性。当反应温度为240℃、反应压力为6MPa、反应时间为6h时,HDO的反应产率达到最大,为87.05%;重复使用CuAl5/SBA-15催化剂36h后,HDO的反应产率能够维持在86.01%左右。本文的研究结果对设计Cu基催化剂用于酯加氢反应具有一定的借鉴意义。

关键词: 催化剂, 分子筛, 加氢, 反应, 优化

Abstract:

The industrial production of 1,6-hexanediol (HDO) is by the hydrogenation of dimethyl adipate (DMA). The rational design and development of the Cu-based catalysts is of great importance to improve the yield of HDO. In this work, a series of CuAl x /SBA-15 catalysts on Al-doped mesoporous molecular sieve SBA-15 were prepared. The catalytic performance and mechanism of the catalysts were investigated, and the reaction conditions were also optimized. The results showed that the CuAl5/SBA-15 catalyst increased the amount of Lewis acid in the catalyst matrix and improved the Cu+/Cu0 ratio, thus enhancing the selectivity of the DMA hydrogenation reaction. Besides, the doping of Al reduced the agglomeration of Cu active species, and therefore, improved the stability of the catalyst. The yield of HDO reached the maximum of 87.05% under the reaction conditions of 240℃, 6MPa, and 6h. After the CuAl5/SBA-15 catalyst was recycled for 36h, the yield of HDO maintained at about 86.01%, implying great stability of catalyst. In summary, the results of this study provided reference for the design of Cu-based catalysts for ester hydrogenation reactions.

Key words: catalyst, molecular sieves, hydrogenation, reaction, optimization

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