过渡金属负载Silicalite-1分子筛的制备及其催化糠醛加氢性能研究
收稿日期: 2023-08-29
网络出版日期: 2024-04-18
基金资助
国家自然科学基金项目(21905144);南开大学2022年自制实验教学仪器设备类项目（气态流动鼓泡反应器的研制）
Study on preparation of transition metal-supported Silicalite-1 zeolite catalyst and its catalytic performance for furfural hydrogenation
Received date: 2023-08-29
Online published: 2024-04-18
糠醛是一种重要的生物质平台分子，研发具有高活性和稳定性的糠醛加氢催化剂是当前的研究焦点，但贵金属催化剂的高成本问题使得其难以满足大规模工业生产的需求。利用一步水热法成功地合成了过渡金属负载Silicalite-1分子筛催化剂，并探讨了引入不同类型的过渡金属（如Ni、Co、Cu和Fe）对Silicalite-1分子筛结构产生的影响。研究结果表明：低金属负载量并不会对分子筛结构的形成产生影响，同时金属物种在分子筛载体的表面也能均匀分布。在糠醛的加氢转化过程中，Ni基催化剂S-Ni2展现出优异的糠醛转化能力，糠醛的转化率高达96%，产物呋喃的选择性保持在71%左右。Cu基催化剂S-Cu1表现出优异的糠醇选择性，产物选择性接近100%，这一性能明显优于通过浸渍法制得的铜基催化剂（76%）。因此，与浸渍法相比，采用一步水热法可以获得具有高选择性的催化剂，且该方法简单易操作。本研究为寻找高效、稳定且经济的金属加氢催化剂开辟了新的方向，并促进了生物质资源的高值化应用。
关键词： 金属负载分子筛; Silicalite-1分子筛; 糠醛加氢; 一步水热法
狄璐 , 王卫国 , 陈珏先 , 吴传淑 . 过渡金属负载Silicalite-1分子筛的制备及其催化糠醛加氢性能研究[J]. 无机盐工业, 2024 , 56(4) : 125 -132 . DOI: 10.19964/j.issn.1006-4990.2023-0423
Furfural is an important biomass-derived platform molecule，and developing robust catalysts with high activity and stability for furfural hydrogenation is a research hotspot.However，noble metal catalysts suffer from high costs，which cannot satisfy the demand towards large-scale industrial production.Herein，the transition metal-supported Silicalite-1 zeolite catalysts were successfully synthesized by a one-step hydrothermal method，and the influence of the introduction of four different types of transition metal elements on the structure of the Silicalite-1 zeolite was studied.Comprehensive characterization results showed that the crystallinity of the zeolite was not affected by low metal loading，and the metal species were uniformly dispersed on the surface of zeolite.In the hydrogenation of furfural，Ni-based catalyst S-Ni2 showed excellent catalytic activity toward furfural transformation with 96% furfural conversion and 71% furan selectivity.Cu-based catalyst S-Cu1 showed extraordinary selectivity toward furfuryl alcohol（100%），which was much higher than that over Cu-based catalyst prepared by impregnation method（76%）.Therefore，compared with the impregnation method，one-step hydrothermal method could be used to obtain a catalyst with high selectivity，and the method wass also simple and easy to operate.This work would open up a new direction for developing highly efficient，stable，and low-cost hydrogenation catalysts，and promote the valorization of biomass.
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