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首页|期刊导航|高等学校化学学报|等级孔结构协同Fe改性提升ZSM-5分子筛催化苯甲醇烷基化性能

等级孔结构协同Fe改性提升ZSM-5分子筛催化苯甲醇烷基化性能OA北大核心CSTPCD

Synergistic Effects of Hierarchically Interconnected Porous Structure and Fe Modification on Zeolite ZSM-5 for Efficient Benzyl Alcohol Alkylation

中文摘要英文摘要

针对ZSM-5分子筛微孔扩散限制和催化活性位单一的问题,使用有序大孔-介孔碳模板为硬模板并结合原位引入金属策略,一步晶化合成了具有高结晶度、高比表面积的有序贯通大孔-介孔-微孔等级结构的Fe/ZSM-5分子筛单晶.通过X射线衍射(XRD)、紫外-可见光谱(UV-Vis)、H2程序升温还原实验(H2-TPR)和X射线光电子能谱(XPS)等手段对催化剂中活性Fe的存在形式进行了表征.结果表明,该材料中位于离子交换位及铁氧八面体(六配位)的孤立Fe(Ⅲ)是主要的氧化还原活性中心,当Fe负载量(质量分数)为1%时,苯甲醇转化率最高为59.3%,产物选择性为83.2%,最终收率达到49.3%,在循环使用5次后仍保持高催化活性.

Constructing hierarchically porous structures and embedding metal species into zeolite frameworks can effectively enable fast diffusion and synergistic catalysis.We report a one-step synthesis method to synthesize hierarchically macro-meso-microporous zeolite ZSM-5 single crystals containing Fe metal nanoclusters,that has advantages compared to multistep methods such as impregnation and ion exchange.Zeolite ZSM-5-Fe catalysts were prepared by steam assisted crystallization with addition of hierarchically porous carbon template and a Fe precursor.The catalyst was systematically characterized by means of X-ray diffraction(XRD),ultraviolet-visible spectroscopy indicated that the isolated Fe(Ⅲ)located at ion exchange sites and ferrite octahedron(six-coordinate)were the main redox-active centers.At a loading amount(mass fraction)of 1%,the highest benzyl alcohol conversion rate reached 59.3%,with a product selectivity of 83.2%,and a final yield of 49.3%.The catalyst maintained high catalytic activity even after five cycles,demonstrating its remarkable stability.

宋宇航;刘湛;吕佳敏;余申;李小云;孙明慧;陈丽华;苏宝连

武汉理工大学材料复合新技术国家重点实验室,武汉 430070武汉理工大学硅酸盐建筑材料国家重点实验室,武汉 430070武汉理工大学材料复合新技术国家重点实验室,武汉 430070||那慕尔大学无机材料化学实验室,那慕尔 B-5000,比利时

化学

ZSM-5分子筛等级结构过渡金属铁芳烃烷基化

ZSM-5 zeoliteHierarchical structureTransition metal FeAromatic alkylation

《高等学校化学学报》 2024 (005)

28-37 / 10

国家重点研发计划项目(批准号:2022YFB3504000)、国家自然科学基金(批准号:22302152,U20A20122,22293020,U22B6011)和中央高校基本科研业务费专项资金(批准号:2024IVA090)资助. Supported by the National Key Research and Development Program of China(No.2022YFB3504000),the National Natural Science Foundation of China(Nos.22302152,U20A20122,22293020,U22B6011)and the Fundamental Research Funds for the Central Universities,China(No.2024IVA090).

10.7503/cjcu20240095

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