表面硅烷功能化钨钼复合金属氧化物高效选择性加氢催化剂性能研究  

Study on the Performance of Highly Efficient Selective Hydrogenation Catalysts of Surface Silane-Functionalized Tungsten-Molybdenum Composite Metal Oxides

作　　者：胡银[1] 曾艳红 徐豪章 陈伟 王玲玲 陈玄烨 章芬 韩飞 奚国安 林城杰 邵伟 HU Yin;ZENG Yanhong;XU Haozhang;CHEN Wei;WANG Lingling;CHEN Xuanye;ZHANG Fen;HANFei;XI Guoan;LIN Chengjie;SHAO Wei(Institute of Applied Chemistry,Jiangxi Academy of Sciences,Nanchang 330096,China;School of Environment and Chemical Engineering,Nanchang Hangkong University,Nanchang 330063,China;Institute of Energy Research,Jiangxi Academy of Sciences,Nanchang 330096,China)

机构地区：[1]江西省科学院应用化学研究所,江西南昌330096 [2]南昌航空大学环境与化学工程学院,江西南昌330063 [3]江西省科学院能源研究所,江西南昌330096

出　　处：《生物化工》2025年第1期1-5,18,共6页Biological Chemical Engineering

基　　金：国家自然科学基金地区基金项目(22062009,22262014);江西省“双千计划”培养类科技创新高端人才(青年)项目(jxsq2023201088);环境与能源催化江西省重点实验室(2024SSY05132);江西省科学院重大产业技术攻关专项(2022YSBG10003);江西省科学院省级人才培育计划项目(2022YRCS004);江西省科学院基础研究项目(2022YJC1001,2023YJC1002)。

摘　　要：温和条件下高效加氢催化剂的开发,一直是精细化学品人工合成研究领域的热点。催化材料的理性设计及性能优化技术多种多样,根据目标催化反应特点可控构筑具有独特性质的催化剂结构可事半功倍。本工作针对α-蒎烯和苯甲酸选择性催化加氢反应,设计硅烷修饰钨钼复合金属氧化物紧密连接表面贵金属活性位点的特殊催化剂结构,同时利用硅烷特性引入表面疏水结构,制备了系列金属/有机硅烷/W_(x)Mo_(y)O_(z)高选择性复合催化剂,其中Ru/APTS/W_(0.4)Mo_(0.6)O_(3)、Rh/TEOS/W_(0.4)Mo_(0.6)O_(3)和Ru/TEOS/W_(0.4)Mo_(0.6)O_(3)分别对苯甲酸和α-蒎烯表现出优异的催化加氢性能。钨钼复合金属氧化物独特的结构和性质、表面硅烷修饰促进金属-载体紧密连接,及其提供的丰富活性基团、形成表面疏水结构等效应协同作用,显著改善催化剂加氢性能。本工作对通过调控材料组分和表面亲疏水结构,可控构筑低温低压下高选择性加氢催化剂的研究有一定的借鉴作用。The development of highly efficient hydrogenation catalysts under mild conditions has always been a hot topic in the research field of artificial synthesis of fine chemicals.There are various techniques for the rational design and performance optimization of catalytic materials.If the controllable construction of catalyst structures with unique properties is according to the characteristics of the target catalytic reaction,it would achieve twice the result with half the effort.This work focuses on the selective catalytic hydrogenation ofα-pinene and benzoic acid.A special catalyst structure is designed with tungsten-molybdenum composite metal oxide modified by silane tightly connected to noble metal active sites on the surface.Meanwhile,the surface hydrophobic structures is also introduced to the catalyst utilizing the characteristics of silane.Thus,a series of metal/organosilane/W_(x)Mo_(y)O_(z)composite catalysts with high hydrogenation selectivity are prepared.Among them,Ru/APTS/W_(0.4)Mo_(0.6)O_(3),Rh/TEOS/W_(0.4)Mo_(0.6)O_(3) and Ru/TEOS/W_(0.4)Mo_(0.6)O_(3) show excellent catalytic performance for the hydrogenation of benzoic acid andα-pinene,respectively.The synergistic effects of the unique structure and properties of tungsten-molybdenum composite metal oxides,and the surface silane modification promoting tight connection between metal and support,providing abundant active groups and forming surface hydrophobic structures significantly improve the hydrogenation performance of catalysts.This work has certain reference value for the study on controllable construction of hydrogenation catalysts with high selectivity under low temperature and low pressure by regulating material composition and surface amphipathic structure.

关 键 词：钨钼氧化物 硅烷修饰 亲疏水 负载型复合催化剂 选择性加氢 

分 类 号：O643.36[理学—物理化学]