基于组氨酸配合物的钯催化剂的制备及2-戊基蒽醌加氢性能  

Preparation of Pd Catalysts with Histidine Coordination Complex and Their Catalytic Performances on 2-Amylanthraquinone Hydrogenation

作　　者：严华 杨晓野[1] 周俊宏 袁中山[1] 李德伏[1] 王树东[1] YAN Hua;YANG Xiaoye;ZHOU Junhong;YUAN Zhongshan;LI Defu;WANG Shudong(Dalian National Laboratory for Clean Energy,Dalian Institute of Chemical Physics,Chinese Academy of Sciences,Dalian 116023,Liaoning,China;University of Chinese Academy of Sciences,Beijing 100049,China)

机构地区：[1]中国科学院大连化学物理研究所,洁净能源国家实验室,辽宁大连116023 [2]中国科学院大学,北京100049

出　　处：《材料导报》2024年第12期267-272,共6页Materials Reports

基　　金：国家自然科学基金(21306184)。

摘　　要：双氧水是一种重要的现代化工原料,其生产工艺的关键是蒽醌加氢催化剂。以组氨酸配位Pd(NO3)2为前驱体,采用浸渍法制备了不同焙烧温度处理的Pd-his/SiO_(2)-T(his表示组氨酸,T为焙烧温度)系列催化剂,并评价了其催化2-戊基蒽醌的加氢反应性能,其中Pd-his/SiO_(2)-500的活性最高。作为对比,直接以Pd(NO3)2为前驱体制备了Pd/SiO_(2)-500催化剂。通过多种表征技术充分研究了催化剂的性质,结果表明,随着焙烧温度的升高,Pd-his/SiO_(2)-T系列催化剂的钯分散度在300~400℃时下降,在400~600℃时基本保持不变,并且所含残留碳成分逐渐减少,Pd0成分的占比和电子云密度上升。Pd-his/SiO_(2)-500相比Pd/SiO_(2)-500催化剂有更高的钯分散度,纳米颗粒更小,而且Pd0组分的电子云密度较高。评价实验表明,Pd-his/SiO_(2)-500的蒽醌加氢反应的加氢效率达到12.8 g/L,选择性为99.67%,活性比Pd/SiO_(2)-500高1.13倍。In order to improve the catalytic activity and selectivity of the catalyst for anthraquinone hydrogenation,a series of Pd-his/SiO_(2)-T(his represents histidine,and T is the calcination temperature)catalysts were prepared by impregnation method,with the coordination complex of Pd-(NO 3)2 and histidine as the precursor.The catalysts were prepared with SiO_(2) as the support through impregnation method under different calcination temperatures,and applied in anthraquinone hydrogenation reaction.For comparison,a Pd/SiO_(2)-500 catalyst free of histidine was prepared with the optimal calcination temperature,and other conditions were kept the same.The SiO_(2) support and all the catalysts were investigated by various characterization techniques in detail.It was found that,with the calcination temperature rising,the Pd dispersion of catalysts decreased during 300—400℃,however from 400℃to 600℃,the Pd dispersion nearly kept the same.The content of residual carbon species shrank,while the ratio of Pd 0 component and its electron cloud density increased.The evaluation of anthraquinone hydrogenation showed that the highest hydrogenation efficiency of the catalysts reached 12.8 g/L,which was 2.13 times as the Pd/SiO_(2)-500,and has a superior selectivity of 99.67%.

关 键 词：蒽醌加氢 钯 组氨酸 焙烧温度 分散度 

分 类 号：TQ426.63[化学工程] TQ123.6