原子层沉积构筑Pd/TiO_(2)限域催化剂及其在1,4-丁炔二醇加氢的应用  

Confined Pd/TiO_(2) Catalyst Constructed by ALD for the Hydrogenation of 1,4-Butynediol

作　　者：张淑芳 杨高举 褚盼楠 张斌[2] 赵永祥[1] ZHANG Shu-fang;YANG Gao-ju;CHU Pan-nan;ZHANG Bin;ZHAO Yong-xiang(Engineering Research Center of Ministry of Education for Fine Chemicals,Shanxi University,Taiyuan 030006,China;State Key Laboratory of Coal Conversion,Institute of Coal Chemistry,Chinese Academy of Sciences,Taiyuan 030001,China)

机构地区：[1]山西大学化学化工学院精细化学品工程研究中心,山西太原030006 [2]中国科学院山西煤炭化学研究所煤转化国家重点实验室,山西太原030001

出　　处：《分子催化》2023年第4期348-355,I0001,I0002,共10页Journal of Molecular Catalysis(China)

基　　金：国家自然科学科学基金青年项目(No.22005181);山西省应用基础研究计划,面上青年基金项目(No.201901D211156)。

摘　　要：利用ALD制备了TiO_(2)限域的Pd催化剂,研究了限域空间内Pd纳米颗粒与TiO_(2)的界面作用对1,4-丁炔二醇(BYD)加氢性能的影响.相比于管外负载型催化剂,限域催化剂在催化1,4-丁炔二醇选择性加氢反应中体现出非常高的催化活性和1,4-丁烯二醇的选择性.HR-TEM、EDX-Mapping、XRD、XPS和H2-TPR表征说明,限域体系中Pd-TiO_(2)的界面相互作用强于传统TiO_(2)表面负载型Pd催化剂,这种强界面作用不仅能够提高BYD的加氢活性,也可抑制半加氢产物1,4-丁烯二醇的异构化和深度加氢,提高1,4-丁烯二醇的选择性,而且限域结构也可阻止管内壁Pd纳米颗粒的脱落,提高催化剂的稳定性.A series of TiO_(2) confined Pd catalysts were prepared by ALD,and the effect of the interfacial interaction between Pd and TiO_(2) on the selective hydrogenation of 1,4-butynediol(BYD)was studied.Compared with TiO_(2) supported Pd catalysts,Pd catalysts confined in TiO_(2) exhibit more highly efficient catalytic activity and selectivity for 1,4-butenediol in the hydrogenation of 1,4-butynediol.The phase structure and electronic properties of catalysts were characterized by HR-TEM,XRD and XPS,and the results showed that stronger Pd-TiO_(2)interaction exited in the confined catalysts.The stronger Pd-TiO_(2) interaction can efficiently inhibit the isomerization and deep hydrogenation of 1,4-butenediol,thus improving the selectivity of 1,4-butenediol.Moreover,the leaching of Pd nanoparticles in the confined catalysts can also be prevented,and the stability of catalysts was improved.

关 键 词：原子层沉积 限域结构 Pd-催化剂 界面相互作用 1 4-丁炔二醇加氢 

分 类 号：O643.3[理学—物理化学]