纳米花状Ir/MoS_(2)催化剂用于CO_(2)加氢高选择性制备甲酸盐  

Nanoflower-Shaped Ir/MoS_(2) Catalyst for Highly Selective Production of Formate by CO_(2) Hydrogenation

作　　者：何君 王红星 余成龙 张艳茹 王莹[2] 王燕燕 张龙博 郭佳 钱庆利 韩布兴[2,3,4] He Jun;Wang Hongxing;Yu Chenglong;Zhang Yanru;Wang Ying;Wang Yanyan;Zhang Longbo;Guo Jia;Qian Qingli;Han Buxing(College of Chemical Engineering and Materials Science,Tianjin University of Science and Technology,Tianjin 300457;Laboratory of Colloid and Interface and Thermodynamics,Institute of Chemistry,Chinese Academy of Sciences,Beijing 100190;c School of Chemical Sciences,University of Chinese Academy of Sciences,Beijing 100049;Shanghai Key Laboratory of Green Chemistry and Chemical Processes,State Key Laboratory of Petroleum Molecular and Process Engineering,School of Chemistry and Molecular Engineering,East China Normal University,Shanghai 200062)

机构地区：[1]天津科技大学化工与材料学院,天津300457 [2]中国科学院化学研究所胶体、界面与化学热力学实验室,北京100190 [3]中国科学院大学化学科学学院,北京100049 [4]华东师范大学化学与分子工程学院石油分子与过程工程国家重点实验室、上海市绿色化学与化工过程重点实验室,上海200062

出　　处：《有机化学》2024年第10期3223-3232,共10页Chinese Journal of Organic Chemistry

基　　金：国家自然科学基金(Nos.22033009,22293015,22072156,22073104,22121002);国家重点研发计划(No.2022YFA1504904)资助项目。

摘　　要：基于简单的水热合成法制备了一系列不同Ir负载量的纳米花状的X%Ir/MoS_(2)催化剂,探究其在CO_(2)加氢反应中的催化活性.Ir/MoS_(2)催化剂呈现出纳米花状的形貌,直径大约为800 nm,纳米花上的二维纳米片分布良好,这有利于活性位点的充分暴露.Ir的掺杂有效地调整了催化剂的电子结构,能够使MoS_(2)局部结构发生相变.在较低的反应压力下,1%Ir/MoS_(2)催化剂表现出了最高的甲酸盐选择性(98%)和活性(8.6 mmol•g^(-1)•h^(-1)),但是过量Ir的负载会导致Ir纳米颗粒发生团聚,降低了产物的选择性和活性.1%Ir/MoS_(2)催化剂还表现出优异的催化稳定性,在重复使用3次后催化活性没有显著降低.还通过控制实验对催化机理和反应的溶剂效应进行了研究和讨论.本研究为开发高性能的CO_(2)加氢合成甲酸/甲酸盐催化剂提供了一条新的途径.A series of nanoflower-shaped X%Ir/MoS_(2) catalysts with different Ir loadings were prepared based on a simple hydrothermal synthesis method and their catalytic activities in CO_(2)hydrogenation were investigated.The Ir/MoS_(2) catalyst has a nanoflower-like shape with a diameter of about 800 nm.The layers of two-dimensional nanosheets on the catalyst were well dispersed,which increased the exposure of the active sites.The doping of Ir could effectively tune the electronic structure of the catalyst,causing the local structure phase change of MoS_(2).Under low reaction pressure,the 1%Ir/MoS_(2) composite showed the highest formate selectivity(98%)and activity(8.6 mmol•g^(-1)•h^(-1)).The excessive Ir loading would lead to the agglomeration of Ir to form nanoparticles,which reduced the selectivity and activity of product.The 1%Ir/MoS_(2) catalyst also showed excellent catalytic stability,and the catalytic activity did not decrease obviously after being reused three times.Based o n control experiments,the catalytic mechanism and solvent effect were also studied and discussed.This study provides a new way for developing high-performance catalysts for CO_(2) hydrogenation to formate.

关 键 词：CO_(2)加氢 甲酸/甲酸盐 纳米花 催化剂 Ir/MoS_(2) 

分 类 号：TQ225.21[化学工程—有机化工] O643.36[理学—物理化学] X701[理学—化学]