有机化学 ›› 2024, Vol. 44 ›› Issue (10): 3223-3232.DOI: 10.6023/cjoc202406017 上一篇    下一篇

研究论文

纳米花状Ir/MoS2催化剂用于CO2加氢高选择性制备甲酸盐

何君a, 王红星a,*(), 余成龙b,c, 张艳茹b,c, 王莹b, 王燕燕b,c, 张龙博b,c, 郭佳b,c, 钱庆利b,c,*(), 韩布兴b,c,d,*()   

  1. a 天津科技大学化工与材料学院 天津 300457
    b 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
    c 中国科学院大学化学科学学院 北京 100049
    d 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
  • 收稿日期:2024-06-12 修回日期:2024-07-29 发布日期:2024-08-30
  • 基金资助:
    国家自然科学基金(22033009); 国家自然科学基金(22293015); 国家自然科学基金(22072156); 国家自然科学基金(22073104); 国家自然科学基金(22121002); 国家重点研发计划(2022YFA1504904)

Nanoflower-Shaped Ir/MoS2 Catalyst for Highly Selective Production of Formate by CO2 Hydrogenation

Jun Hea, Hongxing Wanga,*(), Chenglong Yub,c, Yanru Zhangb,c, Ying Wangb, Yanyan Wangb,c, Longbo Zhangb,c, Jia Guob,c, Qingli Qianb,c,*(), Buxing Hanb,c,d,*()   

  1. a College of Chemical Engineering and Materials Science, Tianjin University of Science and Technology, Tianjin 300457
    b 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
    d 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
  • Received:2024-06-12 Revised:2024-07-29 Published:2024-08-30
  • Contact: *E-mail: wanghx@tust.edu.cn;qianql@iccas.ac.cn;hanbx@iccas.ac.cn
  • Supported by:
    National Science Foundation of China(22033009); National Science Foundation of China(22293015); National Science Foundation of China(22072156); National Science Foundation of China(22073104); National Science Foundation of China(22121002); National Key Research and Development Program of China(2022YFA1504904)

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/MoS2催化剂, 探究其在CO2加氢反应中的催化活性. Ir/MoS2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MoS2局部结构发生相变. 在较低的反应压力下, 1% Ir/MoS2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/MoS2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CO2加氢合成甲酸/甲酸盐催化剂提供了一条新的途径.

关键词: CO2加氢, 甲酸/甲酸盐, 纳米花, 催化剂, Ir/MoS2

A series of nanoflower-shaped X% Ir/MoS2 catalysts with different Ir loadings were prepared based on a simple hydrothermal synthesis method and their catalytic activities in CO2 hydrogenation were investigated. The Ir/MoS2 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 MoS2. Under low reaction pressure, the 1% Ir/MoS2 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/MoS2 catalyst also showed excellent catalytic stability, and the catalytic activity did not decrease obviously after being reused three times. Based on control experiments, the catalytic mechanism and solvent effect were also studied and discussed. This study provid es a new way for developing high-performance catalysts for CO2 hydrogenation to formate.

Key words: CO2 hydrogenation, formate, nanoflower, catalyst, Ir/MoS2