Liquid phase hydrogenation of CO2 to formate using palladium and ruthenium nanoparticles supported on molybdenum carbide

被引:22
|
作者
Mitchell, Claire E. [1 ]
Terranova, Umberto [1 ]
Alshibane, Ihfaf [2 ]
Morgan, David J. [1 ]
Davies, Thomas E. [1 ]
He, Qian [1 ]
Hargreaves, Justin S. J. [2 ]
Sankar, Meenakshisundaram [1 ]
de Leeuw, Nora H. [1 ]
机构
[1] Cardiff Univ, Sch Chem, Cardiff Catalysis Inst, Cardiff CF10 4AT, S Glam, Wales
[2] Glasgow Univ, Sch Chem, Glasgow G12 8QQ, Lanark, Scotland
基金
英国工程与自然科学研究理事会;
关键词
CARBON-DIOXIDE HYDROGENATION; FORMIC-ACID; MOLECULAR-HYDROGEN; CATALYTIC-HYDROGENATION; BIMETALLIC CATALYSTS; METHANOL SYNTHESIS; ROOM-TEMPERATURE; WATER; ENERGY; ADSORPTION;
D O I
10.1039/c9nj02114k
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
We report the development of palladium nanoparticles supported on Mo2C as an active catalyst for the liquid-phase hydrogenation of CO2 to formate under mild reaction conditions (100 degrees C and 2.0 MPa of a 1 : 1 CO2 : H-2 mixture). A series of Pd/Mo2C catalysts were synthesised via the modified wet-impregnation (MIm) and sol-immobilization (SIm) techniques and evaluated for CO2 hydrogenation, in an aqueous 1 M NaOH solution. MIm catalysts synthesised using PdCl2 dissolved in a 2 M HCl solution gave the highest formate yield with turnover numbers of up to 109 after 19 h. We further report the crucial role of base and the pH of the reaction medium for the hydrogenation of CO2 to formate. Based on stability studies, electron microscopic characterisation and density functional theory calculations we found that Ru has a stronger affinity than Pd to Mo2C resulting in the development of a stable bimetallic RuPd/Mo2C catalyst for the hydrogenation of CO2 to formate.
引用
收藏
页码:13985 / 13997
页数:13
相关论文
共 50 条
  • [41] Direct synthesis of ethanol via CO2 hydrogenation using supported gold catalysts
    Wang, Dong
    Bi, Qingyuan
    Yin, Guoheng
    Zhao, Wenli
    Huang, Fuqiang
    Xie, Xiaoming
    Jiang, Mianheng
    CHEMICAL COMMUNICATIONS, 2016, 52 (99) : 14226 - 14229
  • [42] Homogeneous Hydrogenation of CO2 to Methyl Formate Utilizing Switchable Ionic Liquids
    Yadav, Mahendra
    Linehan, John C.
    Karkamkar, Abhijeet J.
    van der Eide, Edwin
    Heldebrant, David. J.
    INORGANIC CHEMISTRY, 2014, 53 (18) : 9849 - 9854
  • [43] Hollow Mesoporous Organosilica Spheres Encapsulating PdAg Nanoparticles and Poly(Ethyleneimine) as Reusable Catalysts for CO2 Hydrogenation to Formate
    Kuwahara, Yasutaka
    Fujie, Yuki
    Mihogi, Takashi
    Yamashita, Hiromi
    ACS CATALYSIS, 2020, 10 (11) : 6356 - 6366
  • [44] Iron catalyzed CO2 hydrogenation to formate enhanced by Lewis acid co-catalysts
    Zhang, Yuanyuan
    MacIntosh, Alex D.
    Wong, Janice L.
    Bielinski, Elizabeth A.
    Williard, Paul G.
    Mercado, Brandon Q.
    Hazari, Nilay
    Bernskoetter, Wesley H.
    CHEMICAL SCIENCE, 2015, 6 (07) : 4291 - 4299
  • [45] Electrochemical Reduction of CO2 to Formate on Easily Prepared Carbon-Supported Bi Nanoparticles
    Avila-Bolivar, Beatriz
    Garcia-Cruz, Leticia
    Montiel, Vicente
    Solla-Gullon, Jose
    MOLECULES, 2019, 24 (11):
  • [46] Selective Hydrogenation of CO2 to Formic Acid over Alumina-Supported Ru Nanoparticles with Multifunctional Ionic Liquid
    Prashant Gautam
    Praveenkumar Ramprakash Upadhyay
    Vivek Srivastava
    Catalysis Letters, 2019, 149 : 1464 - 1475
  • [47] Selective Hydrogenation of CO2 to Formic Acid over Alumina-Supported Ru Nanoparticles with Multifunctional Ionic Liquid
    Gautam, Prashant
    Upadhyay, Praveenkumar Ramprakash
    Srivastava, Vivek
    CATALYSIS LETTERS, 2019, 149 (06) : 1464 - 1475
  • [48] An In Situ Infrared Study of CO2 Hydrogenation to Formic Acid by Using Rhodium Supported on Titanate Nanotubes as Catalysts
    Roberto Ruiz-Garcia, Jesus
    Carlos Fierro-Gonzalez, Juan
    Handy, Brent E.
    Hinojosa-Reyes, Laura
    De Haro Del Rio, David A.
    Lucio-Ortiz, Carlos J.
    Valle-Cervantes, Sergio
    Flores-Escamilla, Gerardo A.
    CHEMISTRYSELECT, 2019, 4 (14): : 4206 - 4216
  • [49] Enhanced selective hydrogenation of CO2 to CH4 on molybdenum carbide hollow sphere catalyst
    Men, Yu-Long
    Liu, Peng
    Cheng, Dang-Guo
    Peng, Chong
    Zhao, Yiyi
    Pan, Yun-Xiang
    AICHE JOURNAL, 2024, 70 (11)
  • [50] Hydrogenation of CO2 to formic acid over efficient heterogeneous ruthenium oxide supported on cubic phase zirconium oxide catalyst
    Bankar, Balasaheb D.
    Naikwadi, Dhanaji R.
    Biradar, Ankush, V
    APPLIED SURFACE SCIENCE, 2023, 631