A promising low pressure methanol synthesis route from CO2 hydrogenation over Pd@Zn core-shell catalysts

被引:85
|
作者
Liao, Fenglin [1 ]
Wu, Xin-Ping [2 ,3 ]
Zheng, Jianwei [4 ]
Li, Molly Meng-Jung [1 ]
Kroner, Anna [5 ]
Zeng, Ziyan [6 ]
Hong, Xinlin [6 ]
Yuan, Youzhu [4 ]
Gong, Xue-Qing [2 ,3 ]
Tsang, Shik Chi Edman [1 ]
机构
[1] Univ Oxford, Dept Chem, Wolfson Catalysis Ctr, Oxford OX1 3QR, England
[2] East China Univ Sci & Technol, Coll Chem & Mol Engn, Ctr Computat Chem, Key Lab Adv Mat, Shanghai 200237, Peoples R China
[3] East China Univ Sci & Technol, Coll Chem & Mol Engn, Res Inst Ind Catalysis, Shanghai 200237, Peoples R China
[4] Xiamen Univ, Coll Chem & Chem Engn, State Key Lab Phys Chem Solid Surfaces,iChEM, Natl Engn Lab Green Chem Prod Alcohols Ethers Est, Xiamen 361005, Peoples R China
[5] Diamond Light Source Ltd, Harwell Sci & Innovat, Didcot OX11 0DE, Oxon, England
[6] Wuhan Univ, Dept Chem, Wuhan 430072, Peoples R China
基金
英国工程与自然科学研究理事会;
关键词
ELASTIC BAND METHOD; HYDROCARBONS; TRANSITION;
D O I
10.1039/c6gc02366e
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
At present, there is no low pressure methanol synthesis from CO2/H-2 with high yield despite the presence of an upstream process of aqueous phase reforming (APR) of biomass derivatives on an industrial scale for CO2/H-2 production at ca. 2 MPa. This is due to the intrinsic thermodynamics of the system which leads to particularly high CO levels at low pressure through reversed water gas shift reaction (RWGS) for most studied catalysts. Here we report a new Pd@Zn core-shell catalyst that offers a significantly higher kinetic barrier to CO/H2O formation in CO2 hydrogenation to reduce the CO levels but facilitates CH3OH formation at or below 2 MPa with CH3OH selectivity maintained at ca. 70% compared to ca. 10% over industrial Cu catalysts. The corresponding methanol yield at 2 MPa reaches 6.1 gmethanol gactive metal(-1) h(-1), which is comparable to the best reported value among a wide variety of catalysts under 5 MPa. It is thus believed that this active Pd based catalyst opens up a promising possibility for low pressure and temperature methanol production using a renewable biomass resource for fossil-fuel-starved countries.
引用
收藏
页码:270 / 280
页数:11
相关论文
共 50 条
  • [1] Pd@Zn core-shell nanoparticles of controllable shell thickness for catalytic methanol production
    Liao, Fenglin
    Wu, Xin-Ping
    Zheng, Jianwei
    Li, Meng-Jung
    Zeng, Ziyan
    Hong, Xinling
    Kroner, Anna
    Yuan, Youzhu
    Gong, Xue-Qing
    Tsang, Shik Chi Edman
    [J]. CATALYSIS SCIENCE & TECHNOLOGY, 2016, 6 (21) : 7698 - 7702
  • [2] CO2 hydrogenation over Pd-modified methanol synthesis catalysts
    Melian-Cabrera, I
    Granados, ML
    Terreros, P
    Fierro, JLG
    [J]. CATALYSIS TODAY, 1998, 45 (1-4) : 251 - 256
  • [3] First-principles investigation of methanol synthesis from CO2 hydrogenation on Cu@Pd core-shell surface
    Liu, Jiangshan
    Ke, Qiang
    Chen, Xin
    [J]. JOURNAL OF MATERIALS SCIENCE, 2021, 56 (05) : 3790 - 3803
  • [4] Core-shell silica@CuxZnAl LDH catalysts for efficient CO2 hydrogenation to methanol
    Lyu, Meng
    Zheng, Jianwei
    Coulthard, Claire
    Ren, Jing
    Zhao, Yufei
    Tsang, Shik Chi Edman
    Chen, Chunping
    O'Hare, Dermot
    [J]. CHEMICAL SCIENCE, 2023, 14 (36) : 9814 - 9819
  • [5] Methanol synthesis from CO2 under atmospheric pressure over supported Pd catalysts
    Iwasa, N
    Suzuki, H
    Terashita, M
    Arai, M
    Takezawa, N
    [J]. CATALYSIS LETTERS, 2004, 96 (1-2) : 75 - 78
  • [6] Methanol Synthesis from CO2 Under Atmospheric Pressure over Supported Pd Catalysts
    Nobuhiro Iwasa
    Hiroshi Suzuki
    Masao Terashita
    Masahiko Arai
    Nobutsune Takezawa
    [J]. Catalysis Letters, 2004, 96 : 75 - 78
  • [7] Methanol synthesis from CO2 hydrogenation over copper based catalysts
    Ahouari, Hania
    Soualah, Ahcene
    Le Valant, Anthony
    Pinard, Ludovic
    Magnoux, Patrick
    Pouilloux, Yannick
    [J]. REACTION KINETICS MECHANISMS AND CATALYSIS, 2013, 110 (01) : 131 - 145
  • [8] Methanol synthesis from CO2 hydrogenation over copper based catalysts
    Hania Ahouari
    Ahcène Soualah
    Anthony Le Valant
    Ludovic Pinard
    Patrick Magnoux
    Yannick Pouilloux
    [J]. Reaction Kinetics, Mechanisms and Catalysis, 2013, 110 : 131 - 145
  • [9] Intermetallic Pd-In catalysts for methanol synthesis by CO2 hydrogenation
    A. V. Rassolov
    G. N. Baeva
    A. R. Kolyadenkov
    P. V. Markov
    A. Yu. Stakheev
    [J]. Russian Chemical Bulletin, 2023, 72 : 2583 - 2590
  • [10] Intermetallic Pd-In catalysts for methanol synthesis by CO2 hydrogenation
    Rassolov, A. V.
    Baeva, G. N.
    Kolyadenkov, A. R.
    Markov, P. V.
    Stakheev, A. Yu.
    [J]. RUSSIAN CHEMICAL BULLETIN, 2023, 72 (11) : 2583 - 2590