Synergistic Effects of Silica-Supported Iron-Cobalt Catalysts for CO2 Reduction to Prebiotic Organics

被引:5
|
作者
Belthle, Kendra S. [1 ]
Martin, William F. [2 ]
Tueysuez, Harun [1 ]
机构
[1] Max Planck Inst Kohlenforsch, Kaiser Wilhelm Pl 1, D-45470 Mulheim An Der Ruhr, Germany
[2] Univ Dusseldorf, Inst Mol Evolut, Univ Str 1, D-40225 Dusseldorf, Germany
基金
欧洲研究理事会;
关键词
Heterogeneous catalysis; Prebiotic Chemistry; Hydrothermal Vent; CO2; Fixation; CoFe Alloy; FISCHER-TROPSCH; CARBON-DIOXIDE; BIMETALLIC CATALYSTS; SELECTIVE HYDROGENATION; HETEROGENEOUS CATALYSTS; FIXATION; ORIGIN; FLUIDS; FIELD; GEOCHEMISTRY;
D O I
10.1002/cctc.202301218
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
To test the ability of geochemical surfaces in serpentinizing hydrothermal systems to catalyze reactions from which metabolism arose, we investigated H-2-dependent CO2 reduction toward metabolic intermediates over silica-supported Co-Fe catalysts. Supported catalysts converted CO2 to various products at 180 degrees C and 2.0 MPa. The liquid product phase included formate, acetate, and ethanol, while the gaseous product phase consisted of CH4, CO, methanol, and C-2-C-7 linear hydrocarbons. The 1/1 ratio CoFe alloy with the same composition as the natural mineral wairauite yielded the highest concentrations of formate (6.0 mM) and acetate (0.8 mM), which are key intermediates in the acetyl-coenzyme A (acetyl-CoA) pathway of CO2 fixation. While Co-rich catalysts were proficient at hydrogenation, yielding mostly CH4, Fe-rich catalysts favored the formation of CO and methanol. Mechanistic studies indicated intermediate hydrogenation and C-C coupling activities of alloyed CoFe, in contrast to physical mixtures of both metals. Co in the active site of Co-Fe catalysts performed a similar reaction as tetrapyrrole-coordinated Co in the corrinoid iron-sulfur (CoFeS) methyl transferase in the acetyl-CoA pathway. In a temperature range characteristic for deeper regions of serpentinizing systems, oxygenate product formation was favored at lower, more biocompatible temperatures.
引用
收藏
页数:12
相关论文
共 50 条
  • [41] Silica-supported polymeric amines as CO2 adsorbents and catalyst supports
    Jones, Christopher W.
    ABSTRACTS OF PAPERS OF THE AMERICAN CHEMICAL SOCIETY, 2014, 247
  • [42] NO reduction with CO on alumina-modified silica-supported palladium and molybdenum-palladium catalysts
    Diaz Consul, Julia Maria
    Costilla, Ignacio
    Gigola, Carlos Eugenio
    Baibich, Ione Maluf
    APPLIED CATALYSIS A-GENERAL, 2008, 339 (02) : 151 - 158
  • [43] CO2 HYDROGENATION FOR C-2+ ALCOHOLS SYNTHESIS OVER SILICA-SUPPORTED IR-MO CATALYSTS
    KISHIDA, M
    YAMADA, K
    NAGATA, H
    WAKABAYASHI, K
    CHEMISTRY LETTERS, 1994, (03) : 555 - 556
  • [44] Reforming Methane with CO2 over Hierarchical Porous Silica-Supported Nickel Catalysts Modified with Lanthanum Oxide
    Li, Bin
    Yuan, Xiaoqing
    Li, Lvyin
    Li, Baitao
    Wang, Xiujun
    INTERNATIONAL JOURNAL OF ENERGY RESEARCH, 2023, 2023
  • [45] Chemistry of Silica-Supported Cobalt Catalysts Prepared by Cation Adsorption. 2. Neoformation of Cobalt Phyllosilicate
    Trujillano, Raquel
    Lambert, Jean-Francois
    Louis, Catherine
    JOURNAL OF PHYSICAL CHEMISTRY C, 2008, 112 (47): : 18551 - 18558
  • [46] The difference of roles of alkaline-earth metal oxides on silica-supported nickel catalysts for CO2 methanation
    Guo, Meng
    Lu, Gongxuan
    RSC ADVANCES, 2014, 4 (102) : 58171 - 58177
  • [47] Reduction of cobalt and iron corroles and catalyzed reduction of CO2
    Grodkowski, J
    Neta, P
    Fujita, E
    Mahammed, A
    Simkhovich, L
    Gross, Z
    JOURNAL OF PHYSICAL CHEMISTRY A, 2002, 106 (18): : 4772 - 4778
  • [48] Enhanced CO2 Conversion to CO by Silica-Supported Perovskite Oxides at Low Temperatures
    Hare, Bryan. J.
    Maiti, Debtanu
    Daza, Yolanda A.
    Bhethanabotla, Venkat R.
    Kuhn, John N.
    ACS CATALYSIS, 2018, 8 (04): : 3021 - 3029
  • [49] Nickel catalysts supported on silica microspheres for CO2 methanation
    Gac, Wojciech
    Zawadzki, Witold
    Slowik, Grzegorz
    Sienkiewicz, Andrzej
    Kierys, Agnieszka
    MICROPOROUS AND MESOPOROUS MATERIALS, 2018, 272 : 79 - 91
  • [50] SYNTHESIS OF HYDROCARBONS FROM CO AND H-2 ON SIO(2) SUPPORTED IRON-COBALT CLUSTERS
    KOVALCHUK, VI
    KUZNETSOV, BN
    MIKOVA, NM
    EFREMOV, AA
    BAKHMUTOVA, NI
    RUSSIAN CHEMICAL BULLETIN, 1993, 42 (06) : 1032 - 1038