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Recently, the Chinese Academy of Sciences Dalian Institute of Chemical Physics Catalytic Foundation National Key Laboratory Dundee Research Fellow and Baoxin and academician led the research team, in the long-term in-depth study of two-dimensional catalytic materials and nano-limit catalysis, found that graphene limit area of the single-atom iron center can be directly at room temperature conditions (25 degrees C) to convert methane catalysis into high value-added C1 oxygen compounds. The findings were published in Chemistry.
is a major component of natural gas, shale gas and combustible ice, and the conversion of methane into high-value-added fuels or chemicals is an urgent need of the world's energy economy
China
. However, methane is the most stable alkane molecule, with a high degree of tetular symmetry, its ionization energy is high, does not have electronic affinity, no permanent electrode moment and the polarization rate is low, its C-H bond bond can be as high as 434 KJ/mol, very difficult to be alive under mild conditions. Therefore, methane selection and conversion has always been a worldwide problem, in order to overcome the high reaction energy base, methane conversion often needs to be carried out at a high reaction temperature (600 to 1100 degrees C), how to reduce the reaction temperature, will be of great significance to its basic research and industrial applications.
Research team in the early study of two-dimensional catalytic materials under mild conditions of the active C-H bond, after up to 6 years of efforts, designed a series of graphene limit area of 3d transition metal center (manganese, iron, cobalt, nickel, copper) catalytic material, found that graphene limit area of monometallic center at room temperature, hydrogen peroxide as an oxidant, can directly convert methane catalysis into C1 oxygen compounds.
Using high-resolution liquid MRI spectrum and flight time mass spectrometry in-place characterization, the researchers found that the monolithic center of graphene limit can directly convert methane into C1 oxygen-containing compounds such as CH3OH, CH3OOH, HOCH2OOH and HCOOH. Further combined with the DFT theory calculation, it is found that the conversion of methane follows the reaction route of free agents, the in-place production of O-FeN4-O during the reaction process has high activity, methane can be converted to CH3OH and CH3OOH first through freelance, the resulting CH3OH will be further converted into HOCH2OOH and HCOOH.
experts believe that this work not only provides new ideas for the design of methane conversion high-efficiency catalysts under mild conditions, but also greatly encourages the development of methane catalytic conversion.
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