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    Home > Research team led by Deng Dehui, researcher of Dalian Institute of chemistry, Chinese Academy of Sciences and Bao Xin and academician to realize direct catalytic conversion of methane at room temperature

    Research team led by Deng Dehui, researcher of Dalian Institute of chemistry, Chinese Academy of Sciences and Bao Xin and academician to realize direct catalytic conversion of methane at room temperature

    • Last Update: 2018-08-30
    • Source: Internet
    • Author: User
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    Recently, a research team led by Deng Dehui, researcher and Bao Xin, academician of the State Key Laboratory of catalysis foundation of Dalian Institute of Chemical Sciences, has found that the graphene bound monatomic iron center can directly convert methane to high value-added C1 oxygenates at room temperature (25 ° C) on the basis of a long-term in-depth study of two-dimensional catalytic materials and nano confinement catalysis The results were published in full in chem (DOI: 10.1016 / j.champr 2018.05.006) Methane is the main component of natural gas, shale gas and combustible ice The conversion of methane into high value-added fuel or chemicals is an urgent need of the world energy economy However, methane is the most stable alkane molecule with high tetrahedral symmetry, high ionization energy, no electron affinity, no permanent electric dipole moment and low polarizability The bond energy of C-H bond is as high as 434 kJ / mol, which is very difficult to be activated under mild conditions Therefore, the selective activation and directional conversion of methane has been a worldwide problem, which is known as the "Holy Grail" research topic in the field of chemistry In order to overcome the high reaction energy barrier, the conversion of methane often needs to be carried out at a high reaction temperature (600-1100 ° C) How to reduce the reaction temperature will be of great significance to its basic research and industrial application Although many researchers have done a lot of exploration, it is still very challenging to directly convert methane into high additional fuel or chemicals under mild conditions, especially at room temperature, without introducing any other forms of energy such as light, electricity, plasma and so on The team previously studied the activation of C-H bonds in two-dimensional catalytic materials under mild conditions (sci.adv 201 5, 1, e1500462; nat.commun 2018, 9, On the basis of 1181), a series of transition metal centers (Mn, Fe, Co, Ni, Cu) with graphene confinement were designed after six years' efforts It was found that the single iron centers with graphene confinement can directly convert methane to C1 oxygenates at room temperature with hydrogen peroxide as oxidant In cooperation with Han Xiuwen, Li Haiyang and other researchers, the team found that the graphene confined single iron center can directly convert methane into C1 oxygenates such as CH3OH, CH3OOH, hoch2ooh and HCOOH by means of high-resolution liquid NMR and in-situ characterization of time-of-flight mass spectrometry Furthermore, DFT calculation shows that the conversion of methane follows the reaction route of free radicals, and o-fen4-o generated in situ has high activity Methane can be converted into CH3OH and CH3OOH through free radicals first, and the CH3OH generated will be further converted into hoch2ooh and HCOOH The publication of the work has attracted wide attention The website of Chemistry World of Royal Society of chemistry reported the work with the title of "catalyst conversions measure to measure at room temperature" At the same time, Professor Wang Ye of Xiamen University introduced this work in the Journal of Joule with the title of "room temperature conversion of measure becomes true" He evaluated the work as "a significant breakthrough in metal chemistry" This work not only provides a new idea for the design of high efficiency catalyst for methane conversion under mild conditions, but also greatly encourages the development of the field of methane conversion The above research has been supported by the key R & D plan of the Ministry of science and technology of the people's Republic of China, the National Natural Science Foundation of the people's Republic of China, the key research project of Frontier Science of the Chinese Academy of Sciences, the special project of strategic leading science and technology of the Chinese Academy of Sciences, the collaborative innovation center of energy, materials and chemistry of the Ministry of Education (2011 · I Chem) and the postdoctoral innovation talent support plan.
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