Room-temperature conversion of ethane and the mechanism understanding over single iron atoms confined in graphene

Abstract(#br)The catalytic conversion of ethane to high value-added chemicals is significantly important for utilization of hydrocarbon resources. However, it is a great challenge due to the typically required high temperature (> 400 °C) conditions. Herein, a highly active catalytic conversion process of ethane at room temperature (25 °C) is reported on single iron atoms confined in graphene via the porphyrin-like N 4 -coordination structures. Combining with the operando time of flight mass spectrometer and density functional theory calculations, the reaction is identified as a radical mechanism, in which the C–H bonds of the same C atom are preferentially and sequentially activated, generating the value-added C 2 chemicals, simultaneously avoiding the over-oxidation of the products to CO 2 . The in-situ formed O–FeN 4 –O structure at the single iron atom serves as the active center for the reaction and facilitates the formation of ethyl radicals. This work deepens the understanding of alkane C–H activation on the FeN 4 center and provides the reference in development of efficient catalyst for selective oxidation of light alkane

Direct Methane Conversion under Mild Condition by Thermo-, Electro-, or Photocatalysis

Direct conversion of earth-abundant methane into value-added chemicals under mild conditions is an attractive technology in response to the increasing industrial demand of feedstocks and worldwide appeal of energy conservation. Exploring advanced low-temperature C-H activation catalysts and reaction systems is the key to converting methane in a direct and mild manner. The recently developed reaction processes operated at low-temperature thermocatalysis systems or driven in electro- and photocatalysis systems shine light on the way to achieve efficient methane conversion with much economical energy input. In this review, we summarize the typical catalytic processes employed in these reaction systems and in particular highlight the potential heterogeneous catalysts with noteworthy C-H activation performance. We also present the progress along with our perspectives on catalyst design, theoretical simulations, the choice of reaction condition, and the method of reaction product analysis to encourage more viable technology for low-temperature methane conversion in the future