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

• 作者: Dehui Deng Haiyang Li Haobo Li Jianping Xiao Lei Hua Liang Yu Mengqi He N.Pethan Rajan Suheng Wang Xiaoju Cui Zhaoxiong Xie
• 来源期刊: 能源化学
• 年，卷（期）: 2019,（9）
• 页码范围: 47-50
• 页数: 4页
• 语种: 英文

摘要

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 ℃) conditions.Herein,a highly active catalytic conversion process of ethane at room temperature (25 ℃) is reported on single iron atoms confined in graphene via the porphyrin-like N4-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 C2 chemicals,simultaneously avoiding the over-oxidation of the products to CO2.The in-situ formed O-FeN4-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 FeN4 center and provides the reference in development of efficient catalyst for selective oxidation of light alkane.