A single iron site confined in a graphene matrix for the catalytic oxidation of benzene at room temperature
By Dehui Deng, Xiaoqi Chen, Liang Yu, Xing Wu, Qingfei Liu, Yun Liu, Huaixin Yang, H. Tian, Yongfeng Hu, Peipei Du and 15 more. Science Advances, 2015
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A coordinatively unsaturated single iron site confined in a graphene matrix shows an ultrahigh activity for catalytic oxidation. Coordinatively unsaturated (CUS) iron sites are highly active in catalytic oxidation reactions; however, maintaining the CUS structure of iron during heterogeneous catalytic reactions is a great challenge. Here, we report a strategy to stabilize single-atom CUS iron sites by embedding highly dispersed FeN4 centers in the graphene matrix. The atomic structure of FeN4 centers in graphene was revealed for the first time by combining high-resolution transmission electron microscopy/high-angle annular dark-field scanning transmission electron microscopy with low-temperature scanning tunneling microscopy. These confined single-atom iron sites exhibit high performance in the direct catalytic oxidation of benzene to phenol at room temperature, with a conversion of 23.4% and a yield of 18.7%, and can even proceed efficiently at 0°C with a phenol yield of 8.3% after 24 hours. Both experimental measurements and density functional theory calculations indicate that the formation of the Fe═O intermediate structure is a key step to promoting the conversion of benzene to phenol. These findings could pave the way toward highly efficient nonprecious catalysts for low-temperature oxidation reactions in heterogeneous catalysis and electrocatalysis.
Subfields: Materials Chemistry, Organic Chemistry
View Paper: https://www.semanticscholar.org/paper/74322465b92748f1aa5676fa417c49945e56c005
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Citations in the corpus
- Room-Temperature Methane Conversion by Graphene-Confined Single Iron Atoms (2018, neutral): “The FeN4 moieties embedded in the lattice structure of GNs were prepared by a well-tested procedure.(28) In brief, the highly dispersed single FeN4 center anchored on graphene was synthesized by high-energy ball milling of iron phthalocyanine (FePc) and GNs.”