Abstract:
: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.
journal_name
Sci Advjournal_title
Science advancesauthors
Deng D,Chen X,Yu L,Wu X,Liu Q,Liu Y,Yang H,Tian H,Hu Y,Du P,Si R,Wang J,Cui X,Li H,Xiao J,Xu T,Deng J,Yang F,Duchesne PN,Zhang P,Zhou J,Sun L,Li J,Pan X,Bao Xdoi
10.1126/sciadv.1500462subject
Has Abstractpub_date
2015-12-04 00:00:00pages
e1500462issue
11issn
2375-2548pii
1500462journal_volume
1pub_type
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