Enhanced selective oxidation of ethylarenes using iron single atom catalysts embedded in Nitrogen-Rich graphene

Enhanced selective oxidation of ethylarenes using iron single atom catalysts embedded in Nitrogen-Rich graphene

•A new low temperature and environmental friendly synthesis of nitrogen rich (19 % w/w) graphene is proposed.•The selective presence (78 % w/w) of pyridinic species allow stabilizing Fe single atom catalysts (leaching < 0.02 % w/w).•The Fe SACs exhibit excellent catalytic activity in the selectiv...

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Bibliographic Details
Published in:Chemical engineering journal (Lausanne, Switzerland : 1996) Vol. 499; p. 156299
Main Authors: Di Vizio, Biagio, Mosconi, Dario, Blanco, Matías, Tang, Panjuang, Nodari, Luca, Tomanec, Ondřej, Otyepka, Michal, Pollastri, Simone, Livraghi, Stefano, Chiesa, Mario, Granozzi, Gaetano, Agnoli, Stefano
Format: Journal Article
Language:English
Published: Elsevier B.V 01-11-2024
Subjects:
Cardiovascular Health
Health Inequity
Heart Rate Variability
Immune Function
Maternal Health
Perinatal
Pregnancy
Preterm Birth
Race
Sleep
Structural Racism
Pregnancy
Cardiovascular Health
Health Inequity
Maternal Health
Sleep
Immune Function
Preterm Birth
Race
Perinatal
Structural Racism
Heart Rate Variability
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Summary:•A new low temperature and environmental friendly synthesis of nitrogen rich (19 % w/w) graphene is proposed.•The selective presence (78 % w/w) of pyridinic species allow stabilizing Fe single atom catalysts (leaching < 0.02 % w/w).•The Fe SACs exhibit excellent catalytic activity in the selective oxidation of ethylarenes (TON=13400 h−1) and a broad scope.•The reaction is genuinely catalytic with O2 as final oxidant, and the selectivity is controlled by choosing the peroxide. Heavily (19 % wt) Nitrogen doped graphene (N-G), with Nitrogen incorporated mainly as pyridinic species (77.8 %), was obtained by reacting fluorographene with ammonia under solvothermal conditions, at mild temperature (140 °C). N-G was used to stabilize single iron atoms (N-G-Fe) in two different configurations: low spin X-(FeIIN4)-Y and high spin X-(FeIIIN4)-Y. The resulting N-G-Fe single atom catalysts exhibit remarkable efficacy in the selective oxidation of ethylarenes, with activity comparable or even superior to state-of-the-art materials, converting ethylbenzene to acetophenone with an initial turnover frequency of 13400 h−1. Notably, N-G-Fe exhibits genuine catalytic activity since it is able to oxidize ethylbenzene using substoichiometric amount of peroxides, and exploiting molecular oxygen as the final oxidant. Moreover, N-G-Fe can be recycled without any metal leaching, and exhibits a broad catalytic scope. Multi-technique characterizations combined with rationally designed catalytic tests allowed us to identify the active sites and propose a plausible mechanism for the catalytic cycle.
ISSN:1385-8947
DOI:10.1016/j.cej.2024.156299