Biagio Di Vizio, Dario Mosconi, Matías Blanco, Panjuang Tang, Luca Nodari, Ondřej Tomanec, Michal Otyepka, Simone Pollastri, Stefano Livraghi, Mario Chiesa, Gaetano Granozzi, Stefano Agnoli
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引用次数: 0
Abstract
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
期刊介绍:
The Chemical Engineering Journal is an international research journal that invites contributions of original and novel fundamental research. It aims to provide an international platform for presenting original fundamental research, interpretative reviews, and discussions on new developments in chemical engineering. The journal welcomes papers that describe novel theory and its practical application, as well as those that demonstrate the transfer of techniques from other disciplines. It also welcomes reports on carefully conducted experimental work that is soundly interpreted. The main focus of the journal is on original and rigorous research results that have broad significance. The Catalysis section within the Chemical Engineering Journal focuses specifically on Experimental and Theoretical studies in the fields of heterogeneous catalysis, molecular catalysis, and biocatalysis. These studies have industrial impact on various sectors such as chemicals, energy, materials, foods, healthcare, and environmental protection.