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Oxidation of benzene to phenol with N_(2)O over a hierarchical Fe/ZSM-5 catalyst

Green Energy & Environment 2023年第4期8卷 1161-1173页

作者： Cui Ouyang Jianwei Li Yaqi Qu Song Hong Songbo He State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing100029China Green Chemical Reaction Engineering Engineering and Technology Institute GroningenUniversity of GroningenNijenborgh 4Groningen9747 AGthe Netherlands CoRe Pro Colijnlaan 21Groningen9722 PJthe Netherlands

Catalytic oxidation of benzene with N_(2)O to phenol over the hierarchical and microporous Fe/ZSM-5-based catalysts in a continuous fixedbed reactor was *** spent catalyst was in-situ regenerated by an oxidative treatment using N_(2)O and in total 10 reaction-regeneration cycles were performed.A 100% N_(2)O conversion,93.3% phenol selectivity,and high initial phenol formation rate of 16.49±0.06mmol_(phenol gcatalyst)^(-1)h^(-1)at time on stream(TOS) of 5 min,and a good phenol productivity of 147.06 mmol_(phenol gcatalyst)^(-1)during catalyst lifetime of 1800 min were obtained on a fresh hierarchical Fe/ZSM-5-Hi2.8 *** the reaction-regeneration cycle,N_(2)O conversion is fully recovered within TOS of 3 h,moreover,the phenol productivity was decreased ca.2.2±0.8% after each cycle,leading to a total phenol productivity of ca.0.44 ton_(pheol kg_(catalyst)^(-1)estimated for 300 *** characterizations imply that the coke is rapidly deposited on catalyst surface in the initial TOS of 3 h(0.28 mgc_(gcatalyst)^(-1)min^(-1)) and gradually becomes graphitic during the TOS of 30 h with a slow formation rate of 0.06 mgc g_(catalyst)^(-1)min^(-1).Among others(e.g.,the decrease of textural property and acidity),the nearly complete coverage of the active Fe-O-Al sites by coke accounts for the main catalyst *** these reversible deactivation characteristics related to coking,the irreversible catalyst deactivation is also observed with the reaction-regeneration *** latter is reflected by a further decreased amount of the active Fe-O-Al sites,which agglomerate on catalyst surface with the cycle,likely associated with the hard coke residue that is not completely removed by the regeneration.

关键词： Hierarchical Fe/ZSM-5 N_(2)O conversion phenol product productivity Reaction-regeneration cycles Irreversible deactivation mechanism

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