Hydrodechlorination of trifluoro-trichloroethane to chlorotrifluoroethylene:Revealing the deactivation mechanism and regeneration strategy of Pd-Cu/AC catalyst  

作　　者：Song Tian Yicheng Chen Xiaoyu Wen Bingcheng Li Jian Lu Zile Li Feng Feng Qingtao Wang Qunfeng Zhang Xiaonian Li 

机构地区：[1]State Key Laboratory Breeding Base of Green Chemistry Synthesis Technology,Institute of Industrial Catalysis of Zhejiang University of Technology,Hangzhou 310014,China [2]State Key Laboratory of Fluorine&Nitrogen Chemicals,Xi'an Modern Chemistry Research Institute,Xi'an 710065,China

出　　处：《Chinese Journal of Chemical Engineering》2024年第6期261-268,共8页中国化学工程学报（英文版）

基　　金：supported by the National Natural Science Foundation of China(22008212,22078292,21902124);Natural Science Basic Research Planning Shaanxi Province of China(2017ZDJC-29);Key Research and Development Project of Shaanxi Province(2018ZDXM-GY-173);China Postdoctoral Science Foundation(2019 M663848);Open cooperative innovation fund of Xi'an Institute of modern chemistry(SYJJ48).

摘　　要：Chlorotrifluoroethylene(CTFE)is a vital fluorinated olefinic monomer produced through the catalytic hydrodechlorination of trichlorotrifluoroethane(CFC-113),an eco-friendly process.However,hydrodechlorination catalysts for olefin production often suffer from poor stability.The Pd/AC catalyst and Pd-Cu/AC catalyst prepared by co-impregnation method exhibited poor stability,Pd-Cu/AC catalyst with CFC-113 conversion dropping to around 37%after 50 h of hydrodechlorination reaction.Brunauer-Emmett-Teller,transmission electron microscopy,X-ray photoelectron spectroscopy,and X-ray diffraction of fresh and deactivated Pd/AC catalysts indicate that the deactivation of Pd/AC catalysts is due to high-temperature agglomeration of Pd.Comparative analysis of fresh and deactivated Pd-Cu/AC catalysts using Brunauer-Emmett-Teller,transmission electron microscopy,and thermogravimetric analysis techniques revealed decreased dispersion of active sites,reduced surface area,catalyst aggregation deactivation,and a significant decrease in Cu content.Furthermore,the results of NH3-TPD revealed that the acid sites of the catalyst increased significantly.X-ray diffraction spectra indicated the formation of new species,basic copper chloride(Cu_(2)(OH)_(3)Cl),during the reaction.As the reaction progressed,these new species agglomerated,leading to a gradual loss of catalyst activity.Moreover,the deactivated catalyst was successfully reactivated using a simple alkaline washing method.

关 键 词：CFC-113 HYDRODECHLORINATION CHLOROTRIFLUOROETHYLENE Catalyst deactivation 

分 类 号：TQ222.423[化学工程—有机化工] TQ426