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

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Chinese Journal of Chemical Engineering 2024年第6期70卷 261-268页

作者： Song Tian Yicheng Chen Xiaoyu Wen Bingcheng Li Jian Lu Zile Li Feng Feng Qingtao Wang Qunfeng Zhang Xiaonian Li State Key Laboratory Breeding Base of Green Chemistry Synthesis Technology Institute of Industrial Catalysis of Zhejiang University of TechnologyHangzhou 310014China State Key Laboratory of Fluorine&Nitrogen Chemicals Xi'an Modern Chemistry Research InstituteXi'an 710065China

Chlorotrifluoroethylene(CTFE)is a vital fluorinated olefinic monomer produced through the catalytic hydrodechlorination of trichlorotrifluoroethane(CFC-113),an eco-friendly ***,hydrodechlorination catalysts for olefin production often suffer from poor *** 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 ***-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 *** 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 ***,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 *** the reaction progressed,these new species agglomerated,leading to a gradual loss of catalyst ***,the deactivated catalyst was successfully reactivated using a simple alkaline washing method.

关键词： CFC-113 hydrodechlorination Chlorotrifluoroethylene Catalyst deactivation

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Effects of particle composition and environmental parameters on catalytic hydrodechlorination of trichloroethylene by nanoscale bimetallic Ni-Fe

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Journal of Environmental Sciences 2014年第5期26卷 1162-1170页

作者： Jianjun Wei Yajing Qian Wenjuan Liu Lutao Wang Yijie Ge Jianghao Zhang Jiang Yu Xingmao Ma Department of Environmental Science and Engineering Beijing University of Chemical Technology Department of Civil and Environmental Engineering Southern Illinois University Carbondale

Catalytic nickel was successfully incorporated into nanoscale iron to enhance its dechlorination efficiency for trichloroethylene （TCE）, one of the most commonly detected chlorinated organic compounds in groundwater. Ethane was the predominant product. The greatest dechlorination efficiency was achieved at 22 molar percent of nickel. This nanoscale Ni-Fe is poorly ordered and inhomogeneous; iron dissolution occurred whereas nickel was relatively stable during the 24-hr reaction. The morphological characterization provided significant new insights on the mechanism of catalytic hydrodcchlorination by bimetallic nanoparticles. TCE degradation and ethane production rates were greatly affected by environmental parameters such as solution pH, temperature and common groundwater ions. Both rate constants decreased and then increased over the pH range of 6.5 to 8.0, with the minimum value occurring at pH 7.5. TCE degradation rate constant showed an increasing trend over the temperature range of 10 to 25℃. However, ethane production rate constant increased and then decreased over the range, with the maximum value occurring at 20℃, Most salts in the solution appeared to enhance the reaction in the first half hour but overall they displayed an inhibitory effect. Combined ions showed a similar effect as individual salts.

关键词： nanoscale Ni-Fe trichloroethylene hydrodechlorination catalytic dechlorination composition environmental parameters

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N,O Co-Doping Enhanced Adsorption of Chloramphenicol for Highly Efficient and Robust Electrocatalytic hydrodechlorination

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Chinese Journal of Chemistry 2024年第20期42卷 2445-2452页

作者： Xue-Feng Cheng Qiang Cao Qing Liu Hao-Yu Zhang Qing-Feng Xu Jian-Mei Lu College of Chemistry Chemical Engineering and Materials ScienceCollaborative Innovation Center of Suzhou Nano Science and TechnologySoochow UniversitySuzhouJiangsu 215123China

Electrocatalysis technology can effectively promote the hydrodechlorination of chloramphenicol(CAP)to reduce the ***,there are still some challenges such as low degradation rate and poor ***,we prepared porous N,O co-doped carbon supported Pd nanoparticles composites(Pd NPs/NO-C)for electrocatalytic degradation of *** doping of N and O not only effectively enhanced the interaction between substrate and CAP,promoting the mass transfer process,but also enhanced the anchoring effect on Pd nanoparticles,avoiding the occurrence of *** prepared composites achieved removal efficiency of CAP over 99%within 1 h,and the rate constant was as high as 6.72 h^(–1),outperforming previous reported ***,Pd NPs/NO-C composites showed a wide range of pH tolerance,excellent ion interference resistance and long-term *** work unravels the importance of mass transfer processes in solution to electrocatalytic hydrodechlorination and provides new research ideas for catalysts design.

关键词： Chloramphenicol hydrodechlorination Electrocatalysis N,O co-doped carbon Mass transfer Supported catalysts Nanoparticles Low-dimensionalmaterials

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Pd nanoparticles on defective polymer carbon nitride:Enhanced activity and origin for electrocatalytic hydrodechlorination reaction

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Chinese Chemical Letters 2020年第10期31卷 2762-2768页

作者： Song Shu Peng Wang Wendong Zhang Weilu Wang Jianjun Li Yinghao Chu Fusheng Wei Xianming Zhang Guangming Jiang College of Architecture and Environment Sichuan UniversityChengdu 610065China Engineering Research Center for Waste Oil Recovery Technology and Equipment Ministry of EducationChongqing Technology and Business UniversityChongqing 400067China Chongqing Key Laboratory of Three Gorges Reservoir Area Surface Process and Environmental Remote Sensing Chongqing Key Laboratory of Inorganic Functional MaterialsChongqing Normal UniversityChongqing 401331China

Here we report a facile defect-engineering strategy on the support to optimize the metal-support interaction and enhance the metal’s electrocatalytic hydrodechlo rination perfo rmance in converting 2,4-dichlorophenol(2,4-DCP)to *** specific activity of the Pd nanoparticles(Pd NPs)on defective polymer carbon nitride(Pd/PCN-x)reaches 0.09 min^(-1) m^-2Pd,which is 1.5 times that of the Pd NPs supported on the perfect PCN(Pd/PCN-0).The combined experimental and theoretical results demonstrate that the strong adsorption of phenol on Pd/PCN-0 passivates the active sites,limiting the dechlorination *** PCN-x containing-C≡N defects can effectively mediate the spatial configuration and electronic structure of Pd NPs,and promote the preferential adsorption of 2,4-DCP rather than phenol,resulting in an enhanced dechlorination efficiency.

关键词： hydrodechlorination Electrocatalysis Adsorption properties Metal-support interaction N defects

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One-step Synthesis of N-Doped Mesoporous Carbon as Highly Efficient Support of Pd Catalyst for hydrodechlorination of 2,4-Dichlorophenol

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Chemical Research in Chinese Universities 2018年第6期34卷 1004-1008页

作者： TANG Haodong XIANG Meng XU Bin LI Ying HAN Wenfeng LIU Zongjian Institute of Industrial Catalysis College of Chemical Engineering Zhej'iang University of Technology Hangzhou 300014 P. R. China

Although the hard template method is often employed to prepare N-doped mesoporous carbon（N-MC）, tile removal of the silica template commonly involves the use of highly toxic HF or repeated treatment with NaOH solution. Herein, we reported a polyvinylidene fluoride-assisted one-step method for synthesis of N-MC, namely the silica-free N-MC can be prepared via temperature-programmed thermal treatment of a slurry obtained by dispersing nano-silica into a solution containing sucrose, urea, oxalic acid, polyvinylidene fluoride and dimethylacetamide. The resulting N-MC, which owns 3.47%（mass fraction） nitrogen and a surface area of 929 m^2/g, is a highly suitable support of Pd catalyst used in hydrodechlorination of 2,4-dichlorophenol, with its performance being much better than those of MC and activated carbon. The excellent catalytic hydrodeehlorination activity of the Pd/N-MC catalyst can be attributed to its strong metal-support interaction, which results in a good Pd dispersion and high resistance to the growth of nanosized Pd under reaction conditions.

关键词： 2,4-Dichlorophenol hydrodechlorination N-Doped mesoporous carbon Polyvinylidene fluoride Pd catalyst

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Palladium nanoparticles assembled on titanium nitride for enhanced electrochemical hydrodechlorination of 2,4-dichlorophenol in water

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Chinese Journal of Catalysis 2018年第4期39卷 693-700页

作者： Wenyang Fu Kaifeng Wang Xiaoshu Lv Hailu Fu Xingan Dong Ling Chen Xianming Zhang Guangming Jiang Engineering Research Center for Waste Oil Recovery Technology and Equipment Ministry of EducationChongqing Technology and Business UniversityChongqing 400067China College of Quality and Safety Engineering China Jiliang UniversityHangzhou 310018ZhejiangChina

We report a one‐pot surfactant‐free wet‐chemical reduction approach to the synthesis of palladium/titanium nitride(Pd/TiN)and Pd/carbon(Pd/C)composites,in which^5 nm Pd NPs were uniformly dispersed on TiN or *** terms of catalytic performance,Pd/TiN showed enhanced efficiency and stability compared with those of Pd/C and bare TiN in the electrocatalytic hydrodechlorination(EHDC)reaction of 2,4‐dichlorophenol(2,4‐DCP)in aqueous *** superior performance of Pd/TiN arises from the promotion effect of *** metal‐support interactions modified the electronic structure of Pd,which optimized generation of H*ads and 2,4‐DCP adsorption/*** cathode potential plays a vital role in controlling the EHDC efficiency and the product distribution.A working potential of?0.80 V was shown to be optimal for achieving the highest EHDC efficiency and maximizing conversion of 2,4‐DCP to phenol(P).Our studies of the reaction pathway show that EHDC of 2,4‐DCP on Pd/TiN proceeded by 2,4‐DCP→p‐chlorophenol(p‐CP),o‐chlorophenol(o‐CP)→P;however,Pd/TiN presented little selectivity for cleavage of p‐C‐Cl vs o‐C‐*** work presents a new approach to enhancing Pd performance towards EHDC through the effects of a *** strategy demonstrated here could also be extended to design highly efficient catalysts for other hydrogenation reactions.

关键词： hydrodechlorination Electrolysis Palladium Titanium nitride Environmental remediation

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hydrodechlorination of chlorobenzene over NiB amorphous catalyst——Influence of solvent and base

Hydrodechlorination of chlorobenzene over NiB amorphous cata...

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第六届全国工业催化技术及应用年会

作者：赵凤玉 State Key Laboratory of Electroanalytical Chemistry Changchun Institute of Applied ChemistryChinese Academy of Sciences

An air-stable and efficient NiB amorphous catalyst were prepared by chemical reduction and characterized by XRD, XPS, BET and TEM. The NiB catalyst showed a high activity in hydrodechlorination of chlorobenzene under mild conditions. Water was the most active solvent and its presence could largely improve the reaction rate in organic solvents. And the reaction rate was the highest in the presence of triethylamine but lower in NaOH, which was discussed from the surface electronic property and surface area of NiB amorphous catalyst.

关键词： NiB amorphous catalyst hydrodechlorination chlorobenzene base effect

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SYNTHESIS OF SYMMETRICALLY TETRA-SUBSTITUTED PALLADIUM PHTHALOCYANINES AS CATALYSTS FOR hydrodechlorination OF CHLOROBENZENE IN GAS PHASE

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化工学报 2002年第5期53卷 450-451页

作者：丁亮中钟桐生 Department of Chemistry Hunan City College 湖南 Yiyang 413049

Catalytic hydrodechlorination is an elegant reaction for disposal of environmentally hazardous chlorocarbons, such as chloro-benzene. Development of a new catalyst with excellent stability is necessary due to the deactivation of supported noble metal catalysts. However the modification of catalytic properties of catalysts in hydrodechlorination reaction by introducing stable ligands to noble metals has been the least studied. here the synthesis of Pd(II) 2, 9, 16, 23 - symetrically tetrasubstituted phthalocyanines PdPTX_4 (where X = -H, -NO_2, -NH_2 respectively) from phthalimide derivatives is reported, and their application as catalysts in hydrodechlorination of chlorobenzene, which is a representative environmentally hazardous materials is discussed.

关键词： palladium phthalocyanine chlorobenzene catalytic hydrodechlorination

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加氢脱氯在环境污染控制中的应用:负载及非负载型钯和镍催化剂性能的比较(英文)

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催化学报 2011年第5期32卷 746-755页

作者： Claudia AMORIM Mark A.KEANE Chemical Engineering School of Engineering and Physical SciencesHeriot-Watt University

Catalytic hydrodechlorination(HDC)is an innovative means of transforming chlorinated waste streams into a recyclable product. In this study,the gas phase HDC of chlorobenzene(CB)has been studied over bulk Pd and Ni and((8±1)wt%)Pd and Ni supported on activated carbon(AC),graphite,graphitic nanofibers(GNF),Al2O3,and *** activation was examined by temperature-programmed reduction(TPR)analysis and the activated catalysts characterized in terms of BET area,transmission electron microscopy,scanning electron microscopy,H2 chemisorption/temperature-programmed desorption,and X-ray diffraction *** surface area(1-19 m 2 /g), TPR,and H2 uptake/release exhibited a dependence on both metal and *** Pd system delivered specific HDC rates that were up to three orders of magnitude greater than that recorded for the Ni catalysts,a result that we link to the higher H2 diffusivity in *** was 100%selective over Ni while Pd also produced cyclohexane(selectivity<4%)as a result of a combined HDC/*** Pd outperformed carbon supported Pd but was less active than Pd on the oxide *** contrast,unsupported Ni presented no measurable activity when compared with supported *** specific HDC rate was found to increase with decreasing metal surface area where spillover hydrogen served to enhance HDC performance.

关键词： hydrodechlorination chlorobenzene bulk palladium and nickel catalysts activated carbon graphite carbon nanofiber alumina silica spillover hydrogen

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