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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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基于人工智能的雷达设备虚拟维修训练仿真模型

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现代电子技术 2024年第8期47卷 182-186页

作者：许诚李小年赵鹏卢坤空军预警学院湖北武汉430019 陇东学院甘肃庆阳745000

雷达设备是重要的电子设备,但在工作过程中可能会出现各种故障。通过开发虚拟维修训练仿真模型,可以提供一个实际环境下的虚拟场景,使维修人员能够在虚拟的情境下进行维修训练,以此提高维修人员的操作技能和判断能力,在面对实际故障时... 详细信息

雷达设备是重要的电子设备,但在工作过程中可能会出现各种故障。通过开发虚拟维修训练仿真模型,可以提供一个实际环境下的虚拟场景,使维修人员能够在虚拟的情境下进行维修训练,以此提高维修人员的操作技能和判断能力,在面对实际故障时能更高效和准确地进行维修,提升雷达设备维修效果。为此,文中设计一种基于人工智能的雷达设备虚拟维修训练仿真模型。依据用户输入的雷达设备虚拟维修训练的相关设计参数,以及线性激光扫描仪采集的点云数据,采用人工智能中的三维重建技术构建雷达设备和维修场景三维模型。利用人工智能中的粒子群算法对仿真过程进行碰撞检测,得到维修训练路径规划结果。对仿真过程展开维修性检验,判断雷达设备是否符合维修性要求,并利用投影仪呈现虚拟维修训练仿真过程的相关数据,显示雷达设备虚拟维修训练结果。实验结果表明:所设计模型可有效实现雷达设备的三维点云重建,得到雷达设备三维模型,完成雷达设备虚拟维修训练仿真。

关键词：人工智能雷达设备虚拟维修训练三维重建技术粒子群算法碰撞检测路径规划

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A novel liquid system of catalytic hydrogenation

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Science China Chemistry 2007年第6期50卷 746-753页

作者： li xiaonian XIANG YiZhi State Key Laboratory Breeding Base of Green Chemistry Synthesis Technology Resources & Environment Catalysis Institute Zhejiang University of Technology Hangzhou 310032 China State Key Laboratory Breeding Base of Green Chemistry Synthesis Technology Resources & Environment Catalysis Institute Zhejiang University of Technology Hangzhou 310032 China

On the basis that endothermic aqueous-phase reforming of oxygenated hydrocarbons for H2 produc- tion and exothermic liquid phase hydrogenation of organic compounds are carried out under extremely close conditions of temperature and pressure over the same type of catalyst, a novel liquid system of catalytic hydrogenation has been proposed, in which hydrogen produced from aqueous-phase re- forming of oxygenated hydrocarbons is in situ used for liquid phase hydrogenation of organic com- pounds. The usage of active hydrogen generated from aqueous-phase reforming of oxygenated hy- drocarbons for liquid catalytic hydrogenation of organic compounds could lead to increasing the se- lectivity to H2 in the aqueous-phase reforming due to the prompt removal of hydrogen on the active centers of the catalyst. Meanwhile, this novel liquid system of catalytic hydrogenation might be a po- tential method to improve the selectivity to the desired product in liquid phase catalytic hydrogenation of organic compounds. On the other hand, for this novel liquid system of catalytic hydrogenation, some special facilities for H2 generation, storage and transportation in traditional liquid phase hydrogenation industry process are yet not needed. Thus, it would simplify the working process of liquid phase hy- drogenation and increase the energy usage and hydrogen productivity.

关键词： novel hydrogenation reaction, aqueous-phase reforming, liquid catalytic hydrogenation, coupling

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Ru/AC和Ru-NPs/AC催化剂对乙炔氢氯化反应催化活性的比较

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高校化学工程学报 2024年第4期38卷 578-585页

作者：徐达王赛赛马腾云万立祺赵佳蔡海婷李小年浙江工业大学化学工程学院浙江杭州310014

针对乙炔氢氯化反应无汞催化剂的开发,Ru基催化剂是最具工业潜力的催化剂之一。结合表面积分析仪(BET)、程序升温还原(TPR)、透射电镜(TEM)和程序升温脱附(TPD),以及动力学实验探究了导致Ru/AC(AC为活性炭)和高温H_(2)处理后Ru-NPs/AC... 详细信息

针对乙炔氢氯化反应无汞催化剂的开发,Ru基催化剂是最具工业潜力的催化剂之一。结合表面积分析仪(BET)、程序升温还原(TPR)、透射电镜(TEM)和程序升温脱附(TPD),以及动力学实验探究了导致Ru/AC(AC为活性炭)和高温H_(2)处理后Ru-NPs/AC催化性能差异的原因。在排除内、外扩散的条件下,通过动力学实验判断了反应级数,初步推测了基元反应步骤和决速步骤。结果表明,Ru-NPs/AC相对于Ru/AC总反应速率更低,表观活化能更高,这是由于高温H_(2)处理后活性组分的分散度降低、Ru物种被还原,并且导致活性中心对C_(2)H_(2)的吸附性能降低。

关键词：乙炔氢氯化 Ru基催化剂反应级数表观活化能活性中心

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Pd/C modified with Sn catalyst for liquid-phase selective hydrogenation of maleic anhydride to gamma-butyrolactone

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Chinese Chemical Letters 2017年第6期28卷 1330-1335页

作者： Rongrong li Jia Zhao Deman Han xiaonian li Industrial Catalysis Institute of Zhejiang University of Technology Hangzhou 310014China School of Pharmaceutical and Chemical Engineering Tai Zhou UniversityTaizhou 317000China

Pd catalysts suffered from poor selectivity and stability for liquid-phase hydrogenation of maleic anhydride（MA） to gamma-butyrolactone（GBL）.Thus,Pd/C catalysts modified with different Sn loadings were synthesized,and characterized by XRD,XPS,TEM and elemental *** types of alloy phase and the amounts of the surface Pd-SnOx sites altered along with Sn/Pd mass ratios from 0-1.0synthesized in the process of *** maximum reaction rate was 0.57 mol-GBL/（mol-Pd min）and selectivity was 95.94%when the Sn/Pd mass ratio was *** might be attributed to the formation of Pd2Sn alloy and less amounts of Pd-SnOx sites.

关键词： Bimetallic catalysts Sn/Pd mass ratio Maleic anhydride Selective hydrogenation Gamma-butyrolactone

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碳负载Cs和Cu基催化剂用于1,1,2-三氯乙烷的气相脱氯化氢

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化工学报 2024年第2期75卷 575-583页

作者：盖星宇岳玉学杨春华张子龙蔡天姿张海丰王柏林李小年东北电力大学化学工程学院吉林吉林132012 浙江工业大学工业催化研究所浙江杭州310014

采用浸渍法制备了Cs/AC和Cu/AC催化剂,并在1,1,2-三氯乙烷的气相脱氯化氢反应中进行了评价。在浸渍过程中,活性炭表面产生高度分散的Cs物种和少量结晶的Cu物种。Cs/AC催化剂具有优异的催化性能,在573 K、1000 h^(−1)的反应条件下,转化... 详细信息

采用浸渍法制备了Cs/AC和Cu/AC催化剂,并在1,1,2-三氯乙烷的气相脱氯化氢反应中进行了评价。在浸渍过程中,活性炭表面产生高度分散的Cs物种和少量结晶的Cu物种。Cs/AC催化剂具有优异的催化性能,在573 K、1000 h^(−1)的反应条件下,转化率稳定在86.7%。实验和理论计算表明,CsCl物种促进了1,1,2-三氯乙烷的吸附和活化,从而提高了原料转化率。这项工作为探索高效经济地合成偏二氯乙烯提供了一种很有前景的策略。

关键词：偏二氯乙烯活性炭催化 1,1,2-三氯乙烷脱氯化氢催化剂载体

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Oxygen and nitrogen-doped metal-free carbon catalysts for hydrochlorination of acetylene

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Chinese Journal of Chemical Engineering 2016年第4期24卷 484-490页

作者： Tongtong Zhang Jia Zhao Jiangtao Xu Jinhui Xu Xiaoxia Di xiaonian li Industrial Catalysis Institute of Zhejiang University of Technology Hangzhou 310014 China

Activated carbon was tested as metal-free catalyst for hydrochlorination of acetylene in order to circumvent the problem of environment pollution caused by mercury and high cost by noble metals. Oxygen-doped and nitrogen-doped activated carbons were prepared and characterized by XPS, TPD and N2 physisorption methods. The influences of the surface functional groups on the catalytic performance were discussed base on these results. Among all the samples tested, a nitrogen-doped sample, AC-n-US00, exhibited the best performance, the acety- lene conversion being 92% and vinyl chloride selectivity above 99% at 240 ~C and C2H2 hourly space velocity 30 h- 1. Moreover, the AC-n-US00 catalyst exhibited a stable performance during a 200 h test with a conversion of acetylene higher than 76% at 210 ~C at a C2H2 hourly space velocity 50 h 1. In contrary, oxygen-doped catalyst had lower catalytic activities. A linear relationship between the amount of pyrrolic-N and quaternary-N species and the catalytic activity was observed, indicating that these nitrogen-doped species might be the active sites and the key in tuning the catalytic performance. It is also found that the introduction of nitrogen species into the sample could significantly increase the adsorption amount of acetylene. The deactivation of nitrogen- doped activated carbon might be caused by the decrease of the accessibility to or the total amount of active sites.

关键词： Acetylene hydrochlorinationActivated carbonSurface chemistryOxygenated groupNitrogen-doped

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Titanium-Containing Mesoporous Materials: Synthesis and Application in Selective Catalytic Oxidation

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Journal of Natural Gas Chemistry 2006年第3期15卷 164-177页

作者： Jie li Chunhui Zhou Huali Xie Zhonghua Ge liangcai Yuan xiaonian li College of Chemical Engineering and Materials Science Zhejiang University of Technology Hangzhou 310014 Zhejiang China

Titanium-containing mesoporous molecular sieves are of great significance in selective catalytic oxidation processes with bulky molecules. Recent researches and developments on the designing and synthesis of Ti-containing mesoporous materials have been reviewed. Various strategies for the preparation of Ti-containing mesoporous materials, such as direct synthesis and post-synthesis, are described. Modifications of Ti-containing mesoporous materials by surface-grafting and atom-planting are also discussed. All approaches aimed mainly at the improving of the stability, the hydrophobicity, and mostly the catalytic activity. Structural and mechanistic features of various synthetic systems are discussed. Ticontaining mesoporous materials in liquid phase catalytic oxidation of organic compounds with H2O2 as an oxidant is briefly summarized, showing their broad utilities for green synthesis of fine chemicals by catalytic oxidative reactions.

关键词： mesoporous materials titanium molecular sieve zeolites characterization catalytic oxidation

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Two-Stage Hydrogenation Modification of C_9 Petroleum Resin over NiWS/γ-Al_2O_3 and PdRu/γ-Al_2O_3 Catalysts in Series

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China Petroleum Processing & Petrochemical Technology 2012年第3期14卷 83-89页

作者： Yu Lujun Jiang Dahao Xu Jiao Ma Lei li xiaonian State Key Laboratory Breeding Base of Green Chemistry Synthesis Technology Zhejiang University of Technology

Hydrogenation modification is one of the most important ways to produce high-quality petroleum resin. The col- orless C9 petroleum resin （CgPR） was obtained by two-stage catalytic hydrogenation over NiWS/？-A1203 catalyst and PdRu/ y-A1203 catalyst connected in series. Via the hydrogenation reaction, aromatic rings in C9PR were converted to alicyclic rings, and its color was reduced from Gardner color grade No. 11 to Gardner color grade No. 0. The optimum Ni/W atomic ratio was found to be close to 0.23, while the optimum Pd/Ru atomic ratio was close to 3.80. The TEM results showed that the morphology and size of sulfide or metal particles of the two kinds of catalysts remained almost unchanged after the reac- tion was carried our for 1 204 hours, attesting to their good catalytic stability.

关键词： C9 petroleum resin hydrogenation modification NiWS/3,- A1203 PdRu/7- A1203

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Gas-phase dehydrochlorination of 1, 1, 2, 2-tetrachloroethane over the non-metal supported ionic liquid catalyst

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Chinese Journal of Chemical Engineering 2020年第6期28卷 1623-1627页

作者： Pengze Zhang Yangzhen Jin Zhaobin Jiang Guanqun Xie Qunfeng Zhang xiaonian li Institute of Industrial Catalysis State Key Laboratory Breeding Base of Green Chemistry-Synthesis TechnologyCollege of Chemical EngineeringZhejiang University of TechnologyHangzhou 310014China School of Environment and Civil Engineering Dongguan University of TechnologyDongguan 523808China

Developing of non-metallic catalyst to replace metal catalyst is a meaningful and challenging *** this work,the non-metallic catalyst was synthetized successfully by loading ionic liquid onto the silica surface,which was applied for the gas-phase dehydrochlorination of 1,1,2,*** 12%TPPC/SiO2(wt%)showed the best results with the conversion of 1,1,2,2-tetrachloroethane reaching 100%.The selectivity of 1,1,2-trichloroethylene was 100%,and no deactivation was found during the evaluation *** catalytic mechanism was investigated and possible reaction route was given,which was a reference for fabricating and design of solid base catalyst.

关键词： Dehydrochlorination catalyst Supported ionic liquids Gas-phase catalysis Base catalysis

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