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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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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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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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Regulation of the selective hydrogenation performance of sulfur-doped carbon-supported palladium on chloronitrobenzene

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Chinese Journal of Chemical Engineering 2023年第6期58卷 69-75页

作者： Qunfeng Zhang Bingcheng li Yuan Zhou Deshuo Zhang Chunshan Lu Feng Feng Jinghui Lv Qingtao Wang xiaonian li Institute of Industrial Catalysis of Zhejiang University of Technology State Key Laboratory Breeding Base of Green Chemistry Synthesis TechnologyHangzhou 310014China

The overall performance of metal catalysts can be efficiently adjusted by modifying carbon carriers with different valence sulfur *** wet impregnation technique successfully prepared carbon material carriers doped with varying sources of sulfur(Na_(2)SO_(4),NaHSO_(3),Na_(2)S·9H_(2)O).Palladium carbon catalysts doped with different sulfur precursors had been prepared with the aid of the liquid-phase reduction method of the selective hydrogenation of o-chloronitrobenzene(o-CNB)to o-chloroaniline(o-CAN).The catalyst prepared for Na_(2)S·9H_(2)O as a precursor has excellent performance,and the selectivity for o-CAN is more than 99.9%at 100%*** addition,the characterization results show that with the decrease of S valence,the electronic effect between S and Pd increases,and the outer electron shift of Pd increases,which reduces the adsorption and dissociation ability of Pd to hydrogen,resulting in excellent *** effects provided a good idea for the hydrogenation of o-CNB and a different point of view on sulfur doping in a variety of hydrogenation reactions.

关键词： Catalyst Hydrogenation Selectivity Sulfur doping Electronic effect

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The highly selective catalytic hydrogenation of CO_(2)to CO over transition metal nitrides

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Chinese Journal of Chemical Engineering 2022年第3期35卷 248-254页

作者： Yichao Wu Zhiwei Xie Xiaofeng Gao Xian Zhou Yangzhi Xu Shurui Fan Siyu Yao xiaonian li lili lin Institute of Industrial Catalysis State Key Laboratory of Green Chemistry Synthesis TechnologyCollege of Chemical EngineeringZhejiang University of TechnologyHangzhou 310014China Key Laboratory of Biomass Chemical Engineering of Ministry of Education College of Chemical and Biological EngineeringZhejiang UniversityHangzhou 310027China

Three transition metal-like facet centered cubic structured transition metal nitrides,γ-Mo_(2)N,β-W_(2)N andδ-NbN,are synthesized and applied in the reaction of CO_(2)hydrogenation to *** the three nitride catalysts,theγ-Mo_(2)N exhibits superior activity to target product CO,which is 4.6 and 76 times higher than the other two counterparts ofβ-W_(2)N andδ-NbN at 600℃,***,γ-Mo_(2)N exhibits excellent stability on both cyclic heating-cooling and high space velocity steady state *** deactivation degree of cyclic heating-cooling evaluation after 5 cycles and long-term stability performance at 773 and 873 K in 50 h are all less than 10%.In-situ XRD and kinetic studies suggest that theγ-Mo_(2)N itself is able to activate both of the reactants CO_(2)and H_(2).Below 400℃,the reaction mainly occurs at the surface ofγ-Mo_(2)N ***_(2)and H_(2)competitively adsorbe on the surface of catalyst and CO_(2)is the relatively stronger surface *** a higher temperature,the interstitial vacancies of theγ-Mo_(2)N can be reversibly filled with the oxygen from CO_(2)*** of the surface and bulk phase sites ofγ-Mo_(2)N participate in the high temperature CO_(2)hydrogenation pathway.

关键词： Carbon dioxide Chemical reaction Catalysis Reverse water gas shift(RWGS)reaction Transition metal nitride In-situ X-ray diffraction characterization

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Low-content Pt-triggered the optimized d-band center of Rh metallene for energy-saving hydrogen production coupled with hydrazine degradation

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Journal of Energy Chemistry 2023年第10期85卷 58-66,I0004页

作者： Qiqi Mao Wenxin Wang Kai Deng Hongjie Yu Ziqiang Wang You Xu xiaonian li liang Wang Hongjing Wang State Key Laboratory Breeding Base of Green-Chemical Synthesis Technology College of Chemical EngineeringZhejiang University of TechnologyHangzhou 310014ZhejiangChina

Utilizing the hydrazine-assisted water electrolysis for energy-efficient hydrogen production shows a promising application, which relies on the development and design of efficient bifunctional electrocatalysts. Herein, we reported a low-content Pt-doped Rh metallene(Pt-Rhene) for hydrazine-assisted water electrolysis towards energy-saving hydrogen(H_(2)) production, where the ultrathin metallene is constructed to provide enough favorable active sites for catalysis and improve atom ***, the synergistic effect between Rh and Pt can optimize the electronic structure of Rh for improving the intrinsic activity. Therefore, the required overpotential of Pt-Rhene is only 37 mV to reach a current density of-10 mA cm^(-2) in the hydrogen evolution reaction(HER), and the Pt-Rhene exhibits a required overpotential of only 11 mV to reach a current density of 10 mA cm^(-2) in the hydrazine oxidation reaction(HzOR). With the constructed HER-HzOR two-electrode system, the Pt-Rhene electrodes exhibit an extremely low voltage(0.06/0.19/0.28 V) to achieve current densities of 10/50/100 mA cm^(-2) for energy-saving H_(2) production, which greatly reduces the electrolysis energy consumption. Moreover,DFT calculations further demonstrate that the introduction of Pt modulates the electronic structure of Rh and optimizes the d-band center, thus enhancing the adsorption and desorption of reactant/intermediates in the electrocatalytic reaction.

关键词： Pt-Rhene Synergistic effect Hydrogen evolution reaction Hydrazine oxidation reaction Energy-saving H_(2)production

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Graphdiyne anchoring to construct highly dense palladium trimer active sites for the selective hydrogenation of acetylene

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Nano Research 2023年第5期16卷 6167-6177页

作者： Rongrong li Yuxue Yue Xianlang Chen Renqin Chang Jiaxin Zhang Bo Zhao Jieyu Zhang Di Cai Yihan Zhu Deman Han Jia Zhao xiaonian li Engineering Research Center of Recycling and Comprehensive Utilization of Pharmaceutical and Chemical Waste of Zhejiang Province Taizhou UniversityTaizhou 318000China Industrial Catalysis Institute of Zhejiang University of Technology Hangzhou 310014China Research Center of Analysis Measurement of Zhejiang University of Technology Hangzhou 310014China School of Science Zhejiang Sci-Tech UniversityHangzhou 310018China

Semi-hydrogenation of acetylene is of growing interest and popularity but subjects to a major challenge in selective hydrogenation to ***,we report a strategy that uses graphdiyne(GDY)as a carrier to prepare single-cluster catalysts(SCCs),which on average clusters composed of three atoms(denoted as Pd3 trimer)and applied it to the acetylene semihydrogenation in the presence of large amounts of *** on experimental results and systematic quantum chemical research and computational screening,we found that there are multiple active Pd structures on GDY and the Pd3 trimer anchored on GDY is a specific and durable cluster with great potential for accurate and efficient heterogeneous *** synergetic effects between neighboring atoms in Pd trimer guarantee easy desorption of ethylene and the absence of unselective hydride species thereby preventing excessive hydrogenation to generate unwanted byproducts,which is a crucial mechanism for the excellent selectivity of the *** new method for precise synthesis Pd clusters provides accurate ways for designing selective hydrogenation catalysts at the atomic scale.

关键词： Pd cluster catalysts acetylene semi-hydrogenation Pd trimer

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Electron-deficient Cu site catalyzed acetylene hydrochlorination

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Green Energy & Environment 2023年第4期8卷 1128-1140页

作者： Bolin Wang Chunxiao Jin Shujuan Shao Yuxue Yue Yuteng Zhang Saisai Wang Renqin Chang Haifeng Zhang Jia Zhao xiaonian li School of Chemical Engineering Northeast Electric Power UniversityJilin132012China Industrial Catalysis Institute of Zhejiang University of Technology Hangzhou310014China Research Center of Analysis Measurement Zhejiang University of TechnologyHangzhou310014China

Rational design of catalytic sites to activate the C≡C bond is of paramount importance to advance acetylene hydrochlorination. Herein, Cu sites with electron-rich and electron-deficient states were constructed by controlling the impregnation solutions. The π electrons flowing from acetylene to Cu site are facilitated over the electron-deficient Cu sites, achieving high activation of C≡C bond. The contradiction between the increased activation of acetylene required for enhanced catalytic activity and the resistance of Cu site to reduction by acetylene required for maintaining catalytic stability can be balanced by establishing strong interactions of Cu site with pyrrolic-N species. The catalytic activity displays a volcano shape scaling relationship as a function of Cu particle size. Tribasic copper chloride is concomitantly generated with the construction of electron-deficient Cu sites. The H–Cl bond of HCl can be activated over the tribasic copper chloride, accelerating the surface reaction of vinyl chloride production. This strategy of inducing electron deficiency provides new insight into the rational design of catalysts for the synthesis of vinyl chloride with a high catalytic performance.

关键词： C≡C bond Acetylene hydrochlorination Cu sites Tribasic copper chloride Electron-deficient

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乙醇脱氢合成乙酸乙酯催化剂的研究进展

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化工生产与技术 2024年第3期30卷 19-24,I0003页

作者：樊潮锦曹羽余灿陈苑萍江大好李小年浙江工业大学化学工程学院杭州310014

阐述了乙醇脱氢合成乙酸乙酯的典型反应机理,并重点综述了近年来乙醇脱氢合成乙酸乙酯领域铜(Cu)基催化剂(Cu-铬(Cr)、Cu-锆(Zr)、Cu-锌(Zn)体系)、贵金属催化剂以及其他催化剂体系的研究进展,分析表明,Cu基催化剂在催化性能、制造成本... 详细信息

阐述了乙醇脱氢合成乙酸乙酯的典型反应机理,并重点综述了近年来乙醇脱氢合成乙酸乙酯领域铜(Cu)基催化剂(Cu-铬(Cr)、Cu-锆(Zr)、Cu-锌(Zn)体系)、贵金属催化剂以及其他催化剂体系的研究进展,分析表明,Cu基催化剂在催化性能、制造成本等方面展现出了更为显著的优势。乙醇脱氢合成乙酸乙酯Cu基催化剂未来的研究方向主要集中在催化剂组成及各组分含量、催化剂制备方法与条件以及结合各类表征技术与理论计算加深对催化剂构效关系的认识等。

关键词：乙醇脱氢乙酸乙酯催化剂研究进展

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