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Rare earth metal based DES assisted the VPO synthesis for n-butane selective oxidation toward maleic anhydride

Green Energy & Environment 2023年第6期8卷 1737-1752页

作者： Muhammad Faizan Yingwei Li Xingsheng Wang Piao Song Ruirui Zhang Ruixia Liu Beijing Key Laboratory of Ionic Liquids Clean Process CAS Key Laboratory of Green Process and EngineeringState Key Laboratory of Multiphase Complex SystemInstitute of Process Engineering Chinese Academy of SciencesBeijing100190China University of Chinese Academy of Sciences Beijing100049China Zhengzhou Institute of Emerging Industrial Technology Zhengzhou450000China

Deep eutectic solvents(DESs) are now considered a new class of ionic liquid analogs that have been generously used in various ***, vanadium phosphorus oxide(VPO) catalysts are synthesized in combination with a deep eutectic solvent containing rare earth metal(rE-DES), and their catalytic performance in n-butane selective oxidation to produce maleic anhydride(MA) is evaluated. The rE-DES is produced from the interaction of choline chloride(ChCl) and rare earth metal salts(Cerium, Europium, Lanthanum, and Samarium metal salt)(ChCl:rE = 1:0.5–1:3) under mild conditions. It was found that DESs served as structural modifiers and electronic promoters during VPO synthesis. It regulated the chemical state of the catalyst surface, such as the vanadium valence state, acid-base properties, and ratios of V^(4+)/V^(5+),Lat–O/Sur–O and P/V. Various characterization techniques, such as FT-IR, DSC, XRD, SEM, EDS, TEM, Raman, TGA, NH3-TPD, and XPS,were used to examine its physical and chemical characteristics. These characteristics were correlated with the catalytic performance. The VPO catalyst modified by rE-DES showed a significant enhancement of n-butane conversion and MA selectivity while suppressing the selectivity of CO and CO_(2)as well as the CO/CO_(2)ratio compared to the unpromoted VPO catalyst. Especially for Ce-DES-VPO, it increased the n-butane conversion and MA mass yield up to approximately 11% and 10%, respectively. In addition, we evaluated the catalytic performance under different activation atmospheres.

关键词： earth anhydride vanadium

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Progress of vanadium phosphorous oxide catalyst for n-butane selective oxidation

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Chinese Journal of Chemical Engineering 2022年第3期35卷 297-315页

作者： Muhammad Faizan Yingwei Li Ruirui Zhang Xingsheng Wang Piao Song Ruixia Liu Beijing Key Laboratory of Ionic Liquids Clean Process State Key Laboratory of Multiphase Complex SystemInstitute of Process Engineering Chinese Academy of SciencesBeijing 100190China University of Chinese Academy of Sciences Beijing 100049China

The utilization of lighter alkanes into useful chemical products is essential for modern chemistry and reducing the CO_(2)***,n-butane has gained special attention across the globe due to the abundant production of maleic anhydride(MA).Vanadium phosphorous oxide(VPO)is the most effective catalyst for selective oxidation of n-butane to MA so ***,the VPO complex exists in more or less fifteen different structures,each one having distinct phase composition and exclusive surface morphology and physiochemical properties such as valence state,lattice oxygen,acidity etc.,which relies on precursor preparation method and the activation conditions of *** catalytic performance of VPO catalyst is improved by adding different promoters or co-catalyst such as various metals dopants,or either introducing template or structural-directing ***,new preparation strategies such as electrospinning,ball milling,hydrothermal,barothermal,ultrasound,microwave irradiation,calcination,sol-gel method and solvothermal synthesis are also employed for introducing improvement in catalytic *** in above-mentioned different aspects will be ascribed in current review in addition to summarizing overall catalysis activity and final *** analyze the performance of the catalytic precursor,the reaction mechanism and reaction kinetics both are discussed in this review to help clarify the key issues such as strong exothermic reaction,phosphorus supplement,water supplement,deactivation,and air/n-butane pretreatment *** to the various industrial applications of VPO.

关键词： N-butane selective oxidation Oxidation of light alkanes Vanadium phosphorus oxide(VPO) Maleic anhydride

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Major challenges and recent advances in characterizing biomass thermochemical reactions

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Resources Chemicals and Materials 2024年第2期3卷 146-158页

作者： Zhennan Han Junrong Yue Xi Zeng Jian Yu Fang Wang Yu Guan Xuejing Liu Fu Ding Liangliang Fu Xin Jia Xingfei Song Chao Wang Yanbin Cui Lei Shi Kangjun Wang Vladimir Zivkovic Dingrong Bai Guangwen Xu Key Laboratory on Resources Chemicals and Material of Ministry of Education Shenyang University of Chemical TechnologyShenyang 110142China The State Key Laboratory of Multi-phase Complex System Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China School of Ecology and Environment Beijing Technology and Business UniversityBeijing 100048China School of Engineering Newcastle UniversityNewcastle Upon Tyne NE17RUUnited Kingdom

Thermochemical conversions are pathways for biomass utilization to produce various value-added energy and chemical products. For the development of novel thermochemical conversion technologies, an accurate understanding of the reaction performance and kinetics is essential. Given the diversity of the thermal analysis techniques, it is necessary to understand the features and limitations of the reactors, ensuring that the selected thermal analysis reactor meets the specific need for reaction characterization. This paper provides a critical overview of the thermal analysis reactors based on the following perspectives: 1) gas flow conditions in the reactor, 2) particle’s external and internal heat and mass transfer limitations, 3) heating rate, 4) temperature distribution, 5) nascent char production and reaction, 6) liquid feeding and atomization, 7) simultaneous sampling and analyzing of bed materials, and 8) reacting atmosphere change. Finally, prospects and future research directions in the development of analysis techniques are proposed.

关键词： Biomass Thermal analysis Quick heating Thermochemical reaction Reaction kinetics

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Micro reactors for measurement and analysis of thermochemical gas-solid reactions

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Resources Chemicals and Materials 2022年第2期1卷 152-166页

作者： Zhennan Han Junrong Yue Chao Wang Xi Zeng Jian Yu Fang Wang Yu Guan Xuejing Liu Fu Ding Liangliang Fu Xin Jia Xingfei Song Dingrong Bai Guangwen Xu Key Laboratory on Resources Chemicals and Material of Ministry of Education Shenyang University of Chemical TechnologyShenyang 110142China The State Key Laboratory of Multi-phase Complex System Institute of Process EngineeringChinese Academy of ScienceBeijing 100190China School of Ecology and Environment Beijing Technology and Business UniversityBeijing 100048China

Micro reactors are the essential part of thermal analysis techniques for characterizing gas-solid thermochemical reactions. The dynamic and diversified needs for investigating various complex materials and gas-solid reactions have led to the development of a variety of different microreactors over the years. Solid particles in microreactors are normally heated by furnaces from outside, resistive elements from inside, direct contact with bed particles, or other non-resistively methods. Solid particles can be fixed or fluidized in reactors where gas-solid contacts vary from diffusion-dominated to nearly diffusion-free conditions. Based on these characteristics, in this article we presented a broad classification for microreactors used for thermal analysis of gas-solid reactions. For each of the most popularly used microreactors, their features and limitations are briefly reviewed. By addressing the diversity of the microreactors used in the field of thermal analysis, the review aims at providing general guidance for the selection and operation of the microreactor to satisfy one's practical specific needs.

关键词： Microreactors Thermal analysis Gas-solid reaction Kinetics Mechanism

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ReaxFF molecular dynamic simulation of primary and secondary reactions involving in sub-bituminous coal pyrolysis for tar production

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Carbon Resources Conversion 2021年第1期4卷 230-238页

作者： Yanan Qian Jin-Hui Zhan Wei Xu Zhennan Han Xiaoxing Liu Guangwen Xu State Key Laboratory of Safety and Control for Chemicals SINOPEC Research Institute of Safety Engineering Co.Ltd.Qingdao 266071China State Key Laboratory of Multiphase Complex System Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Key Laboratory on Resources Chemicals and Materials of Ministry of Education of China Shenyang University of Chemical TechnologyShenyang 110142China

ReaxFF molecular dynamic simulation combined with experimental verification was performed to understand the overall reaction mechanism,especially the primary and secondary reactions involving in tar formation of sub-bituminous coal *** relationship at atomic level is clarified between bond breakage of functional groups and products generation,revealing that the amount and order in forming each product are subject to the number of corresponding functional groups and their bond energies *** primary breakage of-C-O-and-C-C-bridge-bonds present in initial coal macromolecular generates molecular of heavy tar,whereas heavy tar can be converted into light tar through cracking side chain of aromatic rings and cyclic hydrocarbons at increased pyrolysis *** very high temperatures the cracking of short-chain hydrocarbons and residual atoms connecting to aromatic rings further occurs to generate light tar and *** remaining aromatic-ring fragments of heavy tar are likely cross-linked to form ***,the simultaneous evolution tendency of tar yield and tar quality under different pyrolysis temperatures and heating rates is obtained at molecular *** obtaining high yield and quality of tar,appropriately high temperature as well as suitable heating rate are needed to compromise the high yield of primary tar and high quality of secondarily upgraded products.

关键词： ReaxFF MD simulation Sub-bituminous coal pyrolysis Reaction paths Primary formation Secondary upgrading

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Insight into Reaction Performance and Product Formation in a Novel Coal Pyrolyzer of Pilot-Scale Test

SSRN

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SSRN 2023年

作者： Qian, Yanan An, Ping Jia, Xin Han, Zhennan Wu, Rongcheng Liu, Xiaoxing Xu, Guangwen State Key Laboratory of Chemical Safety SINOPEC Research Institute of Safety Engineering Co. Ltd. Qingdao266071 China Key Laboratory on Resources Chemicals and Materials of Ministry of Education of China Shenyang University of Chemical Technology Shenyang110142 China State Key Laboratory of Multiphase Complex System Institute of Process Engineering Chinese Academy of Sciences Beijing100190 China Graduate School of Science and Technology China College of Chemical Engineering China

The pyrolysis behavior of coal in a pilot-scale moving bed with internals is modeled through computational fluid dynamics (CFD) simulations. The temperature field, reaction field, volatile flow paths inside the reactor, and effects of the internal design and operating parameters on the tar yield are systematically investigated. The simulation results show that the central gas channel allows the majority of generated volatiles to laterally pass through the low-temperature bed layer. This not only enhanced the primary volatile generation reaction but also significantly reduced the secondary cracking of tar. However, the placement of the heat transfer plates had a dual effect. While the plates significantly enhanced heat transfer, thereby promoting primary reactions, they could cause the volatiles to bend towards the high-temperature zone near the plates, resulting in the partial loss of tar. The tar yield may decrease with an increase in the number or area of heat transfer plates. Furthermore, investigations into the operational parameters revealed that increasing the furnace temperature appropriately and reducing the mass flux of coal were favorable for the heat transfer and yield increase in tar. © 2023, The Authors. All rights reserved.

关键词： Computational fluid dynamics

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Modeling of co-current and counter-current bubble columns with an extended EMMS approach

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Particuology 2019年第3期17卷 126-135页

作者： Xiaoping Guan Ning Yang State Key Laboratory of Multi-phase Complex System Institute of Process Engineering Chinese Academy of Sciences P.O. Box 353 Beijing 100190 China

Bubble columns can be operated in semi-batch, co-current or counter-current mode. This study attempts to extend the dual-bubble-size (DBS) model, viz., the energy-minimization multi-scale (EMMS) model for gas-liquid systems, to co-current and counter-current bubble columns. With the increase of superficial liquid velocity, the predicted total gas holdup and regime transition are in accordance with experiments. A DBS drag model was then developed and incorporated into the CFD simulation. The total gas holdup and local gas holdup radial distribution in both the co-current and counter-current bubble columns are well estimated. The findings in the present work demonstrate that developing closure laws through the stability condition is of great significance in modeling complicated multi-scale flow in bubble columns.

关键词： Co-current Counter-current Bubble columns CFD Drag model

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A new method of Ionic Fragment Contribution-Gradient Boosting Regressor for predicting the infinite dilution activity coefficient of dichloromethane in ionic liquids

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Fluid phase Equilibria 2023年 564卷

作者： Li, Kaikai Chang, Fei Shi, Sensen Jiang, Chongyang Bai, Yinge Dong, Haifeng Meng, Xianghai Wu, Jeffery C.S. Zhang, Xiangping CAS Key Laboratory of Green Process and Engineering State Key Laboratory of Multiphase Complex System Beijing Key Laboratory of Ionic Liquids Clean Process Institute of Process Engineering Chinese Academy of Sciences Beijing 100190 China College of Chemical and Engineering University of Chinese Academy of Sciences Beijing 100049 China College of Chemical Engineering and Environment China University of Petroleum Beijing 102249 China Langfang Green Industrial Technology Center Langfang06500 China Department of Chemical and Engineering National Taiwan University Taipei10617 Taiwan

Ionic liquids (ILs) have shown huge potential advantages as solvents to absorb and recover dichloromethane (DCM) from waste gasses. The infinite dilution activity coefficient (γ∞) of DCM in ILs is an important parameter, which can be used to predict the vapor-liquid equilibrium of DCM-IL systems. In this work, a new model of calculating the γ∞ of DCM in ILs is established based on ionic fragments contribution (IFC) and gradient boosting regressor (GBR) algorithm. IFC is used to obtain the surface charge density distribution area of ILs (Sσ-profile) that is the input of GBR. GBR is used to learn the mapping relationship between input feature and γ∞ of DCM in ILs. The database of the γ∞ of DCM in ILs composed of 29 cations and 22 anions includes 72 experimental data and 421 COSMO calculation data, which was employed to establish the IFC-GBR model and predict the γ∞ of DCM in ILs. The coefficient of determination (R2) and mean absolute error (MAE) of the IFC-GBR model test set are 0.9703 and 0.0519, respectively. Also, this model has excellent generalization capability of predicting evidenced by high 10-fold cross-validation coefficients of determination in the range 0.9474–0.9481. These results indicate that the proposed model can accurately predict γ∞ of DCM in ILs, then provide the important data for developing a new process of absorbing and desorbing DCM by IL-based technologies. © 2022

关键词： Ionic liquids

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Improved thermal conductivity of epoxy resin by graphene-nickel three-dimensional filler

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Carbon Resources Conversion 2020年第1期3卷 29-35页

作者： Yanjie Liu Jiangyin Lu Yanbin Cui State Key Laboratory of Multiphase Complex System Institute of Process EngineeringChinese Academy of SciencesBeijing 100190China Zhengzhou Institute of Emerging Industrial Technology ZhengzhouHenan 450000China Key Laboratory of Oil&Gas Fine Chemicals Ministry of EducationCollege of Chemistry and Chemical EngineeringXinjiang UniversityUrumqi 830046China Dalian National Laboratory for Clean Energy Dalian 116023China

Owing to high thermal conductivity,carbon nanotube and graphene have been used as nanofillers to improve the thermal conductivity of ***,the agglomeration of nanofillers in polymer inhibits their applications in improving the thermal conductivity of *** overcome this problem,graphene was grown on Ni foam by chemical vapor deposition in this *** graphene-nickel three-dimensional filler was added into epoxy resin to improve the thermal conductivity of epoxy *** foam can prevent the agglomeration of graphene in epoxy resin and a thermally conductive network by graphene and Ni foam was formed in epoxy *** adding graphene-nickel three-dimensional filler into epoxy resin,the thermal conductivity of graphene-nickel/epoxy composite can reach up to 2.6549 W⋅m^(-1)⋅k^(-1),which was 9 times higher than that of raw epoxy resin.

关键词： Epoxy resin Graphene Ni foam Thermal conductivity Composite

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Characteristics of gas-solid micro fluidized beds for thermochemical reaction analysis

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Carbon Resources Conversion 2020年第1期3卷 203-218页

作者： Zhennan Han Junrong Yue Xi Zeng Jian Yu Fang Wang Shaozeng Sun Hong Yao Guangqian Luo Xuejing Liu Yining Sun Fu Ding Liangliang Fu Lei Shi Kangjun Wang Jiebin Yang Shaonan Wang Xueqing Chen Dingrong Bai Guangwen Xu Key Laboratory on Resources Chemicals and Material of Ministry of Education Shenyang University of Chemical TechnologyShenyang 110142China The State Key Laboratory of Multi-phase Complex System Institute of Process EngineeringChinese Academy of ScienceBeijing 100190China Combustion Engineering Research Institute School of Energy Science and EngineeringHarbin Institute of TechnologyHarbin 150001China State Key Laboratory of Coal Combustion Huazhong University of Science and TechnologyWuhan 430074China National Institute of Measurement and Technology Chengdu 610021China

Fuel conversion and clean energy reaction systems involve a variety of catalytic and non-catalytic gas-solid thermochemical reactions.A good understanding of the correct reaction mechanism and kinetics,as well as the profiles of reaction products,is of great significance to the development,design,and operation of such reaction *** micro fluidized bed reaction analysis provides an efficient and reliable method to acquire this essential information with low capital and operating costs,low energy consumption and enhanced *** paper provides an overview of the system and its characteristics for the micro fluidized bed reaction analyzer that has been well proven to be a reliable new approach as well as an instrument for characterizing various gas-solid thermochemical reactions.

关键词： Micro fluidized bed Reaction kinetic analysis Isothermal differential reactor Thermochemical reaction characterization

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