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学者姓名：陈晶晶
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Abstract ：
Dehydroxylation of biomass-based platform molecules is critical for obtaining building blocks for use in the chemical industry. Acid catalytic dehydration has provided a feasible route. However, simultaneously pursuing high product-selective and ultra-stable catalysts for the dehydroxylation of polyols remains an open challenge. In this study, a strategy for in-situ Bronsted acid sites (BAS) with chemo-adsorption selectivity is proposed. The construction of defect sites B[3] and P[4] species has been proved to be a prerequisite for the dynamic acid site formation at hydrothermal conditions. The BPO4 catalyst with in-situ BAS can achieve the high selectivity of acrolein (similar to 80%) and robust stability of catalyst (over 425 h) using glycerol dehydration as a model reaction. In addition, in-situ BAS is highly selective for secondary hydroxyl groups and has been extended to other substrate applications. This catalytic strategy provides a green, efficient, and economical approach for converting biomassderived polyols to high-value-added chemicals.
Keyword ：
Acrolein Acrolein Biomass Biomass Dehydration Dehydration Glycerol Glycerol In -situ Br onsted acid In -situ Br onsted acid
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| GB/T 7714 | Su, Chenxin , Zhou, Shouquan , Wu, Shaoyun et al. Highly efficient dehydration of polyols: In-situ Brempty setnsted acid from boron phosphate catalyst [J]. | CHEMICAL ENGINEERING JOURNAL , 2024 , 483 . |
| MLA | Su, Chenxin et al. "Highly efficient dehydration of polyols: In-situ Brempty setnsted acid from boron phosphate catalyst" . | CHEMICAL ENGINEERING JOURNAL 483 (2024) . |
| APA | Su, Chenxin , Zhou, Shouquan , Wu, Shaoyun , Gao, Mingbin , Zhang, Weiling , Ma, Zhuang et al. Highly efficient dehydration of polyols: In-situ Brempty setnsted acid from boron phosphate catalyst . | CHEMICAL ENGINEERING JOURNAL , 2024 , 483 . |
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The Microscale Oscillatory Flow Reactor (MOFR) can achieve good plug flow and micromixing performance simultaneously at laminar net flow conditions. An unbaffled U-shaped microreactor coupled with oscillating flow technology was designed to study the macro and micromixing performance. Firstly, the influence of oscillations on the flow performance was studied to reveal the formation rule of vortex. The simulation results showed that the continuous formation and destruction of periodic vortexes occurred in the microreactor with oscillation. With the increase of oscillation intensity, the vortex size in the radial direction first gradually increased and then becomes stable, and gradually moved axially, resulting in axial diffusion. Secondly, the effect of oscillation on the macromixing and micromixing performance were investigated. The results showed that the coupling oscillation could greatly improve the macromixing and micromixing performance. The macromixing and micromixing performance were promoted simultaneously at lower oscillation intensity and then tended to be flat due to the axial diffusion at high oscillation intensity. When φ>6.05, the minimum micromixing time and the maximum number of tanks can be achieved at the same time. At a velocity ratio of about 23, FoM reached a maximum of about 3.5. © 2024
Keyword ：
Computational fluid dynamics Computational fluid dynamics Diffusion Diffusion Laminar flow Laminar flow Oscillating flow Oscillating flow Vortex flow Vortex flow
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| GB/T 7714 | Yu, Liping , Zheng, Meiqin , Wang, Jiawei et al. Enhanced mixing characteristics of unbaffled U-shaped microreactor coupled oscillatory flow [J]. | Chemical Engineering and Processing - Process Intensification , 2024 , 205 . |
| MLA | Yu, Liping et al. "Enhanced mixing characteristics of unbaffled U-shaped microreactor coupled oscillatory flow" . | Chemical Engineering and Processing - Process Intensification 205 (2024) . |
| APA | Yu, Liping , Zheng, Meiqin , Wang, Jiawei , Yan, Zuoyi , Yao, Wei , Li, Haohong et al. Enhanced mixing characteristics of unbaffled U-shaped microreactor coupled oscillatory flow . | Chemical Engineering and Processing - Process Intensification , 2024 , 205 . |
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Sustainable synthesis of acrolein, a key chemical intermediate, from biomass-derived glycerol is highly attractive. However, conventional catalysts for the dehydration of glycerol suffer from low acrolein selectivity and high deactivation tendency. Herein, a novel green catalyst (HPW/T-0.6 S-COOH) was prepared and employed in the dehydration of glycerol in a continuous flow reactor. The performance of different catalysts and the effects of reaction conditions (reaction temperature, N-2 flow rate, and glycerol concentration) were examined. The HPW/T-0.6 S-COOH catalyst provides the best glycerol conversion of 96.38% and acrolein selectivity of 92.01%. The NH3-TPD and pyridine-FTIR results indicate that the Bronsted acid site is more susceptible to acrolein, while the weak strength acid site effectively prevents the further reaction of acrolein, providing practical insights for the rational design of efficient and continuous synthesis of acrolein catalysts.
Keyword ：
Acrolein Acrolein Continuous synthesis Continuous synthesis glycerol dehydration glycerol dehydration HPW/T0.6S-COOH catalyst HPW/T0.6S-COOH catalyst
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| GB/T 7714 | Su, Chen-Xin , Chen, Jing-Jing , Wu, Shao-Yun et al. Continuous dehydration of glycerol to Acrolein based on HPW/TS-COOH catalyzation [J]. | JOURNAL OF FLOW CHEMISTRY , 2023 , 13 (2) : 143-154 . |
| MLA | Su, Chen-Xin et al. "Continuous dehydration of glycerol to Acrolein based on HPW/TS-COOH catalyzation" . | JOURNAL OF FLOW CHEMISTRY 13 . 2 (2023) : 143-154 . |
| APA | Su, Chen-Xin , Chen, Jing-Jing , Wu, Shao-Yun , Li, Shao-Heng , Zhou, Shou-Quan , Zheng, Hui-Dong et al. Continuous dehydration of glycerol to Acrolein based on HPW/TS-COOH catalyzation . | JOURNAL OF FLOW CHEMISTRY , 2023 , 13 (2) , 143-154 . |
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The mild alkali-treated 13X was employed in the liquid phase isomerization reaction of alpha-pinene to increase the yield of limonene. A maximum alpha-pinene conversion of 100% and limonene yield of 59.1% could be achieved. Crystallinity could be well retained, and the amounts of medium-strong acid sites and the distribution of Bronsted and Lewis acid sites could be changed after the mild alkali treatment for 13X zeolite. Samples with higher micropore specific surface area were easier to obtain higher yields of limonene due to shape-selectivity. A proper amount of the medium-strong acid and the synergistic effect of Bronsted and Lewis acid sites were beneficial to enhance the catalytic activity and the yield of monocyclic product limonene. The main reason for catalyst deactivation could be the decrease in the active sites due to soft coke deposition. For the regeneration process, the conversions of alpha-pinene were between 95% and 99% during the first seven cycles and the conversion dropped to 90.6% after the eighth cycle, which demonstrated that the ethanol flushing and calcination could be an effective regeneration method for the 13X catalyst used in the alpha-pinene isomerization reaction.
Keyword ：
13X zeolite 13X zeolite Limonene Limonene Mild alkali treatment Mild alkali treatment ?-pinene isomerization ?-pinene isomerization
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| GB/T 7714 | Su, Chenxin , Luo, Xiheng , Chen, Jingjing et al. Effective synthesis of limonene over mild alkali-modified 13X catalysts in alpha-pinene isomerization [J]. | MICROPOROUS AND MESOPOROUS MATERIALS , 2023 , 348 . |
| MLA | Su, Chenxin et al. "Effective synthesis of limonene over mild alkali-modified 13X catalysts in alpha-pinene isomerization" . | MICROPOROUS AND MESOPOROUS MATERIALS 348 (2023) . |
| APA | Su, Chenxin , Luo, Xiheng , Chen, Jingjing , Wu, Dan , Fan, Lihai , Liu, Jie et al. Effective synthesis of limonene over mild alkali-modified 13X catalysts in alpha-pinene isomerization . | MICROPOROUS AND MESOPOROUS MATERIALS , 2023 , 348 . |
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Catalytic epoxidation of alkenes is an important type of organic reaction in chemical industry, and the deep insight into catalyst deactivation will help to develop new epoxidation process. In this work, series of quaternary ammoniums bearing different cationic sizes, i.e. MTOA' (methyltrioctylammonium, [(C8H17)3CH3N]'), HTMA'(hexadecyltrimethylammonium, [(C16H33)(CH3)3N]') and DMDOA' (dimethyl-dioctadecylammonium, [(C18H37)2(CH3)2N]') were incorporated with polyoxometalate (POM) anions to prepare phase transfer catalysts (PTCs), which were used in the styrene epoxidations. Among them, (MTOA)3PW4O24 exhibits the best catalytic performance judged from the highest styrene conversion rate (52%) and styrene oxide selectivity (93%), during which the styrene epoxidation conditions were opti-mized. Meanwhile, the deactivation mechanism of this kind of PTCs was proposed firstly, i.e. in the case of low H2O2 content, the oxidant can only be used in the styrene epoxidation, in which the catalyst can transform into stable Keggin-type POM. But when the content of H2O2 is higher, the excess H2O2 can re-activate the Keggin-type POM into active (PW4O24)3-anions, which can trigger the ring-opening poly-merization of styrene oxide. Consequently, the catalyst is deactivated by adhered poly(styrene oxide) irreversibly, which was determined by NMR spectra. In this situation, the active moiety {PO4[WO (O2)2]4}3-in phase-transfer catalytic system can break into some unidentified species with low W/P ratio with the presence of epoxides. This work will be beneficial for the design of new PTCs in alkene epoxi-dation in fine chemical industry.(c) 2022 The Chemical Industry and Engineering Society of China, and Chemical Industry Press Co., Ltd. All rights reserved.
Keyword ：
Catalyst deactivation mechanism Catalyst deactivation mechanism Cation size effect Cation size effect Phosphotungstic acid phase-transfer catalyst Phosphotungstic acid phase-transfer catalyst Styrene epoxidation Styrene epoxidation
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| GB/T 7714 | Xiao, Qiongna , Jiang, Yuyan , Yuan, Weiqiang et al. Styrene epoxidation catalyzed by polyoxometalate/quaternary ammonium phase transfer catalysts: The effect of cation size and catalyst deactivation mechanism [J]. | CHINESE JOURNAL OF CHEMICAL ENGINEERING , 2023 , 55 : 192-201 . |
| MLA | Xiao, Qiongna et al. "Styrene epoxidation catalyzed by polyoxometalate/quaternary ammonium phase transfer catalysts: The effect of cation size and catalyst deactivation mechanism" . | CHINESE JOURNAL OF CHEMICAL ENGINEERING 55 (2023) : 192-201 . |
| APA | Xiao, Qiongna , Jiang, Yuyan , Yuan, Weiqiang , Chen, Jingjing , Li, Haohong , Zheng, Huidong . Styrene epoxidation catalyzed by polyoxometalate/quaternary ammonium phase transfer catalysts: The effect of cation size and catalyst deactivation mechanism . | CHINESE JOURNAL OF CHEMICAL ENGINEERING , 2023 , 55 , 192-201 . |
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LiFSI (lithium bis(fluorosulfonyl)imide) is a promising lithium salt for electrolytes in Li-ion batteries. However, the accumulation of harmful gases and heat during LiFSI hydrolysis could lead to serious safety accidents. Here we systematically investigate LiFSI hydrolysis processes under comprehensive conditions: higher temperature/ acidity/basicity and lower water content can accelerate the hydrolysis, whereas the presence of DEC (diethyl carbonate) solvent, and other alkali metals (Na+, K+) can stabilize FSI-. Unexpectedly, under alkaline conditions, temperature/water content could not affect the hydrolysis greatly. By monitoring the hydrolysis intermediates and products using time-dependent ion chromatography, infrared spectra, and nuclear magnetic resonance, the hydrolysis routes are proposed and validated by accelerating rate calorimetry, differential scanning calorimetry measurements, and theoretical calculations. Under neutral/acidic conditions, electrophilic attack on the S-N bond generates FSO2NH2 and FSO3 �, while nucleophilic attack on the S-F bond produces FSO2NSO32 � and SO3NHSO32 � under alkaline conditions. As indicated by DFT calculation, the weaker S-N bond and larger S-N-S angle facilitate the electrophilic attack under acid conditions. Furthermore, very unstable intermediates (FSO2NH2 and CH3CH2OSO3H) are determined for the first time. Based on these hydrolysis mechanisms, stra-tegies for inhibiting LiFSI hydrolysis are provided, which is significant for the high-efficiency production and safe storage/transportation of LiFSI.
Keyword ：
DFT calculation DFT calculation Hydrolysis intermediates Hydrolysis intermediates Hydrolysis mechanism Hydrolysis mechanism Lithium bis(fluorosulfonyl)imide Lithium bis(fluorosulfonyl)imide
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| GB/T 7714 | Zhou, Shouquan , Zhang, Siyu , Wang, Shang et al. Direct evidences for bis(fluorosulfonyl)imide anion hydrolysis in industrial production: Pathways based on thermodynamics analysis and theoretical simulation [J]. | JOURNAL OF POWER SOURCES , 2023 , 577 . |
| MLA | Zhou, Shouquan et al. "Direct evidences for bis(fluorosulfonyl)imide anion hydrolysis in industrial production: Pathways based on thermodynamics analysis and theoretical simulation" . | JOURNAL OF POWER SOURCES 577 (2023) . |
| APA | Zhou, Shouquan , Zhang, Siyu , Wang, Shang , Zhang, Weiling , Liu, Yan , Lin, Hui et al. Direct evidences for bis(fluorosulfonyl)imide anion hydrolysis in industrial production: Pathways based on thermodynamics analysis and theoretical simulation . | JOURNAL OF POWER SOURCES , 2023 , 577 . |
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Unbaffled U-shaped mesoscale oscillatory flow reactors (meso-OFRs) were developed to prevent solid deposition and prepare uniform barium sulfate (BaSO4) nanoparticles with environmental protection function. The results showed that the oscillation significantly reduced granular deposition; the greater the intensity of the oscillation, the faster it reached uniformity, and the less likely the granules were to be deposited. These results can be explained by the formation of a larger vortex size, which can strengthen the turbulent mixing of fluid in the reactor, promote the interaction and forced mixing between the liquid phase and solid particles, enhance the internal shear stress of the fluid, and contribute to the secondary suspension of solid particles and the disintegration of particle agglomeration. The prepared BaSO4 nanoparticles with oscillation were smaller in size and lower in pressure drop than those produced without oscillation, which conclusively illustrated that oscillation effectively prevented channel deposition and clogging.
Keyword ：
BaSO 4 nanoparticles BaSO 4 nanoparticles Granular deposition Granular deposition Liquid -solid two-phase flow Liquid -solid two-phase flow Meso-OFR Meso-OFR Vortex Vortex
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| GB/T 7714 | Zheng, Meiqin , Liu, Jianchen , Tian, Linda et al. Unbaffled mesoscale reactor coupled oscillatory flow-enhanced liquid-solid two-phase flow [J]. | POWDER TECHNOLOGY , 2023 , 434 . |
| MLA | Zheng, Meiqin et al. "Unbaffled mesoscale reactor coupled oscillatory flow-enhanced liquid-solid two-phase flow" . | POWDER TECHNOLOGY 434 (2023) . |
| APA | Zheng, Meiqin , Liu, Jianchen , Tian, Linda , Yan, Zuoyi , Zhou, Caijin , Li, Haohong et al. Unbaffled mesoscale reactor coupled oscillatory flow-enhanced liquid-solid two-phase flow . | POWDER TECHNOLOGY , 2023 , 434 . |
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The aspect ratio modulation in the alcoholysis process is highly significant for the production of high-quality sucralose. In this work, antisolvent crystallization (ASC) accompanied by preferred orientation was first adopted in the sucralose separation, based on which simultaneous modulations on aspect ratio, solubility, and stability have been realized. In detail, after the alcoholysis process in methanol, four antisolvents bearing different functional groups were used in ASC, i.e., isopentanol (IPN), isovaleraldehyde (IVD), isovaleric acid (IVA), and isobutyl propionate (IBP). To our interest, when IVA was used as the antisolvent, the highest separation efficiency (49.33%), fastest crystallizing rate (5.64%/h), lowest aspect ratio (1.55), and solubility (9.28 wt %) and good thermal stability (131.65 degrees C) of sucralose were achieved. Single crystal structures of sucralose using different antisolvents have been determined. Sucralose using IVA as the antisolvent exhibits the greatest molecular distortion and strongest intermolecular C-HCl hydrogen bonds; thus, the preferred growth along {002}/{011} directions has occurred and accounted for its lower aspect ratio, worse solubility, and better stability. The strongest methanolIVA interactions due to the presence of a carboxyl group can accelerate the formation of the emulsion, resulting in the fastest crystallizing rate. The antisolvent screening and the discovery about relative mechanisms will provide a theoretical guide for the production of high-quality sucralose.
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| GB/T 7714 | Xu, Qiaoyan , Lv, Zhoulin , Chen, Xiaoping et al. Aspect Ratio Modulation of Sucralose through {002}/{011} Preferred Orientation in Antisolvent Crystallization [J]. | ACS OMEGA , 2023 , 8 (44) : 41145-41155 . |
| MLA | Xu, Qiaoyan et al. "Aspect Ratio Modulation of Sucralose through {002}/{011} Preferred Orientation in Antisolvent Crystallization" . | ACS OMEGA 8 . 44 (2023) : 41145-41155 . |
| APA | Xu, Qiaoyan , Lv, Zhoulin , Chen, Xiaoping , Li, Shaoheng , Huang, Changqi , Chen, Jingjing et al. Aspect Ratio Modulation of Sucralose through {002}/{011} Preferred Orientation in Antisolvent Crystallization . | ACS OMEGA , 2023 , 8 (44) , 41145-41155 . |
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本发明提供了一种三氯蔗糖‑6‑乙酸酯生产工艺：向一次蒸馏得到的蔗糖乙酸酯浓缩液中加入冰醋酸与第一有机溶剂混合溶液，得到蔗糖‑6‑乙酸酯与乙酸的白色共晶体粉末；将共结晶体均匀分散在第二有机溶剂中，加入有机胺处理，使之与乙酸反应形成稳定的化学键，从共晶体骨架中夺取乙酸，对于残留的有机胺以及形成的乙酸‑有机胺结合物使用第二有机溶剂洗涤，烘干完全后获得大于99.8%的蔗糖‑6‑乙酸酯粉末；并将该粉末溶解于N, N‑二甲基甲酰胺溶液中，应用于下一步区域选择性氯代反应，消除了杂质对氯代反应过程的不良影响，提升了氯代收率，简化了三氯蔗糖‑6‑乙酸酯提纯过程，提高了最终三氯蔗糖的产品品质，具有更好的工业价值。
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| GB/T 7714 | 郑辉东 , 陈小平 , 陈子昂 et al. 一种三氯蔗糖-6-乙酸酯生产工艺 : CN202210020727.0[P]. | 2022-01-10 00:00:00 . |
| MLA | 郑辉东 et al. "一种三氯蔗糖-6-乙酸酯生产工艺" : CN202210020727.0. | 2022-01-10 00:00:00 . |
| APA | 郑辉东 , 陈小平 , 陈子昂 , 陈晶晶 , 林诗童 , 李少恒 et al. 一种三氯蔗糖-6-乙酸酯生产工艺 : CN202210020727.0. | 2022-01-10 00:00:00 . |
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本发明公开了一种甘油脱水催化剂及其制备方法和应用，该方法通过浸渍法制备了一种负载型磷酸硼催化剂。在固定床反应器中，反应温度为280~360℃，10%~30%的甘油水溶液为原料，以该催化剂催化甘油脱水反应，甘油转化率100%，丙烯醛选择性可达76%，羟基丙酮选择性达15%。并且该催化剂具有良好的稳定性，可以反应200h未明显失活。并且经过简单再生处理，可快速恢复催化剂活性。本发明提供的催化剂，制备工艺简单，易于工业化，为生物甘油转化为高附加值产品提供了一条良好的道路。
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| GB/T 7714 | 郑辉东 , 苏晨欣 , 周守泉 et al. 一种甘油脱水催化剂及其制备方法和应用 : CN202210060922.6[P]. | 2022-01-19 00:00:00 . |
| MLA | 郑辉东 et al. "一种甘油脱水催化剂及其制备方法和应用" : CN202210060922.6. | 2022-01-19 00:00:00 . |
| APA | 郑辉东 , 苏晨欣 , 周守泉 , 吴乃昕 , 刘杰 , 陈晶晶 . 一种甘油脱水催化剂及其制备方法和应用 : CN202210060922.6. | 2022-01-19 00:00:00 . |
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