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学者姓名：陈晶晶
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Abstract ：
Lithium bis(fluorosulfonyl)imide (LiFSI) is a promising electrolyte for lithium-ion batteries. However, the lithiation reaction during the LiFSI synthesis process is accompanied by a LiFSI hydrolysis reaction, which negatively affects the LiFSI yield and poses potential safety risks. In this study, we delve into the reaction equilibrium and hydrolysis behavior during the lithiation reaction and identify that the high temperature and strong alkali used in the reactive distillation process are the key factors leading to LiFSI hydrolysis. As a solution, a novel method for effectively synthesizing LiFSI using reaction-extraction coupling method is proposed and rigorously tested for various factors, including temperature, alkali equivalent, type of solvent, and dosage. The research culminated in developing a multistage continuous membrane extraction process, which achieves a remarkable conversion of over 99.7 % and minimizes LiFSI hydrolysis to less than 0.05 %.
Keyword ：
Hydrolysis Hydrolysis LiFSI LiFSI Lithiation Lithiation Reaction-extraction coupling method Reaction-extraction coupling method Sequential synthesis Sequential synthesis
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| GB/T 7714 | Zhou, Shouquan , Liu, Yan , Ren, Fengjiao et al. Efficient synthesis of LiFSI based on Reaction-Extraction coupling method [J]. | SEPARATION AND PURIFICATION TECHNOLOGY , 2025 , 362 . |
| MLA | Zhou, Shouquan et al. "Efficient synthesis of LiFSI based on Reaction-Extraction coupling method" . | SEPARATION AND PURIFICATION TECHNOLOGY 362 (2025) . |
| APA | Zhou, Shouquan , Liu, Yan , Ren, Fengjiao , Zhang, Siyu , Shi, Xueying , Wu, Bin et al. Efficient synthesis of LiFSI based on Reaction-Extraction coupling method . | SEPARATION AND PURIFICATION TECHNOLOGY , 2025 , 362 . |
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In the burgeoning sucralose (TGS) production, the separation bottleneck has hindered its further technology upgrading. In this work, the crystal structural of sucrose-6-acetate chlorination product 4,1 ',6 '-trichlorosucrose-6- acetate hydrate (TSA-6.2H2O) from multi-step recrystallization has been determined, thus the bad separation efficiency of the chlorination process was assigned to the easy incorporation of by-products into the cavities or local defects of the respirable TSA-6.2H2O network. Based on this mechanism, the second cheap organic solvents have been pre-embedded into TSA-6.2H2O to generate stable ternary solvates, i. e. TSA-6.H2Osecond solvent (second solvent = DMF (N,N'-dimethylformamide), DMAc (N, N'-dimethylacetamide), and NMP (N-methyl-2pyrrolidone)). Their cellular-type compacted arrangements were constructed from strong hydrogen bonding interactions between H2O.second solvent guests and TSA-6 networks. Consequently, the free space or local defects for the encapsulation of impurities could be inhibited completely. Upon the optimization of the crystallized process (H2O: NMP = 7: 3, solvent: TSA-6 = 12: 1, operating temperature: 288.2 K), high TSA-6 purity (99.74 % wt) and low sum of alpha x (0.023) can be achieved. Furthermore, under the guidance of ternary phase diagrams (TPD), the second solvents could be facilely removed by modulating the H2O/second solvent ratio (TSA-6 purity: 99.91 % wt in 0.5 h). In all, the clarification on the obscure mechanism and the strategy of pre-embedding second solvents have broken the separation bottleneck in TGS production, which can also be applied in other relative glycosyl halides industries.
Keyword ：
1 ' 1 ' 6 ' -trichlorosucrose-6-acetate 6 ' -trichlorosucrose-6-acetate Hydrogen bond framework Hydrogen bond framework Selective separation by solvation-induced Selective separation by solvation-induced Separation mechanism Separation mechanism Ternary phase diagrams Ternary phase diagrams
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| GB/T 7714 | Chen, Xiaoping , Lei, Jiayan , Lv, Zhoulin et al. Breaking separation bottleneck in sucralose production: Clarifying the obscure mechanism and pre-embedding second solvents for highly selective separation of chlorinated product [J]. | CHEMICAL ENGINEERING JOURNAL , 2025 , 504 . |
| MLA | Chen, Xiaoping et al. "Breaking separation bottleneck in sucralose production: Clarifying the obscure mechanism and pre-embedding second solvents for highly selective separation of chlorinated product" . | CHEMICAL ENGINEERING JOURNAL 504 (2025) . |
| APA | Chen, Xiaoping , Lei, Jiayan , Lv, Zhoulin , Chen, Zi'ang , Lin, Shitong , Guo, Zhenming et al. Breaking separation bottleneck in sucralose production: Clarifying the obscure mechanism and pre-embedding second solvents for highly selective separation of chlorinated product . | CHEMICAL ENGINEERING JOURNAL , 2025 , 504 . |
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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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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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Abstract ：
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 phi>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.
Keyword ：
CFD CFD Macromixing Macromixing Micromixing Micromixing MOFR MOFR Vortex Vortex
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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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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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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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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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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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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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