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Enhancement of liquideliquid micromixing performance in curved capillary microreactor by generation of Dean vortices

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Chinese Journal of Chemical Engineering 2024年第4期68卷 76-82页

作者： Shaoyun Wu Zhuang Ma Zichi Yang Suying Zhao Caijin Zhou Huidong Zheng Fujian Engineering Research Center of Advanced Manufacturing Technology for Fine Chemicals College of Chemical EngineeringFuzhou UniversityFuzhou 350108China qingyuan innovation laboratory Quanzhou362114China

Micromixing efficiency is an important parameter for evaluating the multiphase mass transfer performance and reaction efficiency of microreactors.In this work,the novel curved capillary reactor with different shapes was designed to generate Dean flow,which was used to enhance the liquideliquid micromixing performance.The VillermauxeDushman probe reaction was employed to characterize the micromixing performance in different curved capillary microreactors.The effects of experiment parameters such as liquid flow rate,inner diameter,tube length,and curve diameter on micromixing performance were systematically investigated.Under the optimal conditions,the minimum value of the segmentation factor XS was 0.008.It was worth noting that at the low Reynolds number(Re<30),the change of curved shape on the capillary microreactor can significantly improve the micromixing performance with XS reduced by 37.5%.Further,the correlations of segment index XS with dimensionless factor such as Reynolds number or Dean number were developed,which can be used to predict the liquide liquid micromixing performance in capillary microreactors.

关键词： Microreactor Process intensification Micromixing performance Dean flow

Efficient and reversible separation of NH_(3) by deep eutectic solvents with multiple active sites and low viscosities

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Chinese Journal of Chemical Engineering 2024年第3期67卷 97-105页

作者： Jiayin Zhang Lu Zheng Siqi Fang Hongwei Zhang Zhenping Cai Kuan Huang Lilong Jiang National Engineering Research Center of Chemical Fertilizer Catalyst(NERC-CFC) College of Chemical EngineeringFuzhou UniversityFuzhou 350002China qingyuan innovation laboratory Quanzhou 362801China

The efficient separation and collection of ammonia(NH_(3))during NH_(3) synthesis process is essential to improve the economic efficiency and protect the environment.In this work,ethanolammonium hydrochloride(EtOHACl)and phenol(PhOH)were used to prepare a novel class of deep eutectic solvents(DESs)with multiple active sites and low viscosities.The NH_(3) separation performance of EtOHACl+PhOH DESs was analyzed completely.It is figured out that the NH_(3) absorption rates in EtOHACl+PhOH DESs are very fast.The NH_(3) absorption capacities are very high and reach up to 5.52 and 10.74 mol·kg1 at 11.2 and 100.4 kPa under 298.2 K,respectively.In addition,the EtOHACl+PhOH DESs present highly selective absorption of NH_(3) over N_(2) and H_(2) and good regenerative properties after seven cycles of absorption/desorption.The intrinsic separation mechanism of NH_(3) by EtOHACl+PhOH DESs was further revealed by spectroscopic analysis and quantum chemistry calculations.

关键词： Separation Absorption Ionic liquid Deep eutectic solvent Multiple active site Low viscosity

Facile synthesis of hierarchical NaX zeolite from natural kaolinite for efficient Knoevenagel condensation

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Chinese Journal of Chemical Engineering 2024年第1期65卷 75-84页

作者： Wen Xiao Peng Dong Chan Wang Jingdong Xu Tiesen Li Haibo Zhu Tinghai Wang Renwei Xu Yuanyuan Yue National Engineering Research Center of Chemical Fertilizer Catalyst College of Chemical EngineeringFuzhou UniversityFuzhou 350108China qingyuan innovation laboratory Quanzhou 362801China Sinochem Quanzhou Energy Technology Co. Ltd.Quanzhou 362000China

Zeolite catalysts have found extensive applications in the synthesis of various fine chemicals.However,the micropores of zeolites impose diffusion limitations on bulky molecules,greatly reducing the catalytic efficiency.Herein,we explore an economic and environmentally friendly method for synthesizing hierarchical NaX zeolite that exhibits improved catalytic performance in the Knoevenagel condensation reaction for producing the useful fine chemical 2-cyano-3-phenylacrylate.The synthesis was achieved via a low-temperature activation of kaolinite and subsequent in-situ transformation strategy without any template or seed.Systematic characterizations reveal that the synthesized NaX zeolite has both intercrystalline and intra-crystalline mesopores,smaller crystal size,and larger external specific surface area compared to commercial NaX zeolite.Detailed mechanism investigations show that the inter-crystalline mesopores are generated by stacking smaller crystals formed from in-situ crystallization of the depolymerized kaolinite,and the intra-crystalline mesopores are inherited from the pores in the depolymerized kaolinite.This synthesis strategy provides an energy-saving and effective way to construct hierarchical zeolites,which may gain wide applications in fine chemical manufacturing.

关键词： Hierarchical NaX zeolite Template-free synthesis Natural kaolinite Knoevenagel condensation

Online soft measurement for wastewater treatment system based on hybrid deep learning

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Frontiers of Environmental Science & Engineering 2024年第2期18卷 77-89页

作者： Wenjie Mai Zhenguo Chen Xiaoyong Li Xiaohui Yi Yingzhong Zhao Xinzhong He Xiang Xu Mingzhi Huang SCNU Environmental Research Institute Guangdong Provincial Key Laboratory of Chemical Pollution and Environmental Safety&MOE Key Laboratory of Theoretical Chemistry of EnvironmentSchool of EnvironmentSouth China Normal UniversityGuangzhou 510006China Fujian Environmental Protection Design Institute Co.Ltd. Fuzhou 350000China Huashi(Fujian)Environment Technology Co.Ltd. Quanzhou362001China SCNU qingyuan Institute of Science and Technology innovation Co.Ltd. Qingyuan 511517China Econ Technology Co.Ltd. Yantai 265503China

The existing automated wastewater treatment control systems encounter challenges such as the utilization of specialized testing instruments, equipment repair complications, high operational costs, substantial operational errors, and low detection accuracy. An effective soft measure model offers a viable approach for real-time monitoring and the development of automated control in the wastewater treatment process. Consequently, a novel hybrid deep learning CNN-BNLSTM-Attention (CBNLSMA) model, which incorporates convolutional neural networks (CNN), bidirectional nested long and short-term memory neural networks (BNLSTM), attention mechanisms (AM), and Tree-structure Parzen Estimators (TPE), has been developed for monitoring effluent water quality during the wastewater treatment process. The CBNLSMA model is divided into four stages: the CNN module for feature extraction and data filtering to expedite operations;the BNLSTM module for temporal data’s temporal information extraction;the AM module for model weight reassignment;and the TPE optimization algorithm for the CBNLSMA model’s hyperparameter search optimization. In comparison with other models (TPE-CNN-BNLSTM, TPE-BNLSTM-AM, TPE-CNN-AM, PSO-CBNLSTMA), the CBNLSMA model reduced the RMSE for effluent COD prediction by 25.4%, decreased the MAPE by 32.9%, and enhanced the R2 by 14.9%. For the effluent SS prediction, the CBNLSMA model reduced the RMSE by 26.4%, the MAPE by 21.0%, and improved the R2 by 35.7% compared to other models. The simulation results demonstrate that the proposed CBNLSMA model holds significant potential for real-time effluent quality monitoring, indicating its high potential for automated control in wastewater treatment processes.

关键词： Prediction model Soft measurement CNN-BNLSTM-AM model TPE optimization algorithm

An in-situ self-etching enabled high-power electrode for aqueous zinc-ion batteries

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Journal of Energy Chemistry 2024年第1期88卷 399-408,I0009页

作者： Shuang Hou Dingtao Ma Yanyi Wang Kefeng Ouyang Sicheng Shen Hongwei Mi Lingzhi Zhao Peixin Zhang College of Chemistry and Environmental Engineering Shenzhen UniversityShenzhen 518060GuangdongChina Guangdong Provincial Engineering Technology Research Center for Low Carbon and Advanced Energy Materials School of Semiconductor Science and TechnologySouth China Normal UniversityFoshan 528225GuangdongChina SCNU qingyuan Institute of Science and Technology innovation Co. Ltd.Qingyuan 511517GuangdongChina

Sluggish storage kinetics is considered as the main bottleneck of cathode materials for fast-charging aqueous zinc-ion batteries(AZIBs).In this report,we propose a novel in-situ self-etching strategy to unlock the Palm tree-like vanadium oxide/carbon nanofiber membrane(P-VO/C)as a robust freestanding electrode.Comprehensive investigations including the finite element simulation,in-situ X-ray diffraction,and in-situ electrochemical impedance spectroscopy disclosed it an electrochemically induced phase transformation mechanism from VO to layered Zn_(x)V_(2)O_5·nH_(2)O,as well as superior storage kinetics with ultrahigh pseudocapacitive contribution.As demonstrated,such electrode can remain a specific capacity of 285 mA h g^(-1)after 100 cycles at 1 A g^(-1),144.4 mA h g^(-1)after 1500 cycles at 30 A g^(-1),and even 97 mA h g^(-1)after 3000 cycles at 60 A g^(-1),respectively.Unexpectedly,an impressive power density of 78.9 kW kg^(-1)at the super-high current density of 100 A g^(-1)also can be achieved.Such design concept of in-situ self-etching free-standing electrode can provide a brand-new insight into extending the pseudocapacitive storage limit,so as to promote the development of high-power energy storage devices including but not limited to AZIBs.

关键词： In-situ self-etching Free-standing electrode Pseudocapacitive storage High-power Zinc-ion batteries

Controlling reversible complexation-mediated polymerization(RCMP) via deep eutectic solvents: fast kinetics, narrow molecular weight distribution and mechanistic insights

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Science China Chemistry 2024年第8期 2728-2736页

作者： Xin Fu Zhen Lu Shen Li Zheng-Hong Luo Lin-Xi Hou Department of Materials-Oriented Chemical Engineering College of Chemical Engineering Fuzhou University qingyuan innovation laboratory Department of Chemical Engineering School of Chemistry and Chemical Engineering State Key Laboratory of Metal Matrix CompositesShanghai Jiao Tong University Chemical Engineering Zhicheng College of Fuzhou University

The exploitation of new green polymerization avenues for the effective synthesis of polymers by reversible-deactivation radical polymerization plays a critical role in pursuing the development of polymeric materials. In this work, serials of deep eutectic solvents(DES) with intermolecular-hydrogen-bonding interaction were constructed as catalysts and medium for actuating reversible complexation-mediated polymerization(RCMP) for the first time, yielding methacrylate polymers with high monomer conversion and narrow dispersion molecular weight in both water and oil systems. The mechanism and elementary reaction of RCMP were explored deeply, revealing that the complexation of initiator with DES to generate radicals was a ratecontrolling step and intermolecular-hydrogen-bond was primary factor to influence polymerization rate. Moreover, the insights of density functional theory calculations revealed that negative electrostatic potential ensured nucleophilic capacity. This investigation demonstrated the considerable potential of DES for RCMP, which is anticipated for other polymerization applications as a novel medium mode.

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Supported Atomically Dispersed Pd Catalyzed Direct Alkoxylation and Allylic Alkylation

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Chinese Journal of Chemistry 2024年第7期42卷 719-724页

作者： Ruixuan Qin Ziwen Chen qingyuan Wu Nanfeng Zheng Pengxin Liu New Cornerstone Science laboratory State Key Laboratory for Physical Chemistry of Solid SurfacesCollaborative Innovation Center of Chemistry for Energy Materialsand National&Local Joint Engineering Research Center of Preparation Technology of NanomaterialsCollege of Chemistry and Chemical EngineeringXiamen UniversityXiamenFujian 361005China innovation Laboratry for Scences and Technoogies of Energy Materials of Fujan Province(IKKM) Xiamen Fujian 361102China School of Physical Science and Technology Shanghai Tech UniversityShanghai 201210China Fujian Key laboratory of Rare-earth Functional Materials Fujian Shanhai Collaborative Innovation Center of Rare-earth Functional MaterialsLongyanFujian 366300China

A new approach to allylic alkylation is realized using an atomically dispersed palladium catalyst(Pd1/TiO2-EG).Unlike conventional methods that require derivation of substrates and utilization of additives,this method allows for direct allylic alkylation from allylic alcohols,producing H2O as the sole by-product.The catalyst's high efficiency is attributed to the local hydrogen bonding at the or-ganic-inorganic interface(Pd-EG interface),facilitating hydroxyl group activation forη3π-allyl complex formation.The system demonstrates successful direct C—O and C—C coupling reactions with high selectivity,requiring no additives.This study highlights the potential of supported atomically dispersed catalysts for greener and more efficient catalysis,meanwhile,offers unique insights into the distinct behavior of atomically dispersed catalysts in comparison to homogeneous or nanoparticle-based catalysts.

关键词： Atomically dispersed catalyst Alkylation C—C coupling Organic-inorganic Interface Hydrogen bond Tsuji-Trost reaction Green catalysis

Recent advancements in hydrometallurgical recycling technologies of spent lithium-ion battery cathode materials

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Rare Metals 2024年第3期43卷 879-899页

作者： Juan Wu Li Xiao Li Shen Jian-Jun Ran Hui Zhong Yi-Rong Zhu Han Chen College of Materials and Advanced Manufacturing Hunan University of TechnologyZhuzhou412007China School of Resources Processing and Bioengineering Central South UniversityChangsha410083China Guangdong JiaNa Energy Technology Company Qingyuan513000China

The rapidly increasing production of lithium-ion batteries(LIBs)and their limited service time increases the number of spent LIBs,eventually causing serious environmental issues and resource wastage.From the perspectives of clean production and the development of the LIB industry,the effective recovery and recycling of spent LIBs require urgent solutions.This study provides an overview of the current hydrometallurgical processes employed in the recycling of spent cathode materials,focusing on the leaching of valuable metals and their postprocessing.In particular,this research reviews the various leaching systems(inorganic acid,organic acid,and ammonia)and the separation of valuable metals,and then,recommendations for subsequent study are offered in an attempt to contribute to the development of highly efficient methods for recycling spent cathode materials.In addition,a range of existing technologies,such as solvent extraction,chemical precipitation,electrochemical deposition,and regeneration,for the postprocessing of leaching solutions are summarized.Finally,the promising technologies,existing challenges and suggestions with respect to the development of effective and environmentally friendly recycling methods for handling spent cathode materials are identified.

关键词： Spent lithium-ion batteries(LIBs) Cathode material Hydrometallurgy Leaching Recycling

Potential industrial applications of photo/electrocatalysis: Recent progress and future challenges

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Green Energy & Environment 2024年第5期9卷 859-876页

作者： Jinhao Li Jing Ren Shaoquan Li Guangchao Li Molly Meng-Jung Li Rengui Li Young Soo Kang Xiaoxin Zou Yong Luo Bin Liu Yufei Zhao State Key laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing100029China Quzhou Institute for innovation in Resource Chemical Engineering Quzhou324000China State Key laboratory of Organic-Inorganic Composites Beijing University of Chemical TechnologyBeijing100029China Department of Applied Physics The Hong Kong Polytechnic UniversityHong Kong999077China State Key laboratory of Catalysis Dalian Institute of Chemical PhysicsChinese Academy of SciencesDalian National Laboratory for Clean EnergyZhongshan Road 457Dalian116023China Environmental and Climate Technology Track of Korea Institute of Energy Korea Institute of Energy TechnologyNaju-siJeollanam do58217Republic of Korea State Key laboratory of Inorganic Synthesis and Preparative Chemistry College of ChemistryJilin UniversityChangchun130012China

Nowadays,the rapid development of the social economy inevitably leads to global energy and environmental crisis.For this reason,more and more scholars focus on the development of photocatalysis and/or electrocatalysis technology for the advantage in the sustainable production of high-value-added products,and the high efﬁciency in pollutants remediation.Although there is plenty of outstanding research has been put forward continuously,most of them focuses on catalysis performance and reaction mechanisms in laboratory conditions.Realizing industrial application of photo/electrocatalytic processes is still a challenge that needs to be overcome by social demand.In this regard,this review comprehensively summarized several explorations in theﬁeld of photo/electrocatalytic reduction towards potential industrial applications in recent years.Special attention is paid to the successful attempts and the current status of photo/electrocatalytic water splitting,carbon dioxide conversion,resource utilization from waste,etc.,by using advanced reactors.The key problems and challenges of photo/electrocatalysis in future industrial practice are also discussed,and the possible development directions are also pointed out from the industry view.

关键词： Photocatalysis Electrocatalysis Industrial applications H2 economy