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Poisoning effect of polyvinyl chloride on the catalytic pyrolysis of mixed plastics over zeolites

Science China Chemistry 2024年第7期67卷 2265-2273页

作者： Jiangchun Yuan Wenjie Wang Weixiao Sun Zhirong Yang Yueqiang Cao Wenyao Chen Xiaohu Ge Gang Qian Xiang Feng Xuezhi Duan Xinggui Zhou Kevin M.Van Geem Jing Zhang State Key Laboratory of Chemical Engineering East China University of Science and TechnologyShanghai 200237China School of Chemical Engineering Zhengzhou UniversityZhengzhou 450001China Laboratory for Chemical Technology(LCT) Department of MaterialsTextiles and Chemical EngineeringFaculty of Engineering&ArchitectureGhent UniversityZwijnaarde B-9052Belgium State Key Lab of Heavy Oil Processing China University of PetroleumQingdao 266580China

Nowadays,the chemical recycling is applied for only 1%of total waste plastics,largely due to contaminants in plastic waste and difficulty in product *** the major contaminant,polyvinyl chloride(PVC)often forms corrosive hydrogen chloride(HCl)during the chemical recycling,which may cause severe catalyst deactivation and equipment ***,the investigation on catalytic pyrolysis(the major route for plastics chemical recycling)of the PVC containing mixed plastics has been rarely ***,catalytic co-pyrolysis of PVC and polyethylene(PE)was studied over an aromatization catalyst,Pt/ZSM-5,since the basic building block aromatics are desired products from plastics chemical *** poisoning effect of PVC vapor on the catalyst stability was explored by collective efforts of thorough product analysis and catalyst *** was found that the HCl evolving from PVC has an autocatalytic effect that promotes the scission of dehydrochlorinated PVC,resulting in the high yield of benzene and acetylene from *** the other hand,the presence of PVC suppressed the aromatics formation from PE,largely due to the poisoning effect of PVC-derived HCl on the Pt/*** deactivation is irreversible as evidenced by the decreased zeolite crystallinity and the loss of strong acid sites that are key to the aromatization,possibly due to the removal of framework Al upon the interaction with *** modification with octadecylphosphonic acid only slightly alleviated the PVC poisoning *** insights on the PVC poisoning of zeolite catalysts provided in this work may guide the process design of chemical recycling of PVC containing waste plastics.

关键词： polyvinyl chloride polyethylene zeolite aromatics deactivation

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Study on the recovery of NMP waste liquid in lithium battery production by coupled pervaporation-adsorption process and evaluation of technical and economic performances

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Chinese Journal of chemical engineering 2025年第2期78卷 273-283页

作者： Jiayi Zhang Jiali He Guibing Wang Yu Zhao Huairong Zhou Dongliang Wang Dongqiang Zhang School of Petrochemical Engineering Lanzhou University of Technology Key Laboratory of Low Carbon Energy and Chemical Engineering of Gansu Province

N-methyl-pyrrolidone(NMP) is an important solvent for the production of lithium batteries, which causes environmental pollution and wastes resources if it is directly discharged. The current commonly used vacuum distillation recovery process suffers from high operating costs and high energy consumption. Therefore, this paper proposes a coupled pervaporation-adsorption(PV-A) process to recover NMP solvents from lithium battery production waste streams. In this process, pervaporation is used to dewater the NMP waste liquid, it was found that the water content in the raw material liquid decreased from the initial 8.3%(mass) to 0.14%(mass) after 400 min of dewatering, but the membrane separation performance decreased significantly when the water content of the raw material liquid decreased to0.45%(mass), and at the same time, the NMP loss rate increased rapidly. An adsorption process was used to remove trace water from the remaining liquid, and the water content in the feed liquid under the optimal adsorption process conditions was reduced from 0.45%(mass) to 0.014%, which fully meets the purity requirements of electronics-grade NMP for the production of lithium batteries. Steady-state modeling and techno-economic evaluation of the proposed coupled process were carried out, and compared with vacuum distillation and pervaporation technologies, the results showed the PV-A process yielded the best techno-economic performance and the lowest environmental impact, and it can be used as an alternative process to the traditional NMP recycling technology. This study provides a new method for the recycling of NMP in the lithium battery industry.

关键词： Adsorption NaA zeolite membrane NMP recovery Pervaporation Techno-economic evaluation

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HOF skeleton analogues construct fast carrier transfer channels for enhanced photocatalytic hydrogen production

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International Journal of Hydrogen Energy 2025年 137卷 505-512页

作者： Jin, Zhiliang Zhang, Linqing Ma, XiaoLi School of Chemistry and Chemical Engineering Ningxia Key Laboratory of Solar Chemical Conversion Technology Key Laboratory for Chemical Engineering and Technology State Ethnic Affairs Commission North Minzu University Yinchuan750021 China

Photocatalytic water splitting is an ideal approach for hydrogen production due to its cleanability, high-efficiency, and persistence. However, single-semiconductor catalysts suffer from challenges such as slow charge transfer and high electron recombination rates. An effective approach to improve photocatalytic performance is the formation of heterojunctions using surface-loaded catalysts. In this study, a highly efficient and facile method was used to synthesize a Hydrogen bonded organic framework (HOF), which was then assembled onto Co/CoO by taking advantage of its unique compositional stability. The synergy between the two components enabled the HC-10 composite to achieve efficient hydrogen production, while preserving stability. The composite catalyst reduces the electron transfer distance between the two catalysts, enhancing their electron transfer capabilities and minimizing electron-hole recombination, which is crucial for effective catalytic reactions. Furthermore, the directional interactions due to hydrogen bonding and π-π stacking further enhance the stability of the composite catalyst. This approach provides a new perspective on the application of organic materials in photocatalysis. © 2025 Hydrogen Energy Publications LLC

关键词： Photocatalytic activity

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Core-shell-structured Composite ZSM-5@MCM-41 Catalysts:Fabrication,Characterization,and Enhanced Performance in Hexane Catalytic Cracking

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China Petroleum Processing & Petrochemical technology 2023年第4期25卷 41-51页

作者： Zhu Jiale Zhu Xuedong Yang Fan State Key Laboratory of Chemical Engineering School of Chemical EngineeringEast China University of Science&TechnologyShanghai 200237China

A series of core-shell zeolites with a ZSM-5 zeolite core and a MCM-41 shell with varying shell thicknesses were successfully fabricated via a cetyltrimethylammonium bromide(CTAB)-directed sol-gel coating method in an ultradilute solution. Extensive characterization techniques, including XRD, TEM, N_(2) adsorption-desorption, NH_(3)-TPD, and IR measurements, confirmed the successful coating of a microporous ZSM-5 core with a mesoporous MCM-41 shell layer and were further employed to explore the textural properties and acidic properties of the samples. The hexane cracking results revealed a significant enhancement in olefin yields after introducing the MCM-41 shell to ZSM-5. Interestingly, a volcanic trend in olefin yields was observed with the increase in the shell thickness. In particular, the highest olefin yield of 51.5%, exceeding that of the core catalyst by 17.1%, was achieved when the shell thickness was controlled at 40 ***, the catalyst lifetime investigation revealed that the core-shell composite catalyst exhibited a minimal reduction in hexane conversion of merely 3.8% over a 120 h reaction period, significantly outperforming the 11.3% reduction exhibited by the core catalyst. This remarkable catalytic performance was attributed to the passivation of external acid sites and the introduction of more developed pore channels by the shell, which effectively mitigated unwanted side reactions. The successful synthesis of these core-shell structured catalysts presents a novel strategy for improving catalytic performance in hexane cracking, in addition to serving as a solid foundation for the design of industrial catalysts for light naphtha cracking.

关键词： catalytic cracking light olefin core-shell ZSM-5 zeolite

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Triazine-COF@Silicon nanowire mimicking plant leaf to enhance photoelectrocatalytic CO_(2)reduction to C_(2+) chemicals

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Green Energy & Environment 2025年第2期10卷 422-432页

作者： Wenrui Wan Fanhua Meng Si Chen Jianhua Wang Chunyan Liu Yan Wei Chenpu He Li Fan Qiaolan Zhang Weichun Ye Huanwang Jing State Key Laboratory of Applied Organic Chemistry College of Chemistry and Chemical EngineeringLanzhou UniversityLanzhou730000GansuChina Key Laboratory of Green Chemical Media and Reactions(Ministry of Education) School of Chemistry and Chemical EngineeringHenan Normal UniversityXinxiang453007HenanChina School of Chemical Engineering Lanzhou University of Arts and SciencesLanzhou730010China

Converting CO_(2)and water into valuable chemicals like plant do is considered a promising approach to address both environmental and energy *** inspiration from the structures of natural leaves,we designed and synthesized a novel copper-coordinated covalent triazine framework(CuCTF)supported by silicon nanowire arrays on wafer *** marks the first-ever application of such a hybrid material in the photoelectrocatalytic reduction of CO_(2)under mild *** Si@CuCTF6 heterojunction has exhibited exceptional selectivity of 95.6%towards multicarbon products(C_(2+))and apparent quantum efficiency(AQE)of 0.89%for carbon-based *** active sites of the catalysts are derived from the nitrogen atoms of unique triazine ring structure in the ordered porous framework and the abundant Cu-N coordination sites with bipyridine ***,through DFT calculations and operando FTIR spectra analysis,we proposed a comprehensive mechanism for the photoelectrocatalytic CO_(2)reduction,confirming the existence of key intermediate species such as*CO_(2)-,*=C=O,*CHO and*CO-CHO *** work not only provides a new way to mimic photosynthesis of plant leaves but also gives a new opportunity to enter this research field in the future.

关键词： Silicon Photoelectrocatalysis CO_(2)reduction Covalent triazine framework Sustainable chemistry

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Towards the insights into the deactivation behavior of acetylene hydrogenation catalyst

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Petroleum Science 2024年第2期21卷 1405-1414页

作者： Hai-Xia Su Yang Jiao Jian-Gong Shi Zhi-Wei Yuan Di Zhang Xu-Peng Wang Jing Ren Dan Liu Jian-Zhou Gui Hai-Yang Gao Xiao-Li Xu State Key Laboratory of Separation Membranes&Membrane Processes Tianjin Key Laboratory of Green Chemical Technology and Process EngineeringSchool of Material Science and EngineeringTiangong UniversityTianjin300387China Institute of Engineering Technology Sinopec Catalyst Co.LtdBeijing101100China State Key Laboratory of Separation Membranes and Membrane Processes Tianjin Key Laboratory of Green Chemical Technology and Process EngineeringSchool of ChemistryTiangong UniversityTianjin300387China

A series of model catalysts were obtained by treating commercial fresh and spent catalysts unloaded from the factory with different methods, including green oil dipping, extraction and high-temperature regeneration;finally, the deactivation behavior of the commercial catalyst for acetylene hydrogenation were studied. The influence of various possible deactivation factors on the catalytic performance was elucidated via detailed structural characterization, surface composition analysis, and activity *** results showed that green oil, carbon deposit and sintering of active metal were the main reasons for deactivation, among which green oil and carbon deposit led to rapid deactivation, while the activity could be recovered after regeneration by high-temperature calcination. The sintering of active metal components was attributed to the high-temperature regeneration in hydrothermal conditions, which was slow but irreversible and accounted for permanent deactivation. Thus, optimizing the regeneration is expected to extend the service life of the commercial catalyst.

关键词： Acetylene Hydrogenation Green oil Carbon deposit Sintering Catalyst deactivation

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Kinetics of hydrogen sulfide removal from coke oven gas over faujasite zeolite: Experimental and modeling studies

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Chinese Journal of chemical engineering 2025年第2期78卷 232-244页

作者： Feng Gao Sixiao Zhu Liping Chang Weiren Bao Jinghong Ma Junjie Liao State Key Laboratory of Clean and Efficient Coal Utilization Taiyuan University of Technology Key Laboratory of Coal Science and Technology Ministry of Education Taiyuan University of Technology School of Chemistry and Chemical Engineering Taiyuan University of Technology Shanxi-Zheda Institute of Advanced Materials and Chemical Engineering

The removal of H2S from coke oven gas(COG) is an important issue for the further utilization of *** could be used for industrial desulfurization owing to their high thermal stability and regenerability. However, further analysis on the kinetics of deep desulfurization using zeolites is necessary to provide relevant information for industrial design. In this study, the desulfurization breakthrough curves of faujasite(FAU) zeolite in COG were measured using a fixed bed reactor. The adsorption isotherm was investigated using the Langmuir, Freundlich, Temkin, Dubinin-Radushkevich models. The adsorption saturated capacity of H2S was inversely related to the temperature. The results show that the Langmuir model best fits the adsorption isotherm with a lower value of root-mean-square-error(RMSE) and ChiSquare(χ2), and the calculated activation energy is 14.62 k J·mol—1. The adsorption kinetics were investigated using pseudo-first-order(PFO), pseudo-second-order(PSO), Bangham and Weber-Morris models. The Bangham model fitted the kinetic data well, indicating that pore diffusion is an influential factor in the adsorption process. The Weber-Morris model suggests that the adsorption rate was not solely determined by the pore diffusion, but was also influenced by the active site on the FAU zeolite. The adsorption breakthrough curves under different gas flow rates were fitted using the bed depth service time(BDST) model, and it provides an accurate prediction of the breakthrough time with a small relative error. The results of thermodynamic analysis demonstrated the feasibility and spontaneity(ΔG<0) and exothermic(ΔH<0) nature of the adsorption process of the FAU zeolite for H2S under COG.

关键词： Adsorption Coke oven gas FAU zeolite Fixed-bed H2S Kinetics

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A review of over-discharge protection through prelithiation in working lithium-ion batteries

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Journal of Energy Chemistry 2025年第2期101卷 437-452,I0009页

作者： Hanchen Wang Yingtian Liu Mingze Jiang Qiang Zhang School of Aerospace Engineering National Engineering Research Center of NeuromodulationTsinghua UniversityBeijing 100084China Tsinghua Center for Green Chemical Engineering Electrification Department of Chemical EngineeringBeijing Key Laboratory of Green Chemical Reaction Engineering and TechnologyTsinghua UniversityBeijing 100084China

The demand for high safety and high reliability lithium-ion batteries(LIBs)is strongly considered for practical ***,due to their inherent self-discharge properties or abuse,LIBs face the threat of over-discharge,which induces premature end of life and increased risk of thermal *** addition,a strong demand for batteries with zero-volt storage is strongly considered for aerospace and implantable medical *** this review,we firstly introduce the necessity and the importance of over-discharge and zero-volt protection for *** mechanism of damage to the Cu current collectors and SEI induced by potential changes during over-discharge is *** current over-discharge protection strategies based on whether the zero-crossing potential of the electrodes is ***,the fresh insights into the material design of cathode prelithiation additives are presented from the perspective of over-discharge protection.

关键词： Li-ion batteries Over-discharge protection Zero-volt storage Electrode prelithiation Electrode potential regulation

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A new strategy to design isostructural salts: The case of the antitumor drug dimethylaminomicheliolide

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Chinese chemical Letters 2023年第2期34卷 150-153页

作者： Zhonghua Li Haibin Qu Lan Fang Songgu Wu Junbo Gong State Key Laboratory of Chemical Engineering School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China Chemistry and Chemical Engineering Guangdong Laboratory Shantou 515031China

Isostructural multicomponent crystals provide a promising way for fine-tuning physicochemical properties, whereas their design remains quite challenging. The purpose of this work was to provide a new strategy for obtaining isostructural multicomponent crystals by introducing coformers with functional group positional isomerism. Five isostructural salts of an antitumor drug dimethylaminomicheliolide(DMAMCL) were reported and designed with a series of dihydroxybenzoic acid regioisomers for the first time, which were identified by power and single-crystal X-ray diffractions. Similar lattice parameters suggested these obtained salts may have the same crystal packing mode. The quantitative similarity parameters via XPac, Crystal CMP and Mercury program further proved these crystal structures are3D isostructural. Hirshfeld surface maps and 2D fingerprint plots show that the isostructural salts have similar intermolecular interactions. Compared with DMAMCL, obvious improvement was observed in the thermal stability, hygroscopicity, and solubility of these isostructural salts. Meanwhile, isostructural crystals may have different physicochemical properties, even though the shape and molecular size are similar and the packing of crystal structures is equally matched.

关键词： Dimethylaminomicheliolide Crystal engineering Isostructural salt Intermolecular interactions Thermal analysis Hygroscopicity Solubility

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Process analytical technologies and self-optimization algorithms in automated pharmaceutical continuous manufacturing

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Chinese chemical Letters 2024年第3期35卷 87-95页

作者： Peiwen Liu Hui Jin Yan Chen Derong Wang Haohui Yan Mingzhao Wu Fang Zhao Weiping Zhu State Key Laboratory of Bioreactor Engineering Shanghai Key Laboratory of Chemical BiologySchool of PharmacyEast China University of Science and TechnologyShanghai 200237China State Key Laboratory of Chemical Engineering School of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China Engineering Research Center of Pharmaceutical Process Chemistry Ministry of EducationSchool of PharmacyEast China University of Science and TechnologyShanghai 200237China

The pharmaceutical industry is now paying increased attention to continuous *** the revolution to continuous and automated manufacturing is deepening in most of the top pharma companies in the world,the advancement of automated pharmaceutical continuous manufacturing in China is relatively slow due to some key challenges including the lack of knowledge on the related technologies and shortage of qualified *** this review,emphasis is given to two of the crucial technologies in automated pharmaceutical continuous manufacturing,i.e.,process analytical technology(PAT)and self-optimizing *** work published in recent 5 years employing advanced PAT tools and self-optimization algorithms is introduced,which represents the great progress that has been made in automated pharmaceutical continuous manufacturing.

关键词： Pharmaceutical continuous manufacturing Automation Process analytical technology Self-optimization algorithm

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