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A new strategy through polymer in situ ionization to construct high-performance electrolyte for solid-state batteries

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Journal of Energy Chemistry 2025年第6期105卷 814-822页

作者： Ling Chen Xiu Liu Guojing Zang Jinhao Xie Binhong Wu Chi Zhang Ying Xu Yuxin Luo Dingshan Yu Zishou Zhang Key Laboratory for Polymeric Composite and Functional Materials of Ministry of Education Key Laboratory of High Performance Polymer-Based Composites of Guangdong Province School of Chemistry Sun Yat-sen University School of Chemical Engineering and Bioengineering Washington State University

The practical application of poly（ethylene oxide）(PEO)-based solid polymer electrolytes in all-solid-state lithium-metal batteries（ASSLBs） still suffers from persistent challenges associated with low ionic conductivity and poor oxidative *** address these issues,we introduce a novel in-situ ionization strategy using radical polymer poly（2,2,6,6-tetramethyl-1-piperidinyloxy-4-yl acrylate）(PTPA) to enhance ionic conductivity and achieve a high electrochemical stability window in PEO-based *** functional theory（DFT） calculations and molecular dynamics（MD） simulations reveal that the in-situ generation of PTPA+from PTPA within the battery,not only exceptionally decreases the low Highest Occupied Molecular Orbital（HOMO） energy level,but also exhibits a robust anchoring effect on TFSI-anions in the electrolyte,which boosts Li migration and enables dense Li deposition *** a result,the PEO/10 wt%PTPA/LiTFSI electrolyte demonstrates remarkable oxidative stability up to 5 V and a high Li+transference number（0.57）.Li-Li symmetric cells maintain stability over 1000 h at0.2 mA cm-2,and LiFePO4（LFP）//Li battery also presents an enduring cyclic performance over 500 cycles with a remarkable high-capacity retention of 91.8% at ***,by coupling with a high-voltage LiCoO2（LCO） cathode（cut-off voltage 4.6 V）,the assembled ASSLBs reach a capacity retention of 87.1%after 500 cycles at *** study explores the mechanism of radical polymer in PEO-based electrolyte and provides a fire-new strategy for construction of high-performance and multifunctional ASSLBs.

关键词： High-voltage lithium-metal batteries Interfacial stability Radical polymer Solid polymer electrolytes

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Machine learning models for the density and heat capacity of ionic liquid-water binary mixtures

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Chinese Journal of chemical engineering 2024年第9期73卷 244-255页

作者： Yingxue Fu Xinyan Liu Jingzi Gao Yang Lei Yuqiu Chen Xiangping Zhang School of Chemistry and Chemical Engineering Hubei Key Laboratory of Coal Conversion and New Carbon MaterialsWuhan University of Science and TechnologyWuhan 430081China Department of Chemical and Biomolecular Engineering University of Delaware150 Academy StreetNewarkDE 19716United States College of Chemical Engineering and Environment China University of PetroleumBeijing 102249China

Ionic liquids(ILs),because of the advantages of low volatility,good thermal stability,high gas solubility and easy recovery,can be regarded as the green substitute for traditional ***,the high viscosity and synthesis cost limits their application,the hybrid solvent which combining ILs together with others especially water can solve this *** with the pure IL systems,the study of the ILs-H_(2)O binary system is rare,and the experimental data of corresponding thermodynamic properties(such as density,heat capacity,etc.)are ***,it is also difficult to obtain all the data through ***,this work establishes a predicted model on ILs-water binary systems based on the group contribution(GC)*** different machine learning algorithms(ANN,XGBoost,LightBGM)are applied to fit the density and heat capacity of ILs-water binary *** then the three models are compared by two index of MAE and R^(2).The results show that the ANN-GC model has the best prediction effect on the density and heat capacity of ionic liquid-water mixed ***,the Shapley additive explanations(SHAP)method is harnessed to scrutinize the significance of each structure and parameter within the ANN-GC model in relation to prediction *** results reveal that system components(XIL)within the ILs-H_(2)O binary system exert the most substantial influence on density,while for the heat capacity,the substituents on the cation exhibit the greatest *** study not only introduces a robust prediction model for the density and heat capacity properties of IL-H_(2)O binary mixtures but also provides insight into the influence of mixture features on its density and heat capacity.

关键词： Ionic liquids Density Heat capacity Group contribution method Machine learning

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Effect of Particle Orientation on Heat Transfer in Arrays of Prolate Particles

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Computer Modeling in engineering & Sciences 2023年第8期136卷 1509-1526页

作者： Romana Basit Xinyang Li Zheqing Huang Qiang Zhou School of Chemical Engineering and Technology Xi’an Jiaotong UniversityXi’anChina State Key Laboratory of Multiphase Flow in Power Engineering Xi’an Jiaotong UniversityXi’anChina

Direct Numerical Simulations have been carried out to study the forced convection heat transfer of flow through fixed prolate particles for a variety of aspect ratios ar={5/4,5/3,5/1}with Reynolds number(Re)up to *** variations of the solid volume fraction c={0.1,0.2,0.3}with four Hermans orientation factors S={−0.5,0,0.5,1}are *** has been found that changes in S cause prominent variations in the Nusselt *** general,Nusselt number increases with the decrease of *** all three aspect ratios,the Nusselt number remains a linear function of S at different c and ***,it is concluded that,for heat transfer from prolate muti-particle system,the effects of orientations cannot be ignored.A new correlation for Nusselt number has been developed for arrays of prolate particles using the simulation data as a function of Re,c,S and ar.

关键词： Direct Numerical Simulation heat transfer lattice Boltzmann method particle orientations prolate particles

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Oxidation of benzene to phenol with N_(2)O over a hierarchical Fe/ZSM-5 catalyst

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Green Energy & Environment 2023年第4期8卷 1161-1173页

作者： Cui Ouyang Jianwei Li Yaqi Qu Song Hong Songbo He State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing100029China Green Chemical Reaction Engineering Engineering and Technology Institute GroningenUniversity of GroningenNijenborgh 4Groningen9747 AGthe Netherlands CoRe Pro Colijnlaan 21Groningen9722 PJthe Netherlands

Catalytic oxidation of benzene with N_(2)O to phenol over the hierarchical and microporous Fe/ZSM-5-based catalysts in a continuous fixedbed reactor was *** spent catalyst was in-situ regenerated by an oxidative treatment using N_(2)O and in total 10 reaction-regeneration cycles were performed.A 100% N_(2)O conversion,93.3% phenol selectivity,and high initial phenol formation rate of 16.49±0.06mmol_(phenol gcatalyst)^(-1)h^(-1)at time on stream(TOS) of 5 min,and a good phenol productivity of 147.06 mmol_(phenol gcatalyst)^(-1)during catalyst lifetime of 1800 min were obtained on a fresh hierarchical Fe/ZSM-5-Hi2.8 *** the reaction-regeneration cycle,N_(2)O conversion is fully recovered within TOS of 3 h,moreover,the phenol productivity was decreased ca.2.2±0.8% after each cycle,leading to a total phenol productivity of ca.0.44 ton_(pheol kg_(catalyst)^(-1)estimated for 300 *** characterizations imply that the coke is rapidly deposited on catalyst surface in the initial TOS of 3 h(0.28 mgc_(gcatalyst)^(-1)min^(-1)) and gradually becomes graphitic during the TOS of 30 h with a slow formation rate of 0.06 mgc g_(catalyst)^(-1)min^(-1).Among others(e.g.,the decrease of textural property and acidity),the nearly complete coverage of the active Fe-O-Al sites by coke accounts for the main catalyst *** these reversible deactivation characteristics related to coking,the irreversible catalyst deactivation is also observed with the reaction-regeneration *** latter is reflected by a further decreased amount of the active Fe-O-Al sites,which agglomerate on catalyst surface with the cycle,likely associated with the hard coke residue that is not completely removed by the regeneration.

关键词： Hierarchical Fe/ZSM-5 N_(2)O conversion Phenol product productivity Reaction-regeneration cycles Irreversible deactivation mechanism

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Bioinspired drug-delivery system emulating the natural bone healing cascade for diabetic periodontal bone regeneration

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Bioactive Materials 2023年第3期21卷 324-339页

作者： He Wang Xiaowei Chang Qian Ma Boyang Sun Han Li Jinmin Zhou Yiyao Hu Xiaoyu Yang Jie Li Xin Chen Jinlin Song Chongqing Key Laboratory of Oral Diseases and Biomedical Sciences Chongqing Municipal Key Laboratory of Oral Biomedical Engineering of Higher EducationCollege of Stomatology of Chongqing Medical UniversityChongqing401147China Department of Chemical Engineering Shaanxi Key Laboratory of Energy Chemical Process IntensificationInstitute of Polymer Science in Chemical EngineeringSchool of Chemical Engineering and TechnologyXi′an Jiaotong UniversityXi′an710049China

Diabetes mellitus(DM)aggravates periodontitis,resulting in accelerated periodontal bone *** glucose metabolism in DM causes reactive oxygen species(ROS)overproduction resulting in compromised bone healing,which makes diabetic periodontal bone regeneration a major *** by the natural bone healing cascade,a mesoporous silica nanoparticle(MSN)-incorporated PDLLA(poly(DL-lactide))-PEG-PDLLA(PPP)thermosensitive hydrogel with stepwise cargo release is designed to emulate the mesenchymal stem cell“recruitment-osteogenesis”cascade for diabetic periodontal bone *** therapy,SDF-1 quickly escapes from the hydrogel due to diffusion for early rat bone marrow stem cell(rBMSC)***-neously,slow degradation of the hydrogel starts to gradually expose the MSNs for sustained release of metformin,which can scavenge the overproduced ROS under high glucose conditions to reverse the inhibited osteogenesis of rBMSCs by reactivating the AMPK/β-catenin pathway,resulting in regulation of the diabetic microenvironment and facilitation of *** vitro experiments indicate that the hydrogel markedly restores the inhibited migration and osteogenic capacities of rBMSCs under high glucose *** vivo results suggest that it can effectively recruit rBMSCs to the periodontal defect and significantly promote periodontal bone regeneration under type 2 *** conclusion,our work provides a novel therapeutic strategy of a bioinspired drug-delivery system emulating the natural bone healing cascade for diabetic periodontal bone regeneration.

关键词： Periodontal bone regeneration Diabetes mellitus Bioinspired Hydrogel Drug delivery

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Double-stretching as an effective and generalizable strategy towards thinner nanofibers in solution blow spinning

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Nano Research 2023年第4期16卷 5709-5714页

作者： Baopu Zhang Ziwei Li Zekun Cheng Lei Li Chong Yang Haiyang Wang Hui Wu State Key Laboratory of Ceramics and Fine Processing School of Materials Science and EngineeringTsinghua UniversityBeijing 100084China Department of Chemical Engineering Massachusetts Institute of TechnologyCambridge 02139USA

Solution blow spinning(SBS)applies high-speed airflow to prepare fibers by generating a strong stretching *** has the advantages of scalable production,tailorable morphologies,and wide ***,the SBS strategy can hardly prepare fibers down to the sub-100 nanometers,which limits its performance in demanding ***,we overcome the limitation of SBS by introducing a second *** novel strategy is termed double-stretching SBS(DS-SBS)because an extra stretching force is exerted on the fiber when it converges with the second ***6 nanofibers with an average diameter of 80 nm are successfully prepared with the DS-SBS strategy,while the SBS strategy could only prepare submicron fibers with an average diameter of 120 ***,the generality of the DS-SBS strategy to reduce fiber diameter is verified on numerous solute-solvent pairs.

关键词： nanofibers solution blow spinning double-stretching computational fluid dynamics

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Shape/dimension-controllable organic heterostructures from one monomer pair

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Chinese chemical Letters 2025年第3期36卷 239-243页

作者： Yan Chen Xinnan Wang Yifan Lin Chun Liu Cancer Hospital of Dalian University of Technology State Key Laboratory of Fine ChemicalsFrontier Science Center for Smart MaterialsSchool of Chemical EngineeringDalian University of TechnologyDalian 116024China

Controllable construction of organic heterostructures is key to developing supramolecular materials with sophisticated ***,block heterostructures with controllable shape and dimension have been successfully constructed from one molecular pair of Ir(III)complexes 1 and 2 in H_(2)O/CH_(3)*** volume ratios of H_(2)O/CH_(3)CN led to controllable morphologies of assemblies 1 from nanofibers(1NF)to nanosheets(1NS).Through reasonable experimental design,both 1NF and 1NS could be used as seeds to trigger the heterogeneous nucleation-elongation of ***,unprecedented dual control on the length and width of supramolecular block copolymers from the same monomer pair was realized *** corresponding heterogeneous nucleation-elongation process was confirmed by time-dependent UV–vis absorption spectra and emission *** components of each segment of the fibrous and sheet-like block copolymers were identified by TEM,SEM,and *** results reveal that the previously unappreciated solvation effect can serve as a powerful tool to control the morphologies of heterostructures.

关键词： Size controllable Organic heterostructure Supramolecular block copolymer Ir(III)complex Solvation effect

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Experimental and theoretical analysis of loading characteristics of electret filter media for charged particles

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Particuology 2024年第10期93卷 87-98页

作者： Yiqi Cai Rongrong Cai Lizhi Zhang Key Laboratory of Enhanced Heat Transfer and Energy Conservation of Education Ministry School of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhou510640China State Key Laboratory of Subtropical Building Science South China University of TechnologyGuangzhou510640China

The degradation of filtration performance in electret filter media during usage poses a significant challenge. Pre-charging of aerosols has been identified as an effective method to mitigate this issue. However, the effects of particle charging characteristics on the loading characteristics of electret filters still need a comprehensive understanding. In this study, a needle-cylinder corona charger was employed to pre-charge aerosols, and the particle charge state was determined by multiphysics simulation. The effects of particle charge polarity and charge quantity on the loading performance of the electret filter were quantitatively investigated. The results showed that the particle charge polarity had a negligible impact on the loading performance under the condition of the equivalent particle charge quantity. In addition, the charged particles effectively improved the efficiency degradation during the loading process of electret media, with higher charge quantities resulting in more pronounced improvements. The electrostatic attenuation factor showed a negative exponential correlation with the particle charge quantity. This was attributed to the uneven particle deposition on fiber surface due to the attraction of charged particles by the opposite charges on the electret fibers, which alleviated the effect of electrostatic shielding.

关键词： Electret filter Charged particles Loadingcharacteristic Corona charging Electrostatic screening

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Multicolored structural coloration of carbon nanotube fibers

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SusMat 2023年第1期3卷 102-110页

作者： Run Li Shiliang Zhang Hang Chen Ya Huang Baoshun Wang Xueke Wu Qinyuan Jiang Siming Zhao Fei Wang Yanlong Zhao Rufan Zhang Beijing Key Laboratory of Green Chemical Reaction Engineering and Technology Department of Chemical EngineeringTsinghua UniversityBeijingChina

Carbon nanotube fibers(CNTFs)are endowed with excellent mechanical,electrical,and thermal properties and are considered promising candidates in numerous cutting-edge ***,the inherent black color of CNTFs hinders their practical application in fields with high aesthetic requirements such as wearable devices and smart *** to the smooth surface and chemical inertness,CNTFs are hard to be dyed by conventional chemical dyes or colorful ***,we realize a structural coloration of CNTFs by coating them with two metal oxide layers via atomic layer *** three elements of color,that is,hue,saturation,and brightness,can be controlled by adjusting the types and thickness of each oxide *** CNTFs with wide color gamut and high saturation are achieved through different combinations.A film interference model is also established to reveal the mechanism of the structural coloration,which is a comprehensive result of thin-film interference and surface roughness *** calculated reflectance well fits the measured results by introducing surface roughness ***,the colored CNTFs are not iridescent because of retinal signal delay,which will further expand their applications.

关键词： atomic layer deposition carbon nanotube structural color

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A facile ice-templating-induced puzzle coupled with carbonization strategy for kilogram-level production of porous carbon nanosheets as high-capacity anode for lithium-ion batteries

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Carbon Energy 2024年第12期6卷 164-179页

作者： Baolin Xing Feng Shi Zhanzhan Jin Huihui Zeng Xiaoxiao Qu Guangxu Huang Chuanxiang Zhang Yunkai Xu Zhengfei Chen Jun Lu Henan Key Laboratory of Coal Green Conversion College of Chemistry and Chemical EngineeringHenan Polytechnic UniversityJiaozuoChina State Collaborative Innovation Center of Coal Work Safety and Clean-efficiency Utilization JiaozuoChina School of Biological and Chemical Engineering NingboTech UniversityNingboChina College of Chemical and Biological Engineering Zhejiang UniversityHangzhouChina

Two-dimensional porous carbon nanosheets(PCNSs)are considered promising anodes for lithium-ion batteries due to their synergetic features arising from both graphene and porous ***,using naturally abundant and biocompatible sodium humate(SH)as the precursor,PCNSs are prepared from the laboratory scale up to the kilogram scale by a method of a facile ice-templating-induced puzzle coupled with a carbonization *** obtained SH-derived PCNSs(SH-PCNSs)possess a hierarchical porous structure dominated by mesopores having a specific surface area(~127.192 g^(−1)),pore volume(~0.134 cm3 g^(−1)),sheet-like morphology(~2.18nm in thickness),and nitrogen/oxygen-containing functional *** to these merits,the SH-PCNSs present impressive Li-ion storage characteristics,including high reversible capacity(1011mAh g^(−1) at 0.1 A g^(−1)),excellent rate capability(465mAh g^(−1) at 5 A g^(−1)),and superior cycle stability(76.8%capacitance retention after 1000 cycles at 5 A g^(−1)).It is noted that the SH-PCNSs prepared from the kilogram-scale production procedure possess comparable electrochemical ***,coupling with a LiNi1/3Co1/3Mn1/3O2 cathode,the full cells deliver a high capacity of 167mAh g^(−1) at 0.2A g^(−1) and exhibit an outstanding energy density of 128.8Whkg^(−1),highlighting the practicability of this porous carbon nanosheets and the potential commercial opportunity of the scalable processing approach.

关键词： anode materials ice-templating-induced puzzle lithium-ion batteries porous carbon nanosheets sodium humate

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