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Compositional evolution for mixed aerosols containing gluconic acid and typical nitrate and the effect of multiply factors on hygroscopicity

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Journal of Environmental Sciences 2024年第5期139卷 206-216页

作者： Yue Zhu Shufeng Pang Yunhong Zhang school of Chemistry and chemical Engineering Beijing Institute of TechnologyBeijing 100081China

The aging process of atmospheric aerosols usually leads to a mixture of inorganic salts and organic compounds of anthropogenic origin.In organic compounds,polyhydroxy organic acids are important components,however,the study on composition and hygroscopic properties of the mixture containing inorganics and polyhydroxy organic acids is scanty.In this study,gluconic acid,the proxy of polyhydroxy organic acids,is mixed with the representative nitrate(Mg(NO_(3))_(2),Ca(NO_(3))_(2))to form aerosols.ATR-FTIR and optical microscopy are employed to study the component changes and hygroscopicity as a function of relative humidity.As relative humidity fluctuates,the FTIR-ATR spectra display that the internal mixed gluconic acid(CH_(2)(CH)_(4)(OH)_(5)COOH)and nitrate can react to release acidic gases,forming relevant gluconate and further affecting the hygroscopicity.The specific presentation is particles cannot be recovered to their original size after the dehydration-hydration process and there will be some disparities in GF for mixed particles.For the gluconic acid-Ca(NO_(3))_(2)/Mg(NO_(3))_(2)mixtures with molar ratios of 1:1,higher degree of reaction resulting in the production of large amounts of gluconate should be responsible to the lower hygroscopicity compared to ZSR model.For 1:2 gluconic acid-nitrate mixed systems(with higher nitrate content),the hygroscopicity of mixtures are higher than the ZSR prediction.A possible reason could be‘salt-promoting effect’on the organic fractions of the surplus inorganic salt in the mixture.These data can improve the chemical composition list evaluation,in turn hygroscopic properties and phase state of atmospheric aerosol,and then the climate effect.

关键词： Hygroscopicity Gluconic acid Reaction ZSR simulation Size growth factors

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High adsorption selectivity of activated carbon and carbon molecular sieve boosting CO_(2)/N_(2) and CH_(4)/N_(2) separation

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Chinese Journal of chemical Engineering 2024年第3期67卷 282-297页

作者： Siang Chen Wenling Wu Zhaoyang Niu Deqi Kong Wenbin Li Zhongli Tang Donghui Zhang The Research Center of chemical Engineering School of Chemical Engineering and TechnologyTianjin UniversityTianjin 300072China

Flue gas and coal bed methane are two important sources of greenhouse gases.Pressure swing adsorption process has a wide range of application in the field of gas separation,and the selection of adsorbent is crucial.In this regard,in order to assess the better adsorbent for separating CO_(2) from flue gas and CH_(4) from coal bed methane,adsorption isotherms of CO_(2),CH_(4) and N_(2) on activated carbon and carbon molecular sieve are measured at 303.15,318.15 and 333.15 K,and up to 250 kPa.The experimental data fit better with Langmuir 2 compared to Langmuir 3 and Langmuir-Freundlich models,and Clausius-Clapeyron equation was used to calculate the isosteric heat.Both the order of the adsorbed amount and the adsorption heat on the two adsorbents are CO_(2)>CH_(4)>N_(2).The adsorption kinetics are calculated by the pseudo-first kinetic model,and the order of adsorption rates on activated carbon is N_(2)-CH_(4)>CO_(2),while on carbon molecular sieve,it is CO_(2)-N_(2)>CH_(4).It is shown that relative molecular mass and adsorption heat are the primary effect on kinetics for activated carbon,while kinetic diameter is the main resistance factor for carbon molecular sieve.Moreover,the adsorption selectivity of CH_(4)/N_(2) and CO_(2)/N_(2) were estimated with the ideal adsorption solution theory,and carbon molecular sieve performed best at 318.15 K for both CO_(2) and CH_(4) separation.The study suggested that activated carbon is a better choice for separating flue gas and carbon molecular sieve can be a strong candidate for separating coal bed methane.

关键词： Activated carbon Carbon molecular sieve Adsorbent evaluation Adsorption equilibrium and kinetics Heat of adsorption Selectivity

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Regulating ion transport behaviors toward dendrite-free potassium metal batteries:recent advances and perspectives

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Rare Metals 2024年第4期43卷 1435-1460页

作者： Lu-Kang Zhao Xuan-Wen Gao Tian-Zhen Ren Da Wang Da-Wei Wang Zhao-Meng Liu Hong Chen Wen-Bin Luo school of Metallurgy Northeastern University school of chemical Engineering The University of New South Wales

With abundant potassium resources and high capacity,potassium metal batteries（PMBs） present a compelling option for the next generation of energy storage technology.However,PMBs suffer from an unstable anode interface caused by uncontrolled dendrite growth,which results in unsatisfactory cyclability and safety concerns.Extensive investigations suggest that significant progress has been made in enhancing the interfacial stability of PMBs.The various effective strategies for stabilizing interfaces can ultimately be attributed to the regulation of the sluggish ion transfer kinetics and irregular deposition,i.e.,the arrangement of ion transport behaviors at the interface.Rational modulation of ions transport rate and ions deposition directions makes it possible to obtain a dendrite-free and smooth deposition plane.Herein,the influencing factors and action mechanism of K+interface transport behaviors are discussed to understand the nature of material design for constructing stable anode interfaces,including regulating the solvation and desolvation structures,accelerating K+transport kinetics and controlling K+deposition direction.In addition,the deficiencies and prospects of the research on electrolyte,separators and designed electrode involved in the manufacturing and testing and ion transport process of PMBs are discussed.This review is expected to provide some possible directions for constructing dendrite-free interfaces in advanced PMBs-related research and offer significant insights for prospective experimental research and commercial applications.

关键词： Ion transport rate Ion transport direction Interface Potassium metal batteries Dendrites growth

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Recyclable hydrolyzed polymers of intrinsic microporosity-1/Fe_(3)O_(4) magnetic composites as adsorbents for selective cationic dye adsorption

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Frontiers of chemical Science and Engineering 2024年第2期18卷 113-125页

作者： Feng Zhang Shuainan Xu Xiumei Geng Meixia Shan Yatao Zhang school of chemical Engineering Zhengzhou UniversityZhengzhou 450001China

Polymers of intrinsic microporosity shows great potential for dye adsorption and magnetic Fe_(3)O_(4) are easy to be separated.In this work,hydrolyzed polymers of intrinsic microporosity-1/Fe_(3)O_(4) composite adsorbents were prepared by phase inversion and hydrolysis process for cationic dye adsorption.The chemical structure and morphology of the composite adsorbents were systematically characterized by several characterization methods.Using methylene blue as the target dye,the influences of solution pH,contact time,initial dye concentration,and system temperature on the methylene blue adsorption process were investigated.The incorporation of Fe_(3)O_(4) particle into hydrolyzed polymers of intrinsic microporosity-1 endow the adsorbent with high magnetic saturation(20.7 emu·g^(–1))which allows the rapid separation of the adsorbent.Furthermore,the adsorption process was simulated by adsorption kinetics,isotherms and thermodynamics to gain insight onto the intrinsic adsorption mechanism.In addition,the composite adsorbents are able to selectively adsorb cationic dyes from mixed dyes solution.Hydrolyzed polymers of intrinsic microporosity/Fe_(3)O_(4) shows only a slight decrease for methylene blue adsorption after 10 adsorption/regeneration cycles,demonstrating the outstanding regeneration performance.The high adsorption capacity,outstanding regeneration ability,together with simple preparation method,endow the composite adsorbents great potential for selective removal of cationic dyes in wastewater system.

关键词： polymers of intrinsic microporosity magnetic adsorbent cationic dye adsorption

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Preparation of PrFe_(x)Co_(1-x)O_(3)/Mt catalyst and study on degradation of 2-hydroxybenzoic acid wastewater by catalytic wet peroxide oxidation

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Chinese Journal of chemical Engineering 2024年第1期65卷 286-297页

作者： Binxia Zhao Yijia Gao Tiancheng Hun Xiaoxiao Fan Nan Shao Xiaoqian Chen school of chemical Engineering Northwest UniversityXi'an 710069China

In this study,the perovskite nanocomposite PrFe_(x)Co_(1-x)O_(3)(Pr(S))was successfully synthesized by the sol-gel method;PrFe_(x)Co_(1-x)O_(3)/Al-pillared montmorillonite(Pr(S)/Mt)catalysts were prepared by impregnation(D)method and solid-melting(G)method,respectively,with Pr(S)as the active component and Al-pillared montmorillonite as the carrier.The catalysts were applied to treat the 2-hydroxybenzoic acid(2-HA)-simulated wastewater by catalytic wet peroxide oxidation(CWPO)technique,and the chemical oxygen demand(COD)removal rate and the 2-HA degradation rate were used as indicators to evaluate the catalytic performance.The results of the experiment indicated that the solid-melting method was more conducive to preparing the catalyst when the Co/Fe molar ratio of 7:3 and the optimal structural properties of the catalysts were achieved.The influence of operating parameters,including reaction temperature,catalyst dosage,H_(2)O_(2)dosage,pH,and initial 2-HA concentration,were optimized for the degradation of 2-HA by CWPO.The results showed that 97.64%of 2-HA degradation and 75.23%of COD removal rate were achieved under more suitable experimental conditions.In addition,after the catalyst was used five times,the degradation rate of 2-HA could still reach 76.93%,which implied the high stability and reusability of the catalyst.The high catalytic activity of the catalyst was due to the doping of Co into PrFeO_(3),which could promote the generation of HO·,and the high stability could be attributed to the loading of Pr(S)onto Al-Mt,which reduced the leaching of reactive metals.The study of reaction mechanism and kinetics showed that the whole degradation process conformed to the pseudo-firstorder kinetic equation,and the Langmuir-Hinshelwood method was applied to demonstrate that catalysis was dominant in the degradation process.

关键词： Montmorillonite Perovskite Catalytic wet peroxide oxidation(CWPO) 2-Hydroxybenzoic acid

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The homogenous growth of Co-based coordination compound on graphene nanosheet for high-performance K-organic battery and its reaction mechanism

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Rare Metals 2024年第4期43卷 1622-1634页

作者： Qian-Qian Peng Yi-Ting Wang Shuo Qi Yao Xiao Yong Wang Shuang-Qiang Chen school of Environmental and chemical Engineering Shanghai University school of Chemistry and Materials Engineering Wenzhou University

Metal coordination compounds（MCCs） are gaining popularity for potassium-ion batteries（PIBs）owing to their tuneable structure,multiple reaction sites,low cost and unique morphology.However,they are generally subjected to intrinsic features of the sluggish ionic diffusion coefficient,low electronic conductivity and slow kinetics.Herein,a new MCC material of cobalt-1,3,5-trioxy-2,4,6-triamino-benzo（Co-TB） coordination compound was synthesized and homogenously grown on the surface of graphene nanosheets（GNS）,forming a Co-TB@GNS composite with enhanced electronic conductivity and flexible capability.Benefiting from the overall enhanced conductivity,high surface area and abundant activated K-storage sites,Co-TB@GNS electrodes have exhibited superior cycling performance with high reversible capacities(312 mAh·g-1after 100 cycles at 100 mA·g-1,224 mAh·g-1after 500 cycles at 1 A·g-1) and better rate performances compared with the pure Co-TB compound when served as PIB's anodes.Furthermore,multiple in-situ measurement techniques have jointly confirmed that the organic functional groups（C=O,C=N and C=C of benzene rings） and Co2+in Co-TB are the main reversible K-storage sites,including in-situ Fourier transform infrared spectroscopy（FTIR） and X-ray diffraction（XRD）,and partial capacity contribution is originated from GNS by the apparent K-storage behavior in the in-situ XRD pattern,proving the possibility of K-storage for metal-organic materials.

关键词： Metal coordination compounds Potassium-ion battery Cobalt coordination compound K-storage mechanism

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Thin polymer electrolyte with MXene functional layer for uniform Li^(+) deposition in all-solid-state lithium battery

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Green Energy & Environment 2024年第1期9卷 71-80页

作者： Weijie Kou Yafang Zhang Wenjia Wu Zibiao Guo Quanxian Hua Jingtao Wang school of chemical Engineering Zhengzhou UniversityZhengzhou450001China

Solid polymer electrolyte(SPE) shows great potential for all-solid-state batteries because of the inherent safety and flexibility;however, the unfavourable Li+deposition and large thickness hamper its development and application. Herein, a laminar MXene functional layer-thin SPE layer-cathode integration(MXene-PEO-LFP) is designed and fabricated. The MXene functional layer formed by stacking rigid MXene nanosheets imparts higher compressive strength relative to PEO electrolyte layer. And the abundant negatively-charged groups on MXene functional layer effectively repel anions and attract cations to adjust the charge distribution behavior at electrolyte–anode interface. Furthermore,the functional layer with rich lithiophilic groups and outstanding electronic conductivity results in low Li nucleation overpotential and nucleation energy barrier. In consequence, the cell assembled with MXene-PEO-LFP, where the PEO electrolyte layer is only 12 μm, much thinner than most solid electrolytes, exhibits uniform, dendrite-free Li+deposition and excellent cycling stability. High capacity(142.8 mAh g-1), stable operation of 140 cycles(capacity decay per cycle, 0.065%), and low polarization potential(0.5 C) are obtained in this Li|MXene-PEO-LFP cell,which is superior to most PEO-based electrolytes under identical condition. This integrated design may provide a strategy for the large-scale application of thin polymer electrolytes in all-solid-state battery.

关键词： MXene nanosheet Laminar functional layer Thin polymer electrolyte Dendrite-free Liþdeposition All-solid-state lithium battery

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Constructing core@shell structured photothermal nanosphere with thin carbon layer confined Co-Mn bimetals for pollutant degradation and solar interfacial water evaporation

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Rare Metals 2024年第4期43卷 1686-1701页

作者： Hong-Yang Zhu Meng-Ting Liu Gang Wang Rong-Rong Du Hong-Yao Zhao Hao Lu Shi-Qi Yang Sheng Tang Zeng-Jing Guo Jun Yang Cheng-Zhang Zhu Fu Yang school of Environmental and chemical Engineering Jiangsu University of Science and Technology school of Chemistry and chemical Engineering Liaocheng University school of Material Science and Engineering Jiangsu University of Science and Technology school of Environmental Science and Engineering Nanjing Tech University

Photothermal material applied in environmental governance has attracted growing attention.By combining the Stober method and dopamine-triggered coating strategy,Co-Mn precursor was in situ incorporated into the poly dopamine（PDA） layer over the surface of silica cores.Afterwards,a unique photothermal nanosphere with SiO2core and thin carbon layer and dual Co-Mn oxides shell was allowed to form by sequential heat treatment in the inert atmosphere（SiO2@CoMn/C）.The bimetallic fraction of Co/Mn in the carbon layer and post-treatment calcination temperature was comprehensively tuned to optimize the peroxymonosulfate（PMS） activation performance of the catalyst.The state of bimetallic species was studied including their physical distribution,chemical valence,and interplay by various characterizations.Impressively,Co oxides appear as dominant monodispersed nanoparticles（～ 10 nm）,while Mn with cluster-like morphology is observed to uniformly distribute over thin-layer carbon and adhered to the surface of SiO2nanospheres（～ 250 nm）.The calcined temperature could tune the oxidized state of Co species,leading to the optimization of the catalytic performance of introduced dual metal species.As a result,this obtained optimal catalyst integrated the advantages of exposed bimetallic CoMn species and N-doped thin carbon to deliver excellent catalytic PMS activation performance and photothermal synergetic catalytic mineralization ability for diversiform pollutants.Further reactions condition controls and anion interference studies were conducted to identify the adaptability of the optimal catalyst.Moreover,the application of solar-driven interfacial water evaporation using optimal SiO2@Co3Mn1/C-600 catalyst was explored,showing a high water evaporation rate of 1.48 kg·m-2·h-1and an efficiency of 95.2%,further revealing a comprehensive governance functionality of obtained material in the complex pollution condition.

关键词： Photothermal Peroxymonosulfate (PMS) activation Bimetallic synergy Water evaporation Advanced oxidation process

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Impact of Carbon Chain Structures in the Backbone on the Flexibility of Modified Polyarylene Sulfide Resins: Molecular Dynamics Simulations and Mesoscopic Analysis

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Chinese Journal of Polymer Science 2024年第4期42卷 544-557页

作者： Chi Zhang Rong Liu Jing-Yuan Liu Wen-Wei Jiang Key Laboratory of Fine chemical Engineering and Functional Materials School of Chemical EngineeringSichuan UniversityChengdu610065China

In the domain of high-performance engineering polymers, the enhancement of mechanical flexibility in poly(phenylene sulfide) (PPS) resins has long posed a significant challenge. A novel molecular structure, designated as PP-He-IS, wherein imide rings and an aliphatic hexylene chain are covalently incorporated into the PPS backbone to enhance its flexibility, is introduced in this study. Molecular dynamics (MD) simulations are employed to systematically explore the effects of diversifying the backbone chain structures by substituting phenyl units with alkyl chains of varying lengths, referred to as PP-A-IS where “A” signifies the distinct intermediary alkyl chain configurations. Computational analyses reveal a discernable decrement in the glass transition temperature (Tg) and elastic modulus, counterbalanced by an increment in yield strength as the alkyl chain length is extended. Notably, the PP-He-IS variant is shown to exhibit superior yield strength while simultaneously maintaining reduced elastic modulus and Tg values, positioning it as an advantageous candidate for flexible PPS applications. Mesoscopic analyses further indicate that structures such as PP-He-IS, PP-Pe-IS, and PP-Bu-IS manifest remarkable flexibility, attributable to the presence of freely rotatable carbon-carbon single bonds. Experimental validation confirms that a melting temperature of 504 K which is lower than that of conventional PPS, and lower crystallinity are exhibited by PP-He-IS, thereby affording enhanced processability without compromising inherent thermal stability. Novel insights into the strategic modification of PPS for mechanical flexibility are thus furnished by this study, which also accentuates the pivotal role played by molecular dynamics simulations in spearheading high-throughput investigations in polymer material modifications.

关键词： Molecular dynamics simulations Polyarylene Sulfide Main-chain modifications Flexibility Aliphatic hexylene chain

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Large-scale chiral spherulites with controllable circularly polarized luminescence in liquid crystal block copolymers film

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Aggregate 2024年第1期5卷 427-435页

作者： Jianan Yuan Xuemin Lu Qinghua Lu school of Chemistry and chemical Engineering Shanghai Jiao Tong UniversityShanghaiChina school of chemical Science and Engineering Tongji UniversityShanghaiChina

Macroscopic chiral spherulites prepared by hierarchical self-assembly have attracted considerable attention due to their excellent property as chiroptical materials.However,preparing controllable chiral spherulites in bulk film remains a challenge due to the absent knowledge of the evolution mechanism from the molecule to macroscopic crystal during chiral assembly.In this contribution,chiral macroscopic spherulites were constructed with controllable circularly polarized luminescence(CPL)using enantiomeric tartaric acid and rhodamine B co-assembled with liquid crystal block copolymers,poly(ethylene oxide)-b-poly(methyl methacrylate)bearing azobenzene group side chains.It was found that the chiral liquid crystal field induced by exogenous chiral molecules was closely related to the formation of macroscopic chiral spherulites.Moreover,the transformation of azobenzene cis-trans isomerization under photo-thermal endows films with adjustable CPL.This facile strategy provides a platform to design large-scale chiral structures for chiroptical switching,encryption,and memory storage materials.

关键词： block copolymer circularly polarized luminescence macroscopic chirality self-assembly

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