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Antibonding orbital tailor and stress relief engineering for FeS_(2)complex toward superior sodium storage

Rare Metals 2024年第10期43卷 5048-5059页

作者： You-Bin Zhang Zhen-Guo Qi Fu-Sheng Liu Guo-Hui Qin State Key Laboratory Base for Eco-Chemical Engineering College of Chemical EngineeringQingdao University of Science and TechnologyQingdao 266042China Shandong Synergetic Innovation Center of Ecological and Chemical Engineering Qingdao 266042China

The sluggish kinetics behaviors and vast volume variations of Na^(+)hosts to FeS_(2)anode involved intercalation,and conversion reactions plague its applicability of sodium-ion batteries(SIBs).Here,a significantly expedited kinetics via cation intercalation and considerably relieved stress accumulation by constructing the concave scaffold protector are approached for FeS_(2)*** Mn^(2+)intercalation into FeS_(2),a new stable Mn-FeS_(2)was generated with distorted coordination;elevated antibonding orbital occupancy and lowed d band center to the release of more free Na^(+)were achieved,which was further encapsulated by hollow bowl-like carbon spheres(BC)This cation intercalation and concave morphology strategies confer Mn-FeS_(2)@BC significantly enhanced electron ion transport kinetics via reversed electron transfer to FeS_(2)fast desolvation kinetics,and evidently depressed structural deformation during Na^(+)insertion and ***,Mn-FeS_(2)@BC delivers the longevity and stable Na^(+)storage capacity in both half and full cell ***,Mn-FeS_(2)@BC also displays excellen adaptability in a wider temperature *** work proposes new views into the deep regulation of electrochemical performance of transition metal anodes via intercalation chemistry and concave engineering.

关键词： FeS_(2) Intercalation chemistry Concave engineering Sodium capture

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NIR-Ⅱ responsive Janus nanoparticles amplify immunogenic cell death for enhanced cancer immunotherapy

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Science China(Technological Sciences) 2024年第1期67卷 321-329页

作者： CHEN BeiBei GUO KangLi WANG HaoRan XU Fu-Jian WANG JuLin ZHAO NaNa State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China Key Laboratory of Biomedical Materials of Natural Macromolecules(Beijing University of Chemical Technology) Beijing Laboratory of Biomedical MaterialsBeijing University of Chemical TechnologyBeijing 100029China College of Materials Sciences and Engineering Beijing University of Chemical TechnologyBeijing 100029China Beijing Key Laboratory of Electrochemical Process and Technology for Materials Beijing University of Chemical TechnologyBeijing 100029China

Immunotherapy brings new hope for tumor treatment by inducing immunogenic cell death(ICD)of tumor ***,insufficient immunogenicity and low immune response rate greatly limit antitumor ***,by optimizing the composition and morphology,the rational design of Janus nanoparticles composed of Fe_(3)O_(4) nanospheres and SiO_(2)nanorods was realized for enhanced cancer immunotherapy through amplified *** glucose oxidase(GOx)was loaded by the Janus nanoparticles,the resultant M-FS-GOx consumes glucose at tumor sites to generate gluconic acid and hydrogen peroxide(H_(2)O_(2))for starvation therapy while the H_(2)O_(2)supply promotes the production of highly toxic·OH to achieve effective chemodynamic therapy(CDT).Under a 1064 nm light irradiation,the photothermal effect of M-FS-GOx enhances the enzyme activity of GOx for improved starvation ***,both tumor-associated antigens released during the process of ICD and the intrinsic immunoadjuvant property of M-FS-GOx stimulate dendritic cell maturation to activate antitumor immune *** work provides a promising strategy for the construction of Janus nanoparticles to achieve enhanced cancer immunotherapy through combination therapy-amplified ICD.

关键词： Janus nanoparticles immunogenic cell death cancer immunotherapy

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Experiments and kinetic modeling of the sorbitol dehydration to isosorbide catalyzed by sulfuric acid under conditions of non-constant volume

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Chinese Journal of chemical engineering 2024年第9期73卷 281-289页

作者： Dechang Cheng Zhihong Ma Ziyang Liu Xiaohui Liu Tao Liu Weizhen Sun Ling Zhao State Key Laboratory of Chemical Engineering School of Chemical EngineeringEast China University of Science and TechnologyShanghai 200237China Shanghai Key Laboratory of Functional Materials Chemistry Research Institute of Industrial CatalysisSchool of Chemistry and Molecular EngineeringEast China University of Science and TechnologyShanghai 200237China

Isosorbide is a novel bio-based material derived as a secondary dehydration product of *** work focuses on the kinetics of sulfuric acid-catalyzed dehydration of sorbitol under conditions of nonconstant ***,the effects of stirring rate,catalyst dosage,reaction temperature,and reaction time on the dehydration reaction of sorbitol were *** yield of isosorbide up to 77.13%was obtained after 1.5 h of reaction time under conditions of 2 kPa,1.0%(mass)catalyst dosage,and 413.15 *** on the sorbitol dehydration reaction mechanism and a simplified reaction network,a kinetic model was developed in this work.A good agreement was accomplished between kinetic modeling and experiments between 393.15 and 423.15 *** fitting results indicate that side reactions with higher activation energies are more affected by reaction temperatures,and the main side reaction that influences the selectivity of isosorbide is the oligomerization reaction among the primary dehydration products of *** model fitting of the catalyst amounts effect shows that the effective concentration of sulfuric acid would be reduced with the increase of dosage due to the molecular agglomeration ***,the kinetic experiments and modeling results obtained in this work will be helpful to the design and optimization of the industrial sorbitol dehydration process.

关键词： Isosorbide Sorbitol dehydration Non-constant volume Kinetic modeling

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Kinetics insights into size effects of carbon nanotubes'growth and their supported platinum catalysts for 4,6-dinitroresorcinol hydrogenation

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Chinese Journal of chemical engineering 2024年第8期72卷 133-140页

作者： Yan Zhang Xiangxue Zhang Keng Sang Wenyao Chen Gang Qian Jing Zhang Xuezhi Duan Xinggui Zhou Weikang Yuan State Key Laboratory of Chemical Engineering East China University of Science and TechnologyShanghai 200237China

Size effects are a well-documented phenomenon in heterogeneous catalysis,typically attributed to alterations in geometric and electronic *** this study,we investigate the influence of catalyst size in the preparation of carbon nanotube(CNT)and the hydrogenation of 4,6-dinitroresorcinol(DNR)using Fe_(2)O_(3)and Pt catalysts,*** Fe_(2)O_(3)/Al_(2)O_(3)catalysts were synthesized for CNT growth through catalytic chemical vapor *** findings reveal a significant influence of Fe_(2)O_(3)nanoparticle size on the structure and yield of ***,CNT produced with Fe_(2)O_(3)/Al_(2)O_(3)containing 28%(mass)Fe loading exhibits abundant surface defects,an increased area for metal-particle immobilization,and a high carbon *** makes it a promising candidate for DNR *** this catalyst support,we further investigate the size effects of Pt nanoparticles on DNR *** Pt catalysts demonstrate a preference for 4,6-diaminoresorcinol generation at(100)sites,whereas smaller Pt catalysts are more susceptible to electronic *** kinetics insights obtained from this study have the potential to pave the way for the development of more efficient catalysts for both CNT synthesis and DNR hydrogenation.

关键词： Kinetics Size effects Catalytic hydrogenation Active site

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Comprehensive treatment of latex wastewater and resource utilization of concentrated liquid

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Chinese Journal of chemical engineering 2023年第5期57卷 183-192页

作者： Shichao Tian Yuming Tu Rujie Li Yufan Du Zhiyong Zhou Fan Zhang Zhongqi Ren State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China

Latex wastewater is a kind of refractory organic wastewater containing high concentrations of organics and ammonia *** this work,the combined process of forward osmosis(FO)and reverse osmosis(RO)was designed to treat the latex wastewater in the whole process,achieving the water recovery rate of 99%and basically no waste discharge after the catalytic oxidation *** turbidity of the latex wastewater was decreased to below 1 NTU by microfiltration pretreatment,and then using MgCl_2 worked as the draw solution for FO process to treat the latex *** operation conditions including adding acid or scale inhibitor as the pretreatment methods were conducted to improve the treatment performance of the combined *** the treatment of the whole process,the concentration of COD was less than 20 mg·L^(-1),the concentration of NH_3-N was less than 10 mg·L^(-1),and the concentration of TP was less than 0.5 mg·L^(-1)for the treated latex *** water quality met standards of industrial water reuse after the complete analysis of the treated latex wastewater,meanwhile,useful substances of L-Quebrachitol(L-Q)were successfully extracted from the concentrated ***,the combined process of FO and RO could realize the efficient treatment and reuse of latex wastewater,which provided with some important guidance on the industrial application.

关键词： Latex wastewater Resource utilization Forward osmosis Reverse osmosis Concentrated liquid

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Low temperature one-pot synthesis of 1,1-diethoxyethane from ethanol on Bi/BiCeO_(x)with strong metal-support interactions

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Nano Research 2023年第3期16卷 3709-3718页

作者： Zhe An Jiayu Liu Meng Cao Jian Zhang Yanru Zhu Hongyan Song Xu Xiang Jing He State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China

The direct conversion of ethanol to 1,1-diethoxyethane(DEE)through one-pot dehydrogenation-acetalization has attracted broad interest from both academia and *** on thermodynamics,the oxidative dehydrogenation of alcohol to acetaldehyde requires high temperature to activate oxygen to realize the C-H cleavage,while the acetalization of acetaldehyde with ethanol is exothermic reversible reaction favorable at low *** mismatching of the reaction condition for the two consecutive steps makes it a great challenge to achieve both high ethanol conversion and high DEE *** work reports a highly efficient bi-functional catalysis by Bi/BiCeO_(x)for one-pot oxidative dehydrogenation-acetalization route from ethanol to DEE under 150℃and ambient pressure,affording a selectivity of 98.5%±0.5%to DEE at an ethanol conversion of 87.0%±1.0%.An efficient tandem catalysis has been achieved on the interfacial Bi^(δ)+-Ov-Ce^(III)sites in Bi/BiCeO_(x)established by strong metal-support interaction,in which Biδ+-Ov-sites contribute to the oxidative dehydrogenation of ethanol at mild temperature,and-Ov-CeIII sites to the subsequent acetalization between the generated acetaldehyde and ethanol.

关键词： ethanol conversion 1 1-diethoxyethane strong metal-support interaction Biδ+-Ov-CeIII sites

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Adsorption of rubidium ion from aqueous solution by surface ion imprinted materials

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Chinese Journal of chemical engineering 2023年第2期54卷 1-10页

作者： Zhongqi Ren Jie Wang Hewei Zhang Fan Zhang Shichao Tian Zhiyong Zhou State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China

A new type of rubidium ion-imprinted polymer has been synthesized by the surface-imprinting technique using methacrylic acid as the functional monomer,the rubidium ion as the template,methanol as the solvent,and silica as a *** glycol dimethacrylate and 2,2-azobisisobutyronitrile were used as acrosslinker and an initiator,*** addition,based on the macrocyclic effect of crown ethers,the 18-crown-6 ligand was introduced as a ligand to fix the template ions *** electron microscopy,zeta-potential analysis,Fourier transform infrared spectroscopy,thermogravimetric analysis,and X-ray photoelectron spectroscopy were performed to characterize the ion-imprinted *** effects of the preparation and adsorption conditions on the adsorption performance of the rubidium ion-imprinted polymer were *** results indicated that the rubidium ion-imprinted polymer has high selectivity and faster kinetics than other adsorbents,with an equilibrium adsorption capacity of 200.19 mg·g^(-1)at 298 K within 25 *** sorption isotherm was well described by the Freundlich isotherm model,while the adsorption kinetics fitted the pseudo-second-order kinetic *** adsorption-desorption experiments showed that the ion-imprinted polymer had good chemical stability and reusability.

关键词： Surface-imprinted material Adsorption Aqueous solution Silica Selectivity

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Efficient selective activation of sorbitol C–O bonds over C–C bonds on CoGa(221)generated by lattice-induction strategy

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Nano Research 2023年第5期16卷 6200-6211页

作者： Ying Kong Yanru Zhu Zhe An Jian Zhang Xin Shu Hongyan Song Qipeng Yuan Jing He State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China

Sorbitol is a primary platform compound in the conversion of *** conversion of sorbitol to C_(6) hydrocarbons requires a complete cleavage of C–O bonds and meanwhile the inhibition of C–C ***,we demonstrated an efficient selective cleavage of C–O over C–C bond on the(221)facet of supported CoGa.A selectivity of 94%to C_(6) hydrocarbon with conversion of 97%has been *** selective C–O cleavage was demonstrated by tuning the exposed facet as(221)or(110).The supported CoGa was prepared simply by reduction of Co and Ga-containing layered double hydroxides(CoZnGaAl-LDHs),the exposed facets of CoGa crystallites were controlled by tailoring the temperature-programmed rate in the *** reducing CoZnGaAl-LDHs,CoGa(221)was exposed with a temperature-programmed rate of 5℃/min under the induction of ZnO lattice,while CoGa(110)was exposed with a rate of 10℃/min.

关键词： biomass supported CoGa facet exposure preferred C–O activation liquid hydrocarbons

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Highly selective and green recovery of lithium ions from lithium iron phosphate powders with ozone

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Frontiers of chemical Science and engineering 2023年第6期17卷 749-758页

作者： Ruiqi Li Kang Li Wei Wang Fan Zhang Shichao Tian Zhongqi Ren Zhiyong Zhou State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China

Since lithium iron phosphate cathode material does not contain high-value metals other than lithium,it is therefore necessary to strike a balance between recovery efficiency and economic benefits in the recycling of waste lithium iron phosphate cathode ***,we describe a selective recovery process that can achieve economically efficient recovery and an acceptable lithium leaching *** the acid concentration and amount of oxidant enables selective recovery of lithium *** is retained in the leaching residue as iron phosphate,which is easy to *** effects of factors such as acid concentration,acid dosage,amount of oxidant,and reaction temperature on the leaching of lithium and iron are comprehensively explored,and the mechanism of selective leaching is *** process greatly reduces the cost of processing equipment and *** increases the potential industrial use of this process and enables the green and efficient recycling of waste lithium iron phosphate cathode materials in the future.

关键词： lithium iron phosphate powder stoichiometric number selective leaching lithium recovery

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Preparation of sodium alginate gel microspheres catalysts and its high catalytic performance for treatment of ciprofloxacin wastewater

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Chinese Journal of chemical engineering 2023年第11期63卷 158-170页

作者： Gaoyan Shao Jianjie Chen Yuming Tu Feng Liu Zhiyong Zhou Shichao Tian Zhongqi Ren State Key Laboratory of Chemical Resource Engineering Beijing University of Chemical TechnologyBeijing 100029China

The discharge of the antibiotic wastewater has increased dramatically in our country with the development of medical science and wide application of antibiotic,resulting in serious harm to human body and ecological *** this work,ciprofloxacin(CIP)was selected as one of typical antibiotics and heterogeneous Fenton-like catalysts were prepared for the treatment of ciprofloxacin *** sodium alginate(SA)gel microspheres catalysts were prepared by polymerization method using double metal ions of Fe^(3+)and Mn^(2+)as cross-linking *** conditions such as metal ions concentration,mass fraction of SA,polymerization temperature and dual-metal ions as crosslinking agent were ***,the effects of operating conditions such as initial concentration of CIP,pH value and catalyst dosage on CIP removal were *** kinetic equation showed that the effect of the initial concentration of CIP on the degradation rate was in line with second-order kinetics,and the effects of catalyst dosage and pH value on the degradation rate of CIP were in line with first-order *** SA gel microspheres catalysts prepared by dual-metal ions exhibited a high CIP removal and showed a good reusability after six *** SA gel microspheres catalysts with an easy recovery performance provided an economical and efficient method for the removal of antibiotics in the future.

关键词： Sodium alginate gel microspheres Heterogeneous Fenton-like catalysts Dual-metal ions Hydroxyl radical Ciprofloxacin wastewater

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