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Micelle-directed self-assembly of single-crystal-like mesoporous stoichiometric oxides for high-performance lithium storage

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National Science Review 2024年第4期11卷 195-205页

作者： Yanhua Wan Changyao Wang Xingmiao Zhang Yang Yin Mengmeng Liu Bing Ma Linlin Duan Yuzhu Ma Wei Zhang Changlin Zheng Dongliang Chao Fei Wang Yongyao Xia Wei Li Department of Chemistry Laboratory of Advanced Materials Shanghai Key Laboratory of Molecular Catalysis and Innovative Materials State Key Laboratory of Molecular Engineering of Polymers College of Chemistry and Materials ScienceFudan University state key laboratory of Surface Physics and Department of Physics Fudan University

Due to their uncontrollable assembly and crystallization process,the synthesis of mesoporous metal oxide single crystals remains a formidable challenge.Herein,we report the synthesis of single-crystal-like mesoporous Li2TiSiO5by using soft micelles as templates.The key lies in the atomic-scale self-assembly and step-crystallization processes,which ensure the formation of single-crystal-like mesoporous Li2TiSiO5microparticles via an oriented attachment growth mechanism under the confinement of an in-situ formed carbon matrix.The mesoporous Li2TiSiO5anode achieves a superior rate capability(148 mAh g-1at5.0 A g-1) and outstanding long-term cycling stability(138 mAh g-1after 3000 cycles at 2.0 A g-1) for lithium storage as a result of the ultrafast Li+diffusion caused by penetrating mesochannels and nanosized crystal frameworks（5-10 nm）.In comparison,bulk Li2TiSiO5exhibits poor rate capability and cycle performance due to micron-scale diffusion lengths.This method is very simple and reproducible,heralding a new way of designing and synthesizing mesoporous single crystals with controllable frameworks and chemical functionalities.

关键词： mesoporous materials micelles single-crystal-like Li2TiSiO5 lithium-ion batteries

Micro/nano flow chemistry by Beyond Limits Manufacturing

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Chinese Chemical Letters 2024年第5期35卷 3-12页

作者： Peiwen Liu Fang Zhao Jing Zhang Yunpeng Bai Jinxing Ye Bo Bao Xinggui Zhou Li Zhang Changlu Zhou Xinhai Yu Peng Zuo Jianye Xia Lian Cen Yangyang Yang Guoyue Shi Lin Xu Weiping Zhu Yufang Xu Xuhong Qian 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 state key laboratory of bioreactor engineering Shanghai Collaborative Innovation Center for BiomanufacturingEast China University of Science and TechnologyShanghai 200237China School of Biomedical and Pharmaceutical Sciences Guangdong University of TechnologyGuangzhou 510006China School of Mechanical and Power engineering East China University of Science and TechnologyShanghai 200237China Shanghai key laboratory of Green Chemistry and Chemical Processes Department of ChemistrySchool of Chemistry and Molecular EngineeringEast China Normal UniversityShanghai 200241China

In September 2018,we proposed the cutting-edge concept of“Beyond Limits Manufacturing”(BLM).BLM technology is based on the three-dimensional inner engraving or precise outer engraving of ultra-fast laser,to invent micro/nano scale flow chips or devices,which makes it possible for the microform,integration,economy,safety,high efficiency,green and intelligence of research,development and manufacturing process,so as to realize transformational manufacturing in the era of Industry 4.0.In this paper,we reviewed the representative results we made in the field of micro/nano flow chemistry during the implementation of the BLM major project(December 2019 to August 2023),and discussed its application prospects in micro/nano flow chemistry.

关键词： Beyond Limits Manufacturing Flow chemistry Pharmaceutical manufacturing Microreactor

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 manufacturing.While 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 personnels.In 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 algorithm.Research 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

Palladium-Catalyzed anti-Markovnikov Halosulfonamidation of Unactivated Alkene

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Chinese Journal of Chemistry 2024年第5期42卷 464-470页

作者： Bowen Wang Jianxiao Li Wanqing Wu Huanfeng Jiang state key laboratory of Pulp and Paper engineering Key Laboratory of Functional Molecular Engineering of Guangdong ProvinceSchool of Chemistry and Chemical EngineeringSouth China University of TechnologyGuangzhouGuangdong510641 China

Palladium-catalyzed regioselective amination of unactivated alkene remains a challenge and is of great interest.Herein,a three-component coupling of unactivated alkene,sulfonamide,and N-halo compounds accessing vicinal haloamine has been conceived.This aminohalogenation represents a modular and regioselective strategy.The electrophilic halogenating agent enables regioselective anti-Markovnikov aminopalladation and facilitates subsequent halogenation events.And this protocol is characterized by gram-scale syntheses and late-stage functionalizations.Of note,the recovered byproduct phthalimide allows for reusing by conversion to the starting material.

关键词： Unactivated alkene anti-Markovnikov aminopalladation Vicinal haloamine Palladium catalysis Halosulfonamidation Selectivity N-Halo compounds

Effects of serum proteins on corrosion rates and product bioabsorbability of biodegradable metals

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Regenerative Biomaterials 2024年第1期3卷 132-148页

作者： Hongjie Zhang Xin Li Zehua Qu Wanqian Zhang Qunsong Wang Dinglingge Cao Yaoben Wang Xin Wang Yang Wang Lin Yu Jiandong Ding state key laboratory of Molecular engineering of Polymers Department of Macromolecular ScienceFudan UniversityShanghai 200438China

Corrodible metals are the newest kind of biodegradable materials and raise a new problem of the corrosion products.However,the removal of the precipitated products has been unclear and even largely ignored in publications.Herein,we find that albumin,an abundant macromolecule in serum,enhances the solubility of corrosion products of iron in blood mimetic Hank’s solution significantly.This is universal for other main biodegradable metals such as magnesium,zinc and polyester-coated iron.Albumin also influences corrosion rates in diverse trends in Hank’s solution and normal saline.Based on quantitative study theoretically and experimentally,both the effects on corrosion rates and soluble fractions are interpreted by a unified mechanism,and the key factor leading to different corrosion behaviors in corrosion media is the interference of albumin to the Ca/P passivation layer on the metal surface.This work has illustrated that the interactions between metals and media macromolecules should be taken into consideration in the design of the next-generation metal-based biodegradable medical devices in the formulism of precision medicine.The improved Hank’s solution in the presence of albumin and with a higher content of initial calcium salt is suggested to access biodegradable metals potentially for cardiovascular medical devices,where the content of calcium salt is calculated after consideration of chelating of calcium ions by albumin,resulting in the physiological concentration of free calcium ions.

关键词： biodegradable metal macromolecule albumin corrosion bioabsorbability iron polylactide magnesium zinc

Microfluidic-oriented synthesis of enriched iridium nanodots/carbon architecture for robust electrocatalytic nitrogen fixation

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Green Energy & Environment 2024年第3期9卷 544-555页

作者： Hengyuan Liu Xingjiang Wu Yuhao Geng Xin Li Jianhong Xu The state key laboratory of Chemical engineering Department of Chemical EngineeringTsinghua UniversityBeijing100084China

Electrocatalytic nitrogen reduction reaction(NRR)is considered as a promising candidate to achieve ammonia synthesis because of clean electric energy,moderate reaction condition,safe operating process and harmless by-products.However,the chemical inertness of nitrogen and poor activated capacity on catalyst surface usually produce low ammonia yield and faradic efficiency.Herein,the microfluidic technology is proposed to efficiently fabricate enriched iridium nanodots/carbon architecture.Owing to in-situ co-precipitation reaction and microfluidic manipulation,the iridium nanodots/carbon nanomaterials possess small average size,uniform dispersion,high conductivity and abundant active sites,producing good proton activation and rapid electrons transmission and moderate adsorption/desorption capacity.As a result,the as-prepared iridium nanodots/carbon nanomaterials realize large ammonia yield of 28.73 μg h^(-1) cm^(-2) and faradic efficiency of 9.14%in KOH solution.Moreover,the high ammonia yield of 11.21 μg h^(-1) cm^(-2) and faradic efficiency of 24.30%are also achieved in H_(2)SO_(4) solution.The microfluidic method provides a reference for large-scale fabrication of nano-sized catalyst materials,which may accelerate the progress of electrocatalytic NRR in industrialization field.

关键词： Iridium nanodots Carbon Microfluidic technology Efficient synthesis Electrocatalytic nitrogen fixation

Two-dimensional ballistic transistors for advanced-node integrated circuits

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National Science Review 2024年第3期11卷 9-10页

作者： Jia Li Xidong Duan Hunan Provincial key laboratory of Two-Dimensional Materials State Key Laboratory for Chemo/Biosensing and Chemometrics College of Chemistry and Chemical Engineering Hunan University

As the feature size of metal-oxide-semiconductor-field-effect-transistors(MOSFETs) in integrated circuits(ICs)is reduced to sub-10-nm, the traditional channel materials are plagued by enhanced scattering and short-cha... 详细信息

关键词： CONTACT

Promoting effect of FeOx addition on the mechanochemically prepared vanadium-based catalyst for real PCDD/Fs removal and mechanism insight

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Journal of Environmental Sciences 2024年第3期137卷 478-487页

作者： Minghui Tang Ling Wang Hongxian Li Xinlei Huang Cuicui Du Shengyong Lu state key laboratory for Clean Energy Utilization Institute for Thermal Power EngineeringZhejiang UniversityHangzhou 310027China

Industrial-use VOx-based catalysts usually have a higher active temperature window (>250-300℃),which becomes a“bottleneck”for the practical application of PCDD/Fs catalytic degradation technology.In this work,VO_(x)-FeO_(x)/TiO_(2) catalyst prepared via mechanochemically method was investigated for the catalytic removal of PCDD/Fs.The removal efficiency of 1,2-DCBz,pure PCDD/Fs gas generated in the lab,PCDD/Fs from actual fue gas,long-term were studied,and the degradation mechanism was explored using FTIR and TOFMS.The degradation efficiency of 1,2-DCBz and PCDD/Fs on VO_(x)-FeO_(x)/TiO_(2) were higher than that of VO_(x)/TiO_(2)catalyst,and the optimal FeOx addition ratio was 3 wt.%.The characterization results show that the addition of FeOx can effectively improve the pore structure,surface acidity,and VOx dispersion of the catalyst,thus contributing to increasing the V^(5+)content and surface-active oxygen,which is conducive to the improvement of adsorption and redox performance of the catalyst.Under the actual MSWI (municipal solid waste incineration)fue gas,the PCDD/Fs removal efficiency over VTi-3Fe-MC maintained long-term stability,higher than 85%for 240 min.This result was not significantly reduced compared with the data obtained in the laboratory.According to the analysis results of intermediate products by FTIR and GC-TOFMS,it can be inferred that the epoxidation fracture of benzene ring is the rate-limiting step of dioxin catalytic degradation reaction.This work gives an in-depth view into the PCDD/Fs removal over VO_(x)-FeO_(x)/TiO_(2) catalysts and could provide guidelines for the rational design of reliable catalysts for industrial applications.

关键词： PCDD/F removal MSWI fue gas VO_(x)-FeO_(x)/TiO_(2) Mechanochemical GC-TOFMS

Preparation of Self-limiting Heating Cables with Excellent Processability, Mechanical Properties and PTC Effect via Thermal and Electrical Treatments

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Chinese Journal of Polymer Science 2024年第4期42卷 511-520页

作者： Tian-Hao Yang Tong Wu Qiang Fu state key laboratory of Polymer Materials engineering College of Polymer Science and EngineeringSichuan UniversityChengdu610065China state key laboratory of Polymer Materials engineering Polymer Research Institute of Sichuan UniversityChengdu610065China

Polymer/conductive filler composites have been widely used for the preparation of self-limiting heating cables with the positive temperature coefficient (PTC) effect. The control of conductive filler distribution and network in polymer matrix is the most critical for performance of PTC materials. In order to compensate for the destruction of the filler network structure caused by strong shearing during processing, an excessive conductive filler content is usually added into the polymer matrix, which in turn sacrifices its processability and mechanical properties. In this work, a facile post-treatment of the as-extruded cable, including thermal and electrical treatment to produce high-density polyethylene (HDPE)/carbon black (CB) cable with excellent PTC effect, is developed. It is found for the as-extruded sample, the strong shearing makes the CB particles disperse uniformly in HDPE matrix, and 25 wt% CB is needed for the formation of conductive paths. For the thermal-treated sample, a gradually aggregated CB filler structure is observed, which leads to the improvement of PTC effect and the notable reduction of CB content to 20 wt%. It is very interesting to see that for the sample with combined thermal and electrical treatment, CB particles are agglomerated and oriented along the electric field direction to create substantial conductive paths, which leads to a further decrease of CB content down to 15 wt%. In this way, self-limiting heating cables with excellent processability, mechanical properties and PTC effect have simultaneously been achieved.

关键词： Self-limiting heating cables Positive temperature coefficient Thermal treatment Electrical treatment