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Photochemical cycloaddition and temperature-dependent breathing in pillared-layer metal–organic frameworks

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Science Bulletin 2019年第24期64卷 1881-1889页

作者： qingqing pang Binbin Tu Lingyi Yang Qiaowei Li Department of Chemistry Collaborative Innovation Center of Chemistry for Energy Materials (iChEM) and Shanghai Key Laboratory of Molecular Catalysis and InnovativeMaterials Fudan University

Single crystallinity of metal–organic frameworks(MOFs) enables the studies of their flexible behaviors with atomic precision. Here, we investigated the structural transformations triggered by photochemical cycloaddition and with temperature-dependent breathing in a series of pillared-layer MOF structures using a variety of pyrazolecarboxylate linkers for the layers and bipyridyl linkers as the pillars. The ethylenic double bonds from the pillars in close proximity undergo quantitative and seteroselective photochemical [2 + 2] cycloaddition upon UV irradiation, transforming the MOFs into structures with cyclobutane-based pillars. Furthermore, reversible breathing of the new pillared-layer MOF was evidenced by the 10.8% unit cell parameter change along c axis upon temperature change between 298 and 173 K. As revealed by single crystal X-ray diffraction, this transformation originates from the relative flattening of the wavy layers upon cooling. These two different types of characteristic structural transformations responding to inherent reactions and external stimuli happen at single crystalline state, providing a well-defined robust system with controlled flexibility.

关键词： Pillared-layer MOF Photochemical cycloaddition Structural transformation Breathing MOF Reticular chemistry

Complex-frequency waves:beat loss and win sensitivity

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Light(Science & Applications) 2024年第2期13卷 181-183页

作者： qingqing Cheng Tao L School of Optical-Electrical and Computer Engineering University of Shanghai for Science and TechnologyShanghai200093China Department of Respiratory Diseases and Critical Medicine Quzhou Hospital Affiliated to Wenzhou Medical UniversityQuzhou324000China National Laboratory of Solid State Microstructures College of Engineering and Applied SciencesNanjing UniversityNanjing210093China

Recent experiments have demonstrated that synthesized complex-frequency waves can impart a virtual gain to molecule sensing systems,which can effectively restore information lost due to intrinsic molecular *** enhancement notably amplifies the signal of trace molecular vibrational fingerprints,thereby substantially improving the upper limit of sensitivity.

关键词： thereby Complex limit

Stabilization and Blow-up in an Infinite Memory Wave Equation with Logarithmic Nonlinearity and Acoustic Boundary Conditions

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Journal of Systems Science & Complexity 2024年第4期37卷 1368-1391页

作者： PENG qingqing ZHANG Zhifei School of Mathematics and Statistics Huazhong University of Science and TechnologyWuhan 430074China Hubei Key Laboratory of Engineering Modeling and Scientific Computing Huazhong University of Science and TechnologyWuhan 430074China

In this paper,the authors consider the stabilization and blow up of the wave equation with infinite memory,logarithmic nonlinearity and acoustic boundary *** authors discuss the existence of global solutions for the initial energy less than the depth of the potential well and investigate the energy decay estimates by introducing a Lyapunov ***,the authors establish the finite time blow up results of solutions and give the blow up time with upper bounded initial energy.

关键词： Acoustic boundary condition finite time blow-up general decay infinite memory logarithmic nonlinearity

Supramolecular Biomaterials for Cancer Immunotherapy

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Research 2024年第2期2023卷 491-509页

作者： Huan Liang qingqing Lu Jie Yang Guocan Yu College of Science Nanjing Forestry UniversityNanjing 210037P.R.China Key Laboratory of Bioorganic Phosphorus Chemistry&Chemical Biology Department of ChemistryTsinghua UniversityBeijing 100084P.R.China

Cancer immunotherapy has achieved tremendous successful clinical results and obtained historic victories in tumor ***,great limitations associated with feeble immune responses and serious adverse effects still cannot be neglected due to the complicated multifactorial etiology and pathologic microenvironment in *** rapid development of nanomedical science and material science has facilitated the advanced progress of engineering biomaterials to tackle critical *** supramolecular biomaterials with flexible and modular structures have exhibited unparalleled advantages of high cargo-loading efficiency,excellent biocompatibility,and diversiform immunomodulatory activity,thereby providing a powerful weapon for cancer *** past decades,supramolecular biomaterials were extensively explored as versatile delivery platforms for immunotherapeutic agents or designed to interact with the key moleculars in immune system in a precise and controllable *** this review,we focused on the crucial role of supramolecular biomaterials in the modulation of pivotal steps during tumor immunotherapy,including antigen delivery and presentation,T lymphocyte activation,tumor-associated macrophage elimination and repolarization,and myeloid-derived suppressor cell *** on extensive research,we explored the current limitations and development prospects of supramolecular biomaterials in cancer immunotherapy.

关键词： biomaterials limitations thereby

Emerging perovskite materials for supercapacitors:Structure,synthesis,modification,advanced characterization,theoretical calculation and electrochemical performance

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Journal of Energy Chemistry 2024年第2期89卷 41-70,I0003页

作者： Yuehua Qian qingqing Ruan Mengda Xue Lingyun Chen Department of Applied Chemistry School of Chemistry and Chemical EngineeringChongqing UniversityChongqing 401331China

As a new generation electrode materials for energy storage,perovskites have attracted wide attention because of their unique crystal structure,reversible active sites,rich oxygen vacancies,and good *** this review,the design and engineering progress of perovskite materials for supercapacitors(SCs)in recent years is ***,the review will focus on four types of perovskites,perovskite oxides,halide perovskites,fluoride perovskites,and multi-perovskites,within the context of their intrinsic structure and corresponding electrochemical performance.A series of experimental variables,such as synthesis,crystal structure,and electrochemical reaction mechanism,will be carefully analyzed by combining various advanced characterization techniques and theoretical *** applications of these materials as electrodes are then featured for various ***,we look forward to the prospects and challenges of perovskite-type SCs electrodes,as well as the future research direction.

关键词： Perovskite Modification engineering Oxygen vacancy Theoretical calculation methodology Supercapacitor

Emerging two-dimensional Mo-based materials for rechargeable metal-ion batteries:Advances and perspectives

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Journal of Energy Chemistry 2024年第2期89卷 487-518,I0012页

作者： qingqing Ruan Yuehua Qian Mengda Xue Lingyun Chen Qichun Zhang Department of Applied Chemistry School of Chemistry and Chemical EngineeringChongqing UniversityChongqing 401331China Department of Materials Science and Engineering City University of Hong Kong999077Hong KongChina

With the rapid development of rechargeable metal-ion batteries(MIBs)with safety,stability and high energy density,significant efforts have been devoted to exploring high-performance electrode *** recent years,two-dimensional(2D)molybdenum-based(Mo-based)materials have drawn considerable attention due to their exceptional characteristics,including low cost,unique crystal structure,high theoretical capacity and controllable chemical ***,like other transition metal compounds,Mo-based materials are facing thorny challenges to overcome,such as slow electron/ion transfer kinetics and substantial volume changes during the charge and discharge *** this review,we summarize the recent progress in developing emerging 2D Mo-based electrode materials for MIBs,encompassing oxides,sulfides,selenides,*** introducing the crystal structure and common synthesis methods,this review sheds light on the charge storage mechanism of several 2D Mo-based materials by various advanced characterization *** latest achievements in utilizing 2D Mo-based materials as electrode materials for various MIBs(including lithium-ion batteries(LIBs),sodium-ion batteries(SIBs)and zinc-ion batteries(ZIBs))are discussed in ***,the modulation strategies for enhancing the electrochemical performance of 2D Mo-based materials are highlighted,focusing on heteroatom doping,vacancies creation,composite coupling engineering and nanostructure ***,we present the existing challenges and future research directions for 2D Mo-based materials to realize high-performance energy storage systems.

关键词： Molybdenum-based materials Two-dimensional materials Lithium-ion batteries Sodium-ion batteries Zinc-ion batteries

Facile intercalation of alkali ions in WO_(3)for modulated electronic and optical properties:Implications for artificial synapses and chromogenic application

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Science China(Physics,Mechanics & Astronomy) 2024年第2期67卷 149-160页

作者： Changmeng Huan Zihan Lu Silin Tang Yongqing Cai qingqing Ke School of Microelectronics Science and Technology Sun Yat-sen UniversityZhuhai 519082China Guangdong Provincial Key Laboratory of Optoelectronic Information Processing Chips and Systems Sun Yat-sen UniversityZhuhai 519082China Institute of Applied Physics and Materials Engineering University of MacaoTaipaMacao 999078China

Tungsten oxides(WO_(3))are widely recognized as multifunctional systems owing to the existence of rich *** diverse phases exhibit distinct octahedra-tilting patterns,generating substantial tunnels that are ideally suited for ***,a quantitative comprehension regarding the impact of distinct phases on the kinetics of intercalated conducting ions remains ***,we employ first-principles calculations to explore the spatial and orientational correlations of ion transport inγ-and h-WO_(3),shedding light on the relationship between diffusion barriers and the size of the conducting *** findings reveal that different types and concentrations of alkali-metals induce distinct and continuous lattice distortions in WO_(3)***,γ-WO_(3)is more appropriate to accommodate Li+ions,exhibiting a diffusion barrier and coefficient of 0.25 eV and 9.31×10^(-8)cm^(2)s^(-1),***,h-WO_(3)features unidirectional and sizeable tunnels that facilitate the transport of K+ions with an even lower barrier and a high coefficient of 0.11 e V and 2.12×10^(-5)cm^(2)s^(-1),***,the introduction of alkali-metal into WO_(3)tunnels tends to introduce n-type conductivity by contributing s-electrons to the unoccupied W 5d states,resulting in enhanced conductivity and tunable electronic *** alkali metals in WO_(3)tunnels are prone to charge transfer,forming small polaronic states and modulating the light absorption in the visible and nearinfrared *** tunable electronic and optical properties,combined with the high diffusion coefficient,underscore the potential of WO_(3)in applications such as artificial synapses and chromogenic devices.

关键词： WO_(3)polymorphs ion insertion kinetic activity tunable electronic and optical properties iontronics

Indium-based electrocatalysts for CO_(2) reduction to C1 products

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Chinese Chemical Letters 2024年第6期35卷 134-145页

作者： Qin Cheng Ming Huang qingqing Ye Bangwei Deng Fan Dong Research Center for Carbon-Neutral Environmental&Energy Technology Institute of Fundamental and Frontier SciencesUniversity of Electronic Science and Technology of ChinaChengdu 611731China Yangtze Delta Region Institute(Huzhou)&Institute of Fundamental and Frontier Sciences University of Electronic Science and Technology of ChinaHuzhou 313000China Suzhou Industrial Technology Research Institute of Zhejiang University Suzhou 215163China

Electrocatalytic CO_(2) reduction at mild conditions is a promising strategy to transform greenhouse gases into fuels or value-added chemicals to solve the increasingly serious environmental and energy *** most crucial factor in determining the CO_(2) reduction performance is to develop efficient electrocatalysts with high selectivity and *** the various electrocatalysts,indium-based catalysts have attracted extensive attention due to their non-toxicity,low cost,and high formic acid/formate *** this work,we comprehensively review the recent development and research progress of indium-based electrocatalysts for CO_(2)*** reaction mechanism,reaction pathways,structure-activity relationship,and strategies to enhance the activity of CO_(2)RR on indium-based catalysts have also been briefly presented and ***,the existing challenges and future developments for indium-based highperformance catalysts for CO_(2)RR are proposed.

关键词： Electrocatalytic CO_(2) reduction In-based catalysts Formate Reaction mechanism Structure-activity relationship

Cross-linkedα-amylase aggregates on Fe3O4 magnetic nanoparticles modified with polydopamine/polyethyleneimine for efficient hydrolysis of starch

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Particuology 2024年第7期90卷 98-105页

作者： Jiandong Cui Xiuming Tang qingqing Ma Yuyan Chang Qunli Zhang Shiru Jia State Key Laboratory of Food Nutrition and Safety Laboratory of Industrial Fermentation MicrobiologyMinistry of EducationTianjin University of Science and TechnologyTianjin 300457China Key Laboratory of Biomass Chemical Engineering of Ministry of Education Zhejiang UniversityHangzhou 310027China

In this workα-amylase was immobilized on magnetic Fe3O4 nanoparticles with polyethylenimine(PEI)/polydopamine(PDA)coating or 3-aminopropyl triethoxysilane(APTES)for the first time via adsorption–precipitation–*** with the freeα-amylase,the resultant magnetic cross-linkedα-amylase aggregates(PEI/PDA-M-CLEAs and N-M-CLEAs)exhibited excellent thermal and storage stability as well as pH *** storage at 25°C for 60 days,freeα-amylase only retained 60%of its initial activity,while PEI/PDA-M-CLEAs and N-M-CLEAs retained 80%and 78%of their initial activities,***,N-M-CLEAs and PEI/PDA-M-CLEAs showed good *** 6 repeated uses,PEI/PDA-M-CLEAs and N-M-CLEAs still maintained 65%and 62%of their initial activities,***,PEI/PDA-M-CLEAs and N-M-CLEAs exhibited higher starch hydrolysis efficiency than freeα-*** maximum dextrose equivalent(DE)values of starch hydrolysis by PEI/PDA-M-CLEAs and N-M-CLEAs reached 29.24%and 28.79%within 90 min,***,the maximum DE values of starch hydrolysis by the freeα-amylase was only 27.89%even in 150 *** magnetic cross-linkedα-amylase aggregates could be introduced as effective biocatalyst for industrial applications in production of maltose syrups.

关键词： α-amylase Magnetic nanoparticles Functional modification Magnetic cross-linked enzyme aggregates Hydrolysis of starch