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Nano Research 2024年第3期17卷 1818-1826页

作者： Kun Chen Shengqiu Liu Yujun Wei South China Advanced Institute for soft matter Science and Technology School of Emergent Soft MatterSouth China University of TechnologyGuangzhou 510641China Guangdong Provincial key laboratory of Technique and Equipment for Macromolecular Advanced Manufacturing South China University of TechnologyGuangzhou 510641China Guangdong Provincial key laboratory of Functional and Intelligent Hybrid Materials and Devices South China University of TechnologyGuangzhou 510641China

Obesity is closely related with insulin resistance and chronic inflammation.Here,we report that unsaturated lipid-modified polyoxovanadates(ULPOVs)can restrict weight gain of diet-induced obese mice and improve their glycemic control and obesity-associated inflammation.Oral administration of the sub-nanosized ULPOVs at a low dosage for 7 weeks reduces the body weight and almost normalizes the blood glucose levels of obese mice fed on a high-fat diet.ULPOV treatment increases the activity of the nuclear receptor peroxisome proliferator-activated receptorγ(PPARγ)and reduces intestinal caloric intake,which may be the main reason for blood sugar and body weight control.In addition to insulin-sensitizing,PPARγactivation induced by ULPOV treatment in obese mice with atopic dermatitis(AD)promotes the type 2 T helper(TH_(2))cell selective responses and therapeutic effects on immune dysregulation caused by obesity.These data suggest sub-nanosized polyoxovanadate clusters as a class of potential candidates to relieve symptoms accompanied by diet-induced obesity.

关键词： polyoxovanadates lipid modification glucose homeostasis obesity inflammatory disease peroxisome proliferator-activated receptorγ(PPARγ)

Highly elastic and degradable vitrimeric elastomers using polycondensation

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Chinese Chemical Letters 2024年第3期35卷 434-438页

作者： Yue Liu Yongshuang Huang Chao Li Guifu Si Min Chen Institutes of Physical Science and Information Technology Key Laboratory of Structure and Functional Regulation of Hybrid Materials of Ministry of EducationAnhui UniversityHefei 230601China CAS key laboratory of soft matter chemistry Department of Polymer Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China

Introducing covalently crosslinked network to polymer matrix can merge the advantages in reprocessing and durability of polymers.In this contribution,a series of high-performance vitrimeric elastomers were achieved via polycondensation.The topological structures of polymers were tuned by varying the feeding ratios of bisacetoacetate,hex–substituted bisacetoacetate,bisamine and tris(2-aminoethyl)amine.With these structural manipulations,the vitrimeric elastomers presented great elastic recovery properties(strain recovery value up to 80%)benefiting from the introduction of long chain branch.Furthermore,the elastomers exhibited excellent reprocessing property,water vapor/oxygen barrier and adhesive properties.Specially,the elastomers could be degraded into monomer under acid conditions which enabled the elastomer synthesis again in closed loop recycling system.The ease of the polycondensation in this work to prepare highly elastic and recyclable vitrimeric elastomers demonstrated exciting opportunities for the synthesis of sustainable polymers.

关键词： Polycondensation Vitrimeric elastomers Highly elastic Degradable polymers

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

Merging non-covalent and covalent crosslinking:En route to single chain nanoparticles

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Chinese Chemical Letters 2024年第6期35卷 307-311页

作者： Yifei Zhang Yuncong Xue Laiwei Gao Rui Liao Feng Wang Fei Wang CAS key laboratory of soft matter chemistry Department of Polymer Science and EngineeringUniversity of Science and Technology of ChinaHefei 230026China Department of Neurosurgical The First Affiliated Hospital of University of Science and Technology of ChinaDivision of Life Sciences and MedicineHefei 230026China

Single-chain nanoparticles represent an emerging class of nanomaterials designed to mimic protein's folding paradigm.Intrachain covalent crosslinking toward the formation of single-chain nanoparticles encounters complex energy landscapes,leading to the potential occurrence of misfolding issues.While noncovalent crosslinking can circumvent this issue,the resulting single-chain nanoparticles exhibit lower structural stability compared to their covalently crosslinked counterparts.In this study,we present a novel approach for the synthesis of single-chain nanoparticles,achieved through the combination of non-covalent and covalent intramolecular crosslinking.Cyanostilbenes grafted onto the linear polymer form intrachain non-covalent stacks aided by hydrogen bonds,leading to the formation of non-covalently crosslinked single-chain nanoparticles.These nanoparticles undergo conversion to covalently crosslinked nanostructures through subsequent photo-irradiation using[2+2]photocycloaddition,a process facilitated by the supramolecular confinement effect.Consequently,the resulting single-chain nanoparticles demonstrate both intrachain folding efficiency and substantial stability,offering significant potential for advancing applications across diverse fields.

关键词： Single chain nanoparticles Intrachain folding Supramolecular confinement Cyanostilbenes [2+2]photocycloaddition

Deciphering the high-carbonization-temperature triggered enzymatic activity of wool-derived N,S-co-doped carbon nanosheets

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Chinese Chemical Letters 2024年第3期35卷 182-188页

作者： Jiachen Zhao Deshuai Yu Jianmin Chen Shihao Lin Yonghua Tang Chaoyu Fan Dongfang Zhou Youhui Lin Department of Physics Research Institute for Biomimetics and Soft MatterFujian Provincial Key Laboratory for Soft Functional Materials ResearchXiamen UniversityXiamen 361005China School of Pharmacy and Medical Technology Putian UniversityPutian 351100China key laboratory of Mental Health of the Ministry of Education NMPA Key Laboratory for Research and Evaluation of Drug Metabolism&Guangdong Provincial Key Laboratory of New Drug ScreeningSchool of Pharmaceutical SciencesSouthern Medical UniversityGuangzhou 510515China key laboratory of Pharmaceutical Analysis and laboratory Medicine(Putian University) Fujian Province UniversityPutian 351100China

It is well-established that high carbonization temperature will trigger the enzyme-like activity of carbon-based materials.However,the catalytic mechanism is still ambiguous,which hinders the further rational design of nanomaterials as enzyme mimics.Hereby,N,S-rich carbonized wool nanosheets(CWs)were synthesized at different pyrolysis temperatures.As expected,only CWs treated with high-temperature possess intrinsic oxidase-and peroxidase-like activities.Meanwhile,density functional theory(DFT)calculations demonstrate that graphitic nitrogen and the co-existence of nitrogen and sulfur in the carbon matrix serve as the active sites for the enzyme-like process.More importantly,combining theoretical calculations and experimental observations,the high-temperature triggered catalytic mechanism can be ascribed to the fact that an appropriate high-temperature maximizes the graphitization degree to a certain extent,at which most of the catalytic active sites are well retained rather than evaporating.Moreover,coupling with excellent photothermal conversion efficiency and catalytic performance,CWs can be applied to photothermal-catalytic cancer therapy under near-infrared region(NIR)light irradiation.We believe this work will contribute to understanding the catalytic mechanism of carbon-based nanozymes and promote the development of new biomedical and pharmaceutical applications.

关键词： Carbon-based nanozyme Catalytic mechanism Density functional theory High-temperature carbonization

Matrix-Mediated Color-Tunable Ultralong Organic Room Temperature Phosphorescence of 7H-Benzo[c]carbazole Derivatives

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CCS chemistry 2024年第3期6卷 798-811页

作者： Chen Qian Xue Zhang Zhimin Ma Xiaohua Fu Zewei Li Huiwen Jin Mingxing Chen Hong Jiang Zhiyong Ma Beijing Advanced Innovation Center for soft matter Science and Engineering State Key Laboratory of Organic–Inorganic CompositesCollege of Chemical EngineeringBeijing University of Chemical TechnologyBeijing 100029 Beijing National laboratory for Molecular Sciences College of Chemistry and Molecular EngineeringPeking UniversityBeijing 100871

Building on the recent systematic research on 1Hbenzo[f]indole(Bd),an important advancement in constructing ultralong organic room temperature(UORTP)materials with a universal strategy via a readily obtained unit(7H-Benzo[c]carbazole,BCz)is proposed in this work.Pure powders of BCz and its derivatives merely exhibit blue fluorescence at ambient condition.However,when BCz and its derivatives are dispersed into polymer or powder matrixes,strong photo-activated green UORTP can be observed from their doped systems at room temperature.Moreover,the UORTP color can be tuned between green and yellow depending on the matrix.The ultralong phosphorescence originates from the generation of charge-separated states via radicals.The matrixes play a key role in both stabilizing charge-separated states and controlling UORTP color.More interestingly,when using polymethyl methacrylate as matrix,the doped films achieve stronger photo-activated ultralong phosphorescence underwater than in air at room temperature.Comparedwith Bd,BCz achieves better performance not only in ultralong phosphorescence properties but also in practical applications.This work gains a deeper insight into the mechanism of UORTP and paves a new approach to applying organic phosphorescent materials to underwater coating and imaging.

关键词： 7H-Benzo[c]carbazole ultralong organic room temperature phosphorescence ion radical matrix-mediated color tunning underwater application

Current Status and Perspectives of Dual-Atom Catalysts Towards Sustainable Energy Utilization

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Nano-Micro Letters 2024年第7期16卷 402-440页

作者： Yizhe Li Yajie Li Hao Sun Liyao Gao Xiangrong Jin Yaping Li Zhi LV Lijun Xu Wen Liu Xiaoming Sun State key laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science EngineeringCollege of ChemistryBeijing University of Chemical TechnologyBeijing 100029People’s Republic of China Xinjiang Coal Mine Mechanical and Electrical Engineering Technology Research Center Xinjiang Institute of EngineeringUrumqi 830023Xinjiang Uygur Autonomous RegionPeople’s Republic of China

The exploration of sustainable energy utilization requires the imple-mentation of advanced electrochemical devices for efficient energy conversion and storage,which are enabled by the usage of cost-effective,high-performance electro-catalysts.Currently,heterogeneous atomically dispersed catalysts are considered as potential candidates for a wide range of applications.Compared to conventional cata-lysts,atomically dispersed metal atoms in carbon-based catalysts have more unsatu-rated coordination sites,quantum size effect,and strong metal-support interactions,resulting in exceptional catalytic activity.Of these,dual-atomic catalysts(DACs)have attracted extensive attention due to the additional synergistic effect between two adja-cent metal atoms.DACs have the advantages of full active site exposure,high selectiv-ity,theoretical 100%atom utilization,and the ability to break the scaling relationship of adsorption free energy on active sites.In this review,we summarize recent research advancement of DACs,which includes(1)the comprehensive understanding of the synergy between atomic pairs;(2)the synthesis of DACs;(3)characterization meth-ods,especially aberration-corrected scanning transmission electron microscopy and synchrotron spectroscopy;and(4)electrochemical energy-related applications.The last part focuses on great potential for the electrochemical catalysis of energy-related small molecules,such as oxygen reduction reaction,CO_(2) reduction reaction,hydrogen evolution reaction,and N_(2) reduction reaction.The future research challenges and opportunities are also raised in prospective section.

关键词： Dual-atom catalysts Synergetic effect Electrocatalysis Oxygen reduction reaction CO_(2)reduction reaction Hydrogen evolution reaction N2 reduction reaction

Numerical Investigation on Heat Transfer Characteristics of Microencapsulated Phase Change Material Slurry in a Rectangular Minichannel

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Journal of Thermal Science 2024年第2期33卷 564-577页

作者： WANG Zhibin LI Zilong JIA Lisi DING Bin CHEN Ying School of Materials and Energy Guangdong University of TechnologyGuangzhou510006China Guangdong Provincial key laboratory of Functional soft Condensed matter Guangzhou510006China College of New Energy China University of Petroleum(East China)Qingdao266580China

Microencapsulation phase change material slurry(MEPCMS) becomes a potential working fluid for cooling high energy density miniaturized components,thanks to the latent heat absorption of particles in the heat transfer process.In this work,the Discrete Phase Model(DPM) based on the Euler-Lagrangian method is used to numerically investigate the convective heat transfer characteristics of MEPCMS flowing through a rectangular minichannel with constant heat flux.The results show that particles of MEPCMS are mainly subjected to drag force during the flow.Even so,they can migrate from the high-temperature region to the low-temperature region driven by the thermophoretic force,affecting the particle distribution and phase change process.Moreover,the Nux of the MEPCMS fluctuates due to particle phase change with varying specific heat capacities.Specifically,the value increases first,then decreases,and eventually increases again until it approaches the fully developed value of the pure base fluid as the particles gradually melt.Furthermore,the heat transfer performance of the MEPCMS is influenced by the combination of fluid inlet temperature fluid inlet velocity(v),and mass concentration(c_(m)) of MEPCM particles.The result shows that the maximum reduction of the maximum bottom wall temperature difference(ΔT_(w)) is 23.98% at T_(in)=293.15 K,v=0.15 m·s^(-1),c_(m)=10%.

关键词： Microencapsulated Phase Change Material Slurry(MPCMS) Discrete Phase Model(DPM) particle-fluid interaction force minichannel heat sink thermophoresis

Atomically dispersed Fe sites on hierarchically porous carbon nanoplates for oxygen reduction reaction

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Journal of Energy chemistry 2024年第3期90卷 7-15,I0002页

作者： Ruixue Zheng Qinglei Meng Hao Zhang Teng Li Di Yang Li Zhang Xiaolong Jia Changpeng Liu Jianbing Zhu Xiaozheng Duan Meiling Xiao Wei Xing State key laboratory of Electroanalytical chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina School of Applied chemistry and Engineering University of Science and Technology of ChinaHefei 230026AnhuiChina laboratory of Advanced Power Sources Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina Institute of Functional Nano&soft Materials(FUNSOM) Jiangsu Key Laboratory for Carbon-Based Functional Materials&DevicesJiangsu Key Laboratory of Advanced Negative Carbon TechnologiesSoochow UniversitySuzhou 215123JiangsuChina State key laboratory of Polymer Physics and chemistry Changchun Institute of Applied ChemistryChinese Academy of SciencesChangchun 130022JilinChina

Developing cost-effective,robust and stable non-precious metal catalysts for oxygen reduction reaction(ORR) is of paramount importance for electrochemical energy conversion devices such as fuel cells and metal-air batteries.Although Fe-N-C single atom catalysts(SACs) have been hailed as the most promising candidate due to the optimal binding strength of ORR intermediates on the Fe-N_(4) sites,they suffer from serious mass transport limitations as microporous templates/substrates,i.e.,zeolitic imidazolate frameworks(ZIFs),are usually employed to host the active sites.Motivated by this challenge,we herein develop a hydrogen-bonded organic framework(HOF)-assisted pyrolysis strategy to construct hierarchical micro/mesoporous carbon nanoplates for the deposition of atomically dispersed Fe-N_(4) sites.Such a design is accomplished by employing HOF nanoplates assembled from 2-aminoterephthalic acid(NH_(2)-BDC) and p-phenylenediamine(PDA) as both soft templates and C,N precursors.Benefitting from the structural merits inherited from HOF templates,the optimized catalyst(denoted as Fe-N-C SAC-950) displays outstanding ORR activity with a high half-wave potential of 0.895 V(vs.reversible hydrogen electrode(RHE)) and a small overpotential of 356 mV at 10 mA cm^(-2) for the oxygen evolution reaction(OER).More excitingly,its application potential is further verified by delivering superb rechargeability and cycling stability with a nearly unfading charge-discharge gap of 0.72 V after 160 h.Molecular dynamics(MD) simulations reveal that micro/mesoporous structure is conducive to the rapid mass transfer of O_(2),thus enhancing the ORR performance.In situ Raman results further indicate that the conversion of O_(2) to~*O_(2)-the rate-determining step(RDS) for Fe-N-C SAC-950.This work will provide a versatile strategy to construct single atom catalysts with desirable catalytic properties.

关键词： Fe single atom catalysts Oxygen reduction reaction Mesoporous structure Active sites Zinc-air battery

Analysis of Piezoelectric Semiconductor Structures Considering Both Physical and Geometric Nonlinearities

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Acta Mechanica Solida Sinica 2024年第1期37卷 72-81页

作者： Zhengguang Xiao Shuangpeng Li Chunli Zhang key laboratory of soft Machines and Smart Devices of Zhejiang Province Department of Engineering MechanicsZhejiang UniversityHangzhou 310027China Huanjiang laboratory Zhuji 311816China

Piezoelectric semiconductors(PSs),such as ZnO and GaN,known as the third-generation semiconductors,have promising applications in electronic and optoelectronic devices due to the coexistence and interaction of piezoelectricity and semiconductor properties.Theoretical modeling of PS structures under external loads,such as thermal and mechanical loads,plays a crucial role in the design of PS devices.In this work,we propose a nonlinear fully coupling theoretical model and investigate the multi-field coupling behaviors of PS structures and PN junctions under thermal and mechanical loads,considering physical and geometric nonlinearities.The electromechanical and semiconducting behaviors of a PS rod-like structure with flexural deformations under different combinations of temperature changes and mechanical loads are evaluated.The tuning effect of temperature changes and mechanical loads on multi-field coupling behaviors of PSs is revealed.The current–voltage characteristics of PS PN junctions are studied under different combinations of temperature changes and mechanical loads.The obtained results are helpful for the development of novel PS devices.

关键词： Piezoelectric semiconductor Nonlinearity Multi-field Coupling Tuning