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Acceptor-engineering tailored type-Ⅰ photosensitizer with aggregation-induced NIR-II emission for cancer multimodal phototheranostics

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Science China Chemistry 2024年第8期67卷 2647-2660页

作者： Jiangao Li niu niu Deliang Wang Xue Liu Yi Qin Lei Wang Ben Zhong Tang Dong Wang Center for AIE Research Shenzhen Key Laboratory of Polymer Science and TechnologyGuangdong Research Center for Interfacial Engineering of Functional MaterialsCollege of Materials Science and EngineeringShenzhen UniversityShenzhen 518060China guangzhou Municipal and guangdong Provincial Key Laboratory of Molecular Target Clinical Pharmacologythe State Key Laboratory of Respiratory DiseaseSchool of Pharmaceutical Sciences and the Fifth Affiliated HospitalGuangzhou Medical UniversityGuangzhou 511436China School of Science and Engineering Shenzhen Institute of Aggregate Science and TechnologyThe Chinese University of Hong KongShenzhen(CUHK-Shenzhen)Shenzhen 518172China

Exploration of single molecular species synchronously featured by long excitation/emission wavelength, accurate diagnosis, and effective therapy, remains supremely appealing to implement high-performance cancer phototheranostics. However, those previously established phototheranostic agents are undiversified and stereotyped in terms of structural skeleton, and generally exhibit insufficient phototheranostic outcomes. Herein, we innovatively utilized indanone-condensed thiadiazolo[3,4-g]quinoxaline(ITQ) as electron acceptor to construct novel photosensitizer with second near-infrared(NIR-II) emission. Experimental study and theoretical calculation demonstrated that comparing with the counterparts constituting by widely employed NIR-II building block benzobisthiadiazole(BBTD) and 6,7-diphenylthiadiazoloquinoxaline(DPTQ), ITQ-based photosensitizer(TITQ) showed superior aggregation-induced emission(AIE) characteristics, much stronger type-I reactive oxygen species(ROS) production, and prominent photothermal conversion capacity. Furthermore, TITQ nanoparticles with excellent biocompatibility were capable of effectively accumulating in the tumor site and visualizing tumor through fluorescence-photoacoustic-photothermal trimodal imaging with highly spatiotemporal resolution, and completely eliminating tumor by type-I photodynamic-photothermal therapy.

关键词： phototheranostics aggregation-induced emission NIR-Ⅱfluorescence acceptor engineering photodynamic-photothermal therapy

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A Study on the Impact of Chemical Structure on the Evolution of Aggregate Structure in Fiber-shaped High Density Polyethylene Vitrimer

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Chinese Journal of Polymer Science 2024年第10期42卷 1557-1565,I0013页

作者： Bing Wang Yuan-Chu gao Hai Wang Hui niu State Key Laboratory of Fine Chemicals School of Chemical EngineeringDalian University of TechnologyDalian116024China

Vitrimers have emerged as a prominent research area in the field of polymer *** of the studies have focused on synthesizing polymers with versatile dynamic crosslinking structures,while the impact of chemical structure on aggregate structure of vitrimers,particularly during polymer processing,remains insufficiently *** present study employed commercial maleic anhydride-grafted-high density polyethylene(M-g-HDPE)as the matrix and hexanediol as the crosslinker to facilely obtain fiber-shaped HDPE vitrimers through a reaction extrusion and post-drawing *** chemical structure characterization,morphology observation,thermal and mechanical properties investigation,as well as aggregate structure analysis,this work revealed the influence of dynamic bonds on the formation of aggregate structures during fiber-shaped vitrimers processing.A small amount of dynamic bonds in HDPE restricts the motion of PE chain during melt-extruding and post-drawing,resulting in a lower orientation of the PE ***,lamellar growth and fibril formation during post-drawing at high temperature are enhanced to some extent due to the competition between dynamic bond and chain *** uneven morphology of fibershaped HDPE vitrimers can be attributed to the stronger elastic effect brought by dynamic bonding,which plays a more dominant role in determining the mechanical properties of fiber-shaped vitrimers compared to aggregate *** Vitrimers have emerged as a prominent research area in the field of polymer *** of the studies have focused on synthesizing polymers with versatile dynamic crosslinking structures,while the impact of chemical structure on aggregate structure of vitrimers,particularly during polymer processing,remains insufficiently *** present study employed commercial maleic anhydride-grafted-high density polyethylene(M-g-HDPE)as the matrix and hexanediol as the crosslinker to facilely obtain fiber-shap

关键词： High density polyethylene vitrimer Fiber-shaped Aggregate structures Transesterification reaction

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A unified pre-training and adaptation framework for combinatorial optimization on graphs

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Science China Mathematics 2024年第6期67卷 1439-1456页

作者： Ruibin Zeng Minglong Lei Lingfeng niu Lan Cheng School of Computer Science and Technology University of Chinese Academy of SciencesBeijing100049China Faculty of Information Technology Beijing University of TechnologyBeijing100124China School of Economics and Management University of Chinese Academy of SciencesBeijing100190China School of Mathematics and Statistics Central South UniversityChangsha410075China

Combinatorial optimization(CO)on graphs is a classic topic that has been extensively studied across many scientific and industrial ***,solving CO problems on graphs through learning methods has attracted great *** deep learning methods,e.g.,graph neural networks(gNNs),have been used to effectively assist the process of solving ***,current frameworks based on gNNs are mainly designed for certain CO problems,thereby failing to consider their transferable and generalizable abilities among different COs on ***,simply using original graphs to model COs only captures the direct correlations among objects,which does not consider the mathematical logicality and properties of *** this paper,we propose a unified pre-training and adaptation framework for COs on graphs with the help of the maximum satisfiability(Max-SAT)*** first use Max-SAT to bridge different COs on graphs since they can be converted to Max-SAT problems represented by standard formulas and clauses with logical *** we further design a pre-training and domain adaptation framework to extract the transferable and generalizable features so that different COs can benefit from *** the pre-training stage,Max-SAT instances are generated to initialize the parameters of the *** the fine-tuning stage,instances from CO and Max-SAT problems are used for adaptation so that the transferable ability can be further *** experiments on several datasets show that features extracted by our framework exhibit superior transferability and Max-SAT can boost the ability to solve COs on graphs.

关键词： combinatorial optimization graph neural networks domain adaptation maximum satisfiability problem

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Diatomic fe-Co catalysts synergistically catalyze oxygen evolution reaction

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Nano Research 2024年第5期17卷 3794-3800页

作者： Tianmi Tang Jingyi Han Zhenlu Wang Xiaodi niu Jingqi guan Institute of Physical Chemistry College of ChemistryJilin UniversityChangchun 130021China College of Food Science and Engineering Jilin UniversityChangchun 130062China

The design of diatomic catalysts with uniformly dispersed metal atoms is expected to improve catalytic performance,which is conducive to the intensive comprehending of the synergistic mechanism between dual-metal sites for the oxygen evolution reaction(OER)at the atomic ***,we design a strategy to immobilize bimetallic fe-Co atoms onto nitrogen-doped graphene to obtain a diatomic catalyst(DA-FC-Ng)with feN_(3)-CoN_(3) *** DA-FC-Ng shows excellent OER activity with a low overpotential(η_(10)=268 mV),which is superior to commercial iridium dioxide *** calculations uncover that the excellent activity of DA-FC-Ng is due to the interaction between fe and Co diatoms,which causes charge rearrangement and induces the adsorption of intermediates on the fe-O-Co bridge structure,thus improving the catalytic OER *** work is of great significance for the design of highly active diatomic catalysts to replace noble metal catalysts for energy-related applications.

关键词： oxygen evolution reaction diatomic catalyst feN_(3)-CoN_(3) X-ray absorption spectroscopy(XAS)spectrum theoretical calculation

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Charge-asymmetry fe_(1)Cu single-atom alloy catalyst for efficient oxygen reduction reaction

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Nano Research 2024年第6期17卷 4702-4710页

作者： Xudong niu Jian Wei Dongyao Xu Jiajing Pei Rui Sui School of Chemical&Environmental Engineering China University of Mining and TechnologyBeijing 100083China Institute of Water Ecology and Environment Chinese Research Academy of Environmental SciencesBeijing 100083China Beijing Synchrotron Radiation Facility Institute of High Energy PhysicsChinese Academy of SciencesBeijing 100049China Engineering Research Center of Advanced Rare Earth Materials Department of ChemistryTsinghua UniversityBeijing 100084China

The development of high-efficient and low-cost oxygen reduction reaction(ORR)electrocatalysts is crucial for the practical applications of metal-air *** promising way is to develop fe single-atom ***,the single active center and inherent electronic structure of fe single-atom catalysts lead to the undesirable adsorption of multiple ORR ***,a charge-asymmetry single-atom alloy(SAA)catalyst with fe-Cu dual sites supported on nitrogen-doped carbon nanosheet(fe_(1)Cu SAA/NC)was *** characterizations manifest the existence of electron interaction between fe and Cu in fe_(1)Cu SAA/NC,which facilitates the adsorption of ORR intermediate for fast ***,the charge-asymmetry fe_(1)Cu SAA/NC exhibits much faster ORR kinetics with a half-wave potential of 0.917 V *** hydrogen electrode(RHE),outperforming its counterparts in the ***,fe_(1)Cu SAA/NC still maintains a high half-wave potential with only a drop of 5 mV after 5000 cycles,indicating excellent *** work provides a new strategy to design highly active and non-noble metal ORR electrocatalysts,which hold great potential for various catalytic applications.

关键词： fe_(1)Cu single-atom alloy(SAA) electrocatalysis oxygen reduction reaction charge-asymmetry

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On traceable iterated line graph and hamiltonian path index

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Applied Mathematics(A Journal of Chinese Universities) 2024年第2期39卷 239-252页

作者： niu Zhao-hong XIONg Li-ming YANg Wei-hua School of Mathematical Sciences Shanxi UniversityTaiyuan 030006China School of Mathematics and Statistics Beijing Key Laboratory on MCAACIBeijing Institute of TechnologyBeijing 100081China Department of Mathematics Taiyuan University of TechnologyTaiyuan 030024China

Xiong and Liu[21]gave a characterization of the graphs g for which the n-iterated line graph L^(n)(g)is hamiltonian,for n≥*** this paper,we study the existence of a hamiltonian path in L^(n)(g),and give a characterization of g for which L^(n)(g)has a hamiltonian *** applications,we use this characterization to give several upper bounds on the hamiltonian path index of a graph.

关键词： iterated line graph traceable hamiltonian index hamiltonian path index

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An advanced 2D/3D g-C_(3)N_(4)/TiO_(2)@MnO_(2) multifunctional membrane for sunlight-driven sustainable water purification

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Nano Research 2024年第4期17卷 2368-2380页

作者： Fan Yu Chunjia Luo Xiaohan niu Min Chao Pengfei Zhang Luke Yan Polymer Materials&Engineering Department School of Materials Science&EngineeringChang’an UniversityXi’an 710064China Key Laboratory of Road Construction Technology and Equipment MOEChang’an UniversityXi’an 710064China School of Textile Science and Engineering Xi’an Polytechnic UniversityXi’an 710064China

graphitic carbon nitride(g-C_(3)N_(4))nanosheets have attracted widespread interest in the construction of advanced separation ***,dense stacking and a single functionality have limited the membrane ***,an advanced two-/three-dimensional(2D/3D)g-C_(3)N_(4)/TiO_(2)@MnO_(2) membrane is constructed by intercalating 3D TiO_(2)@MnO_(2) nanostructures into g-C_(3)N_(4) *** 3D flower-like nanostructures broaden the transport channels of the composite *** membrane can effectively separate five oil-in-water(O/W)emulsions,with a maximum flux of 3265.67±15.01 L·m^(-2)·h^(-1)·bar^(-1) and a maximum efficiency of 99.69%±0.45%for toluene-in-water emulsion(T/W).Meanwhile,the TiO_(2)@MnO_(2) acts as an excellent electron acceptor and provides positive spatial separation of electrons–holes(e^(-)–h^(+)).The formation of 2D/3D heterojunctions allows the material with wider light absorption and smaller bandgap(2.10 eV).These photoelectric properties give the membrane good degradation of three different pollutants,with about 100%degradation for methylene blue(MB)and malachite green(Mg).The photocatalytic antibacterial efficiency of the membrane is also about 100%.After cyclic experiment,the membrane maintains its original separation and photocatalytic *** remarkable multifunctional and self-cleaning properties of the g-C_(3)N_(4) based membrane represent its potential value for complex wastewater treatment.

关键词： graphitic carbon nitride(g-C_(3)N_(4))based membrane three-dimensional(3D)nanostructures self-cleaning multifunction

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Polyoxometalates coupled covalent organic frameworks as highly active photothermal nanoreactor for CO_(2)cycloaddition

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Nano Research 2024年第7期17卷 5975-5984页

作者： Tian Wang Yunqing Zhu Wei Wang Junfeng niu Zhiyi Lu Peilei He School of Environmental Science and Engineering Shaanxi University of Science and TechnologyXi’an 710021China Key Laboratory of Advanced Fuel Cells and Electrolyzers Technology of Zhejiang Province Ningbo Institute of Materials Technology and EngineeringChinese Academy of SciencesNingbo 315201China College of Environmental Science and Engineering North China Electric Power UniversityBeijing 102206China University of Chinese Academy of Sciences Beijing 100049China

Covalent organic frameworks(COFs)-based nanoreactors have attracted broad interest in many fields due to their voidconfinement ***,the inherent drawback of conventional nanoreactors is the lack of internal active sites,which limits their widespread ***,we report the construction of hierarchical COF(EB-TFP)nanoreactor with pre-synthesized polyoxometalates(POM,[PV_(2)W_(10)O_(40)]^(5–)(PV_(2)W_(10)))clusters encapsulated inside of COF(POM@COF).PV_(2)W_(10)@EB-TFP anchors nucleophilic-group(Br–ions)and PV_(2)W_(10)anion cluster within the COF framework via electrostatic interactions,which not only simplifies the reaction system but also enhances catalytic *** reaction performance of the PV_(2)W_(10)@EB-TFP nanoreactor can be tuned to achieve excellent catalytic activity in CO_(2)cycloaddition reaction(CCR)for~97.63%conversion and~100%selectivity under visible light irradiation.A mechanistic study based on density functional theory(DFT)calculations and insitu characterization was also carried *** summary,we have reported a method for achieving the uniform dispersion of POM single clusters into COF nanoreactor,demonstrating the potential of POM@COF nanoreactor for synergistic photothermal catalytic CO_(2)cycloaddition.

关键词： photothermal nanoreactor CO_(2)cycloaddition polyoxometalate photothermal-synergistic catalysis covalent organic frameworks

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Time-dependent deviation of bridge pile foundations caused by adjacent large-area surcharge loads in soft soils and its preventive measures

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Frontiers of Structural and Civil Engineering 2024年第2期18卷 184-201页

作者： Shuanglong LI Limin WEI Jingtai niu Zhiping DENg Bangbin WU Wuwen QIAN feifei HE School of Hydraulic Engineering Nanchang Institute of TechnologyNanchang 330099China School of Civil Engineering Central South UniversityChangsha 410075China

Time-dependent characteristics(TDCs)have been neglected in most previous studies investigating the deviation mechanisms of bridge pile foundations and evaluating the effectiveness of preventive *** this study,the stress-strain-time characteristics of soft soils were illustrated by consolidation-creep tests based on a typical engineering *** extended Koppejan model was developed and then embedded in a finite element(fe)model via a user-material subroutine(UMAT).Based on the validated fe model,the time-dependent deformation mechanism of the pile foundation was revealed,and the preventive effect of applying micropiles and stress-release holes to control the deviation was *** results show that the calculated maximum lateral displacement of the cap differs from the measured one by 6.5%,indicating that the derived extended Koppejan model reproduced the deviation process of the bridge cap-pile foundation with *** additional load acting on the pile side caused by soil lateral deformation was mainly concentrated within the soft soil layer and increased with the increase in load *** with t=3 d(where t is surcharge time),the maximum lateral additional pressure acting on Pile 2#increased by approximately 47.0%at t=224 *** bridge pile foundation deviation in deep soft soils,stress-release holes can provide better prevention compared to micropiles and are therefore recommended.

关键词： bridge pile foundation surcharge load soft soil time-dependent deformation interaction mechanism preventive measure

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Microstructural Evolutions and Mechanical Properties of Energetic Al_(1) (TiZrNbTaMoCr)_(15) High-Entropy Alloys

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Acta Metallurgica Sinica(English Letters) 2024年第4期37卷 620-632页

作者： Xuan-Hong Cai Zhen-Hua Wang Ben niu Jin-feng Li Qing Wang Show authors Key Laboratory of Materials Modification By Laser Ion and Electron Beams(Ministry of Education)Engineering Research Center of High Entropy Alloy Materials(Liaoning Province)School of Materials Science and EngineeringDalian University of TechnologyDalian116024China Institute of Materials China Academy of Engineering PhysicsMianyang621908China

The present study focuses on investigating the microstructural evolutions and mechanical properties of energetic Al_(1)(TiZrNbTaMoCr)_(15) refractory high-entropy alloys with the different heat treatments at low Al content state. It is found that even with a reduction in the Al content, the strength of these alloys remains unaffected at room temperature and high temperature, while the plasticity improves significantly. In particular, the coherent BCC/B_(2) microstructure with needle-like B_(2) nanoprecipitates dispersed into the BCC matrix is formed in 873 K-aged Al_(1)Ti_(6)Zr_(2)Nb_(3)Ta_(3)Mo_(0.5)Cr_(0.5) alloy. Therefore, this alloy exhibits the highest compression yield strength (σ_(YS) = 1333 and 717 MPa) at room temperature and 1073 K, respectively. After 973 K-aged, the coherent BCC/B_(2) microstructure underwent destabilization, and the B_(2) phase transforms into the brittle Zr5Al3 phase which then coarsens and dominates the microstructure of S3-AlTa_(3) alloy after 1073 K-aged. Moreover, these current alloys exhibit exceptionally high theoretical exothermic enthalpy (ΔH), surpassing 11606 J·g^(−1), which highlights their significant potential as innovative high-performance energetic structural materials.

关键词： Refractory high-entropy alloy Coherent microstructure Mechanical property Exothermic enthalpy

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