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Precise immobilization of metal single atoms into a porphyrinic metal-organic framework for an efficient alkene hydrosilylation

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Nano Research 2024年第7期17卷 5914-5921页

作者： Chun-Ying Chen Qi-Jie Mo Fu-zhen li Hai-li Song li Zhang MOE Laboratory of Bioinorganic and Synthetic Chemistry Lehn Institute of Functional MaterialsSchool of ChemistrySun Yat-Sen UniversityGuangzhou 510006China

Alkene hydrosilylation is one of the most concise and atom-economical methods to synthesize organosilicon ***,we reported the precise immobilization of metal single atoms(M-SAs;M=Ru,Rh,Ir,Pd,Pt,and Au)into a porphyrinic metalorganic framework(MOF)of PCN-222(PCN=porous coordination network),and then applied the resultant MOF composites of M-SAs@PCN-222 to alkene *** solvent-free conditions,Pt-SAs@PCN-222 displayed an especially high catalytic efficiency with the turnover frequency up to 119 s−1 and the maximum turnover number of 906,250 at room *** and theoretical studies revealed that there existed strong interactions between Pt-SAs@PCN-222 and the substrates,which helped to condense the substrates in the cavities of the porous *** density functional theory calculations and molecular dynamics simulations disclosed that PCN-222 could transfer electrons to Pt-SAs to enhance the silane oxidative addition and drive the reaction to proceed smoothly via Chalk–Harrod pathway.

关键词： alkene hydrosilylation single atom catalysts metal-organic frameworks precision chemistry synergistic catalysis

NIR-IIb-triggered photodynamic therapy combined with chemotherapy platform based on rare-earth-doped nanoparticles

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Rare Metals 2024年第7期43卷 3220-3231页

作者： Zhuo Tu Yong Wan Juan Ge Chen-Chen li Tao liang zhen li College of Health Science and Engineering College of Chemistry and Chemical EngineeringHubei University

Photodynamic therapy（PDT）,with high spatiotemporal selectivity,minimal side effects and less drug resistance,has emerged as a promising approach for the treatment of ***,inadequate penetration depth and poor efficacy seriously restrict its practical *** address these challenges,we developed a combined therapy platform（RENP@C/D-FA） based on rare-earth-doped nanoparticles（RENPs） with a structure of NaErF4:Tm（0.5%）@NaYF4,on which photosensitizer Ce6（chlorin e6） and chemo-therapeutic drug（DOX）(doxorubicin) were loaded by encapsulating with an amphiphilic polymer distearoyl phosphatidylethanolamine-polyethylene glycol-folic acid（DSPE-PEG-FA）.RENPs with NaErF4as the matrix possess multiple excitation/emission peaks,enabling activation of PDT under near-infrared-Ⅱb（NIR-Ⅱb,1500-1700 nm） excitation and luminescence imaging in NIR-Ⅱb region by absorbing 808 nm near-infrared ***,DOX can be selectively released in the acidic microenvironment of *** from the tumor targeting capability of folic acid,this platform can successfully ablate tumor cells and inhibit tumor growth by combining PDT and *** innovative approach holds great promise as a powerful tool for cancer treatment,showing the potential to revolutionize PDT.

关键词： Photodynamic therapy Rare-earth-doped nanoparticles NIR-IIb Chemotherapy Combined therapy

Molecular Chaperone-Dependent Polymer Translocation through Nanopores: The Effects of Chaperone Concentration and Chaperone-Polymer Interaction

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Chinese Journal of Polymer Science 2024年第1期42卷 125-132,I0011页

作者： Chang-Sheng Zuo Kang Wang li-zhen Sun Ting-Ting Sun Department of Physics Zhejiang University of Science and TechnologyHangzhou 310023China Department of Applied Physics Zhejiang University of TechnologyHangzhou 310014China

The polymer translocation through a nanopore from a donor space(or named cis side) to a receiver space(trans side) in the chaperone-induced crowded environment has attracted increasing attention in recent years due to its significance in biological systems and technological applications. In this work, we mainly focus on the effects of chaperone concentration and chaperone-polymer interaction on the polymer translocation. By assuming the polymer translocation to be a quasi-equilibrium process, the free energy F of the polymer can be estimated by Rosenbluth-Rosenbluth method and then the translocation time τ can be calculated by Fokker-Plank equation based on the obtained free energy landscape. Our calculation results show that the translocation time can be controlled by independently tuning the chaperone concentration and chaperone-polymer interaction at the cis side or the trans side. There exists a critical chaperone-polymer attraction ε~*=-0.2 at which the volume exclusion and interaction effects of the chaperone can balance each other. Additionally, we also find that at large chaperone-polymer attraction, the translocation time is mainly governed by the diffusion coefficient of the polymer.

关键词： Polymer translocation Rosenbluth-Rosenbluth method Fokker-Plank equation Free energy landscapes

Biomimetic design of highly flexible metal oxide nanofibrous membranes with exceptional mechanical performance for superior phosphopeptide enrichment

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Nano Research 2024年第5期17卷 4270-4278页

作者： Xue Mao zhen-zhen li Dong-lian Hao Wei-Dong Han Gao-Peng li Yao-Yu Wang Kun Zhang School of Textile Science and Engineering Key Laboratory of Functional Textile Material and Product(Ministry of Education)Xi’an Polytechnic UniversityXi’an 710048China Key Laboratory of Magnetic Molecules&Magnetic Information Materials of the Ministry of Education School of Chemistry&Material ScienceShanxi Normal UniversityTaiyuan 030031China Department of Clinical Laboratory The Second Affiliated Hospital of Xi’an Jiaotong UniversityXi’an 710004China Shanghai iProteome Biotechnology Co. LtdShanghai 201210China College of Chemistry&Materials Science Northwest UniversityXi'an 710127China

Developing free-standing and mechanical robust membrane materials capable of superior enrichment of phosphopeptides for analyzing and identifying the specific phosphoproteome of cancer cells is significant in understanding the molecular mechanisms of cancer development and exploring new therapeutic approaches,but still a significant challenge in materials *** this end,we firstly constructed highly flexible ZrTiO_(4) nanofibrous membranes(NFMs)with excellent mechanical stability through a cost-effective and scalable electrospinning and subsequent calcination ***,to further increase the enrichment capacity of the phosphopeptide,the biomimetic TiO_(2)@ZrTiO_(4) NFMs with root hair or leaf like branch microstructure are developed by the hydrothermal post-synthetic modification of ZrTiO_(4) NFMs through growing unfurling TiO_(2) nanosheets onto the ZrTiO_(4) ***,remarkable flexibility and mechanical stability enable the resulting TiO_(2)@ZrTiO_(4) NFMs excellent practicability,while the biomimetic microstructure allows it outstanding enrichment ability of the phosphopeptide and identification ability of the specific phosphoproteins in the digest of cervical cancer ***,6770 phosphopeptides can be enriched by TiO_(2)@ZrTiO_(4) NFMs(2205 corresponding phosphoproteins can be identified),and the value is much higher than that of ZrTiO_(4) NFMs(6399 phosphopeptides and 2132 identified phosphoproteins)and commercial high-performance TiO_(2) particles(4525 phosphopeptides and 1811 identified phosphoproteins).These results demonstrate the super ability of TiO_(2)@ZrTiO_(4) NFMs in phosphopeptide enrichment and great potential for exploring the pathogenesis of cancer.

关键词： inorganic nanofibers flexible ceramic nanofibrous membranes biomimetic materials exceptional mechanical performance flexibility

Efficacy and safety of Nafamostat mesylate in patients with endstage renal failure

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World Journal of Clinical Cases 2024年第1期12卷 68-75页

作者： Kun liu zhen-Hua li Department of Critical Care Medicine The Third People's Hospital Of Hubei ProvinceWuhan 430030Hubei ProvinceChina Department of Critical Care Medicine General Hospital of The Yangtze River ShippingWuhan Brain HospitalWuhan 430015Hubei ProvinceChina

BACKGROUND Recent studies on dialysis anticoagulation therapy in patients with renal failure have shown that Nafamostat mesylate,a broad-spectrum potent serine protease inhibitor,has strong anticoagulation and anti-fiber *** To evaluate the efficacy and safety of Nafamostat mesylate in patients with end-stage renal *** Seventy-five patients with end-stage renal failure who received hemodialysis at our hospital between January 2020 and August 2021 were selected and divided into the observation group(Nafamostat mesylate for injection,n=33)and control group(heparin sodium injection,n=32).General patient data,indicators of clinical efficacy,dialyzer hemocoagulation parameters,coagulation function indices,and hemoglobin concentration and platelet count before and after treatment,and the occurrence of adverse reactions after treatment were compared between the two *** The two groups showed no significant differences in general patient data(P>0.05).The post-treatment effectiveness rate in the control group was lower than that in the observation group(P0.05),while the number of patients in grade 0 was lower in the control group,and the number of patients in grades II and III was higher in the control group(Plized ratio values in the control group were higher than those in the observation group,while the fibrinogen level in the control group was lower than that in the observation group(P0.05).The total number of post-treatment adverse reactions in the observation group was lower than that in the control group(P<0.05).CONCLUSION Treatment of patients showing end-stage renal failure with Nafamostat mesylate can s

关键词： End-stage renal failure Nafamostat mesylate Effectiveness Safety study Chronic kidney diseases

The mechanisms of enhanced thickness-dependent DC breakdown strength of EP/MWCNTs nanocomposites

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High Voltage 2024年第2期9卷 440-452页

作者： zhen li He Gao Longfei Zhang Shouming Wang Ji liu Shengtao li Key Laboratory of Engineering Dielectrics and Its Application Ministry of EducationHarbin University of Science and TechnologyHarbinChina State Key Laboratory of Electrical Insulation and Power Equipment Xi'an Jiaotong UniversityXi'anChina

Owing to advanced power electronic and electrical applications developing towards miniaturisation and integration,the thickness-dependent DC breakdown mechanism of epoxy/multiwall-carbon-nanotube nanocomposites is under *** results indicate that the breakdown strength of nanocomposites containing 0.05 wt%multiwall-carbon-nanotubes rises by~18%,and the breakdown strength falls exponentially with increasing *** clarify the microscopic mechanism,a simulation model of DC breakdown,including carriers transport and segmental dynamics,is developed,and the accordant simulation results with experimental results indicate that the thickness-dependent DC breakdown of epoxy/multiwall-carbon-nanotube nanocomposites is determined both by segment chain dynamics and charge *** to the breakdown model analysis,the effects of multiwall-carbon-nanotube on enhanced breakdown strength are caused by the increased amount of deep traps in the interfacial region,while the influence of thickness is attributed to the enlarged segment chain displacement and electric field distortion as the voltage raising time increases.

关键词： strength breakdown nanocomposites

Hole-Transporting Materials with Rational Combination of Pyridine and Dibenzo[a,c]phenazine as Electron Acceptor for Dopant-Free Perovskite Solar Cells

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Chinese Journal of Chemistry 2024年第10期42卷 1100-1106页

作者： Weidong ling Fei Wu Wentao Yuan linna Zhu Qianqian li zhen li Hubei Key Lab on Organic and Polymeric Opto-Electronic Materials Department of ChemistryWuhan UniversityWuhanHubei 430072China Chongqing Key Laboratory for Advanced Materials and Technologies of Clean Energy Faculty of Materials&EnergySouthwest UniversityChongqing400715China TaiKang Center for life and Medical Sciences Wuhan UniversityWuhanHubei 430072China

Perovskite solar cells(PSCs)have been proven to be a promising option for photovoltaic *** the aim to achieve efficient and stable PSCs,it is essential to explore dopant-free hole-transporting materials(HTMs)with high hole ***,HTMs bearing electron donor(D)-electron acceptor(A)-electron donor(D)structures have been constructed with strong intramolecular charge transfer(ICT)effect,based on rational combination of dibenzo[a,c]phenazine and pyridine as electronic acceptors and anchoring groups to perovskite ***,high hole mobility(7.31×10^(-5) cm^(2)·V^(-1)·s^(-1))and photoelectric conversion efficiency(20.45%)have been achieved by dopant-free DPyP-based *** afforded an efficient way to design HTMs with high hole mobility by adjustment of molecular configurations and electronic property of conjugated systems.

关键词： Perovskite solar cell Charge transfer Donor-acceptor systems Energy conversion Hole mobility

A scalable one-pot strategy for the development of polymer electrolytes adaptable to room-temperature high-voltage lithium batteries

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Chinese Chemical Letters 2024年第3期35卷 461-467页

作者： Yue Guo Xinxin Qu zhen li Ruiyuan Tian Xiaokong liu State Key Laboratory of Supramolecular Structure and Materials College of ChemistryJilin UniversityChangchun 130012China Key Laboratory of Physics and Technology for Advanced Batteries(Ministry of Education) College of PhysicsJilin UniversityChangchun 130012China

Poly(ethylene oxide)(PEO)polymer electrolytes(PEs)have been commercially applied in liFePO_(4)||li solid-state lithium batteries(SSLBs).However,it remains challenging to develop PEO-based PEs applicable to the high-voltage SSLBs with higher energy density,owing to the poor electrochemical stability of ***,we report a scalable strategy for fabricating PEO-based PEs with high-voltage compatibility,by exploiting a new mechanism to stabilize the cathode-electrolyte interface in the highvoltage *** protocol only involves a one-pot synthesis procedure to covalently crosslink the PEO chains,in the presence of high-content lithium bis(trifluoromethylsulphonyl)imide(liTFSI)salts and N,N-dimethylformamide(DMF).liTFSI-DMF supramolecular aggregates are formed and firmly embedded in the polymer network,endowing the PE with high room-temperature ionic *** dissociated and highly concentrated TFSI^-anions can enter the Helmholtz layer close to the high-voltage cathode,leading to the formation of a thin and homogeneous cathode electrolyte interface(CEI),mainly composed of liF,on the *** CEI with high electrochemical stability can effectively stabilize the cathode-electrolyte interface,enabling long-term stable cycling of the high-voltage liCoO_(2)||li and nickelrich NCM_(622)||li batteries at room *** simplicity and scalability of the strategy makes the reported PEO-based PE potentially applicable in high-voltage SSLBs in practice.

关键词： lithium batteries Polymer electrolytes Poly(ethylene oxide) Energy density High-voltage cathodes

Enhancing flotation recovery of residual carbon from gasification waste by mixing hydrophobic powder with diesel as collector

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Particuology 2024年第6期89卷 211-217页

作者： Rui Han Ningning Zhang Anning Zhou zhen li Jinzhou Qu Hong Wang College of Chemistry and Chemical Engineering Xi’an University of Science and TechnologyXi’anShaanxi 710054China

Coal gasification fine slag(CGFS)is a solid waste containing residual carbon and ash generated during the coal gasification process,and the separation of the two components is the essential way to realize its environmental pollution reduction and resource value *** flotation is the preferred method for separating CGFS,but there is a barrier of low carbon recovery in this process due to the extensive adsorption of collector by the well-developed pores on residual *** this study,a sufficiently simple yet innovative collector,a mixture of hydrophobic powder and diesel,was proposed in an attempt to break the *** experiments with common diesel and this novel collector were performed respectively,and FTIR,XPS,and SEM-EDX were employed to analyze the collector action *** results revealed that the novel collector could significantly improve the residual carbon recovery;test results demonstrated that the novel collector could increase the hydrophobic functional group content on the fine slag surface,and the hydrophobic powders in this novel collector mainly appeared at the pore openings of the flotation *** essence of the mechanism is that the hydrophobic powders play a dual role of blocking pores and providing adsorption sites,thus facilitating the spreading of diesel on the carbon surface and promoting its *** study can provide creative ideas for the efficient disposal of coal gasification waste.

关键词： Coal gasification fine slag Carbon recovery Collector Fotation Hydrophobic powder