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Zwitterionic ring-opening polymerization of macrocyclic ethyleneoxy-substituted carbonate:Access to cyclic PEG-like polycarbonate

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Chinese Chemical Letters 2024年第3期35卷 282-286页

作者： Jin Huang Jinwen Li Rui Yan Yuanyuan qu Fengzhen guo Lei Shen Can-liang Ma Jie Sun Zhenjiang Li Kai guo State Key Laboratory of Materials-Oriented Chemical Engineering College of Biotechnology and Pharmaceutical EngineeringNanjing Tech UniversityNanjing 211816China Institute of Nanjing Advanced Biomaterials&Processing Equipment Lishui Economic Development ZoneNanjing 211299China

The innovation in polymer design to rival conventional polyethylene glycol(PEG)is an important approach to achieving a more sustainable ***,cyclic PEG-like polycarbonates having high molecular weight(4.4–49.5 kg/mol)were enabled through zwitterionic ring-opening polymerization(ZROP)of macrocyclic carbonates(MCs)mediated by N-heterocyclic carbene(NHC).The thermodynamic behavior of polymerization depends on the ring size of *** this process,the ZROP of 11-membered MC was driven by the change of enthalpy(ΔH_(p))which differed from the ZROP of 14-membered MC driven by the entropic change(ΔS_(p)).Cyclic polycarbonates depicted improved thermostability(T_(d5%)≥204℃)and higher glass transition temperatures(T_(g)>–40℃)in comparison to their linear analogues(T_(d5%)≤185℃,T_(g)~–50℃).In addition,the mechanism of ZROP of MC was addressed through computational study.A distinct mechanism of polymerization distinguishable from the well-known NHC-mediated ZROP of cyclic esters was revealed,where the zwitterion from nucleophilic addition to MC,*** intermediate,cannot be ring-opened probably due to the delocalization of negative charge on the carbonate group,but serves as an active center for the *** comparison to PEG,the attained polymer demonstrated comparable hydrophilic and biocompatible properties,as revealed by the results of contact angle and in vitro cytotoxicity studies,suggesting that cyclic polycarbonate hold the promise as the alternative of PEG.

关键词： Zwitterionic ring-opening polymerization Cyclic polycarbonate Macrocycles Tetrahedral intermediate NHC carbene

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Optimization on crystallization process of the magnetic core lysozyme

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Particuology 2024年第4期87卷 106-113页

作者： Lixia Hou Chunxiao qu Min Su Zhihan liang Qi Hao School of Chemical Engineering Hebei University of TechnologyTianjin300130China

The continuous growth of the biomedical market highlights the significance of improvement in the ef-ficiency of batch production for protein drug ***,we investigated the effect of polymer-modified Fe_(3)O_(4) nanoparticles on lysozyme(Lys)crystallization at different conditions,using function-alized Fe_(3)O_(4) magnetic nanoparticles(Polymer C@Fe_(3)O_(4))as nucleation *** study revealed that the surface charge density of Polymer C@Fe_(3)O_(4) was highest at a modification mass ratio of Fe_(3)O_(4) to Polymer C is 8∶*** ratio facilitates the augmentation of electrostatic interaction and the promotion of *** adding 15%of the PolymerC@Fe_(3)O_(4) prepared from Fe_(3)O_(4) with an average particle size of 150 nm,the magnetic core lysozyme(M-Lys)crystals with an average particle size of 11.08μm,narrow size distribution,and regular morphology were obtained in a yield of 82.42%within 60 min.

关键词： Protein Crystallization Magnetic particle Lysozyme

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Enhancing the peroxidase-like activity of MoS_(2)-based nanozymes by introducing attapulgite for antibacterial application and sensitive detection of glutathione

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Nano Research 2024年第8期17卷 7415-7426页

作者： Feng Feng Yihe Zhang Xiao Zhang Bin Mu Jiahe Zhang Wenjie qu Wangshu Tong Minmin liang Qi An Zhanjun guo Lu Zhao Engineering Research Center of Ministry of Education for Geological Carbon Storage and Low Carbon Utilization of Resources Beijing Key Laboratory of Materials Utilization of Nonmetallic Minerals and Solid WastesNational Laboratory of Mineral MaterialsSchool of Materials Science and TechnologyChina University of Geosciences(Beijing)Beijing 100083China Key Laboratory of Clay Mineral Applied Research of Gansu Province Lanzhou Institute of Chemical PhysicsChinese Academy of SciencesLanzhou 730000China Experimental Center of Advanced Materials School of Materials Science and Engineering School of Materials Science and EngineeringBeijing Institute of TechnologyBeijing 100081China

Nanozymes are next-generation of nanomaterials with enzyme-like *** particular,nanozymes with peroxidase(POD)-like activity have been utilized in various fields,including antibacterial,detection,degradation,***,their extensive applications were limited by their low catalytic activity ***,we have presented a composite nanozyme based on attapulgite(ATP)(Fe-ATP-MoS_(2)(FAM)),which exhibited enhanced POD-like activity(185.33 U·mg^(−1)),4.25 times higher than that of Fe-MoS_(2)(FM)(43.63 U·mg^(−1)).The density functional theory(DFT)calculations indicated that the addition of ATP increased the electron density of metal centers(Mo and Fe).More importantly,Michaelis–Menten kinetics revealed that the introduction of ATP significantly enhanced the binding affinities of substrates through the pores of ATP,forming a highly concentrated substrate microenvironment and thus promoting its POD-like ***,from molecular size and kinetic analysis,we proposed that the changes in substrate size before and after oxidation also significantly affected its Michaelis-constant(Km)***,we utilized FAM in the applications of highly effective antibacterial application and sensitive detection of glutathione(GSH).In conclusion,this work provides a novel approach for designing a highly efficient nanozyme based on natural mineral composites.

关键词： attapulgite peroxidase electron density affinity antibacterial

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Enhanced degradation of refractory organics in ORR-EO system with a blue TiO_(2)nanotube array modified Ti-based Ni-Sb co-doped SnO_(2)anode

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Chinese Chemical Letters 2024年第8期35卷 391-395页

作者： Yifen He Chao qu Na Ren Dawei liang Department of Materials Chemistry School of Materials Science&EngineeringBeihang UniversityBeijing 102206China Department of Environmental Science Faculty of Environment&LifeBeijing University of TechnologyBeijing 100124China

Recently,a novel 2-electron oxygen reduction reaction(ORR)based electro-oxidation(EO)system was developed,which utilizes a H_(2)O_(2)generation cathode instead of H_(2)evolution cathode.A Ti-based Ni-Sb co-doped SnO_(2)(Ti/NATO)anode was selected for efficient degradation of refractory organics and O_(3)*** synergistic reaction of O3/H_(2)O_(2)further accelerated the generation of hydroxyl radicals(·OH)in the ORR-EO ***,the catalytic activity and long-term effectiveness of the Ti/NATO anode limited the large-scale application of the ORR-EO *** this study,a blue TiO_(2)nanotube array(blue-TiO_(2)-NTA)inter-layer was introduced into the fabrication process between the Ti substrate and NATO catalyst *** to the Ti/NATO anode,the Ti/blue-TiO_(2)-NTA/NATO anode achieved higher efficiency of organic removal and O_(3)***,the accelerated lifetime of the Ti/blue-TiO_(2)-NTA/NATO anode was increased by 7 times compared to the Ti/NATO *** combined with CNTs-C/PTFE air cathode in ORR-EO system,all anodic oxidation and O_(3)/H_(2)O_(2)processes achieved higher•OH *** 92%of TOC in leachate bio-effluent was effectively eliminated with a relatively low energy cost of 45 kWh/t.

关键词： Electro-oxidation Blue TiO_(2)nanotube array O_(3)/H_(2)O_(2)process Refractory organics Leachate bio-effluent

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Cascade utilization of full spectrum solar energy for achieving simultaneous hydrogen production and all-day thermoelectric conversion

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Journal of Energy Chemistry 2024年第9期96卷 318-327页

作者： Tuo Zhang liang Dong Baoyuan Wang Jingkuo qu Xiaoyuan Ye Wengao Zeng Ze Gao Bin Zhu Ziying Zhang Xiangjiu Guan Liejin guo International Research Center for Renewable Energy(IRCRE) State Key Laboratory of Multiphase Flow in Power EngineeringXi’an Jiaotong UniversityXi’an 710049ShaanxiChina

Solar-driven photocatalytic water/seawater splitting holds great potential for green hydrogen ***,the practical application is hindered by the relatively low conversion efficiency resulting from the inadequate utilization of solar spectrum with significant waste in the form of ***,current equipment struggles to maintain all-day operation subjected to the lack of light during ***,a novel hybrid system integrating photothermal catalytic(PTC)reactor,thermoelectric generator(TEG),and phase change materials(PCM)was proposed and designed(named as PTC-TEG-PCM)to address these challenges and enable simultaneous overall seawater splitting and 24-hour power *** PTC system effectively maintains in an optimal temperature range to maximize photothermal-assisted photocatalytic hydrogen *** TEG component recycles the low-grade waste heat for power generation,complementing the shortcoming of photocatalytic conversion and achieving cascade utilization of full-spectrum solar ***,exceptional thermal storage capability of PCM allow for the conversion of released heat into electricity during nighttime,contributing significantly to the overall power output and enabling PTC-TEG-PCM to operate for more than 12 h under the actual *** to traditional PTC system,the overall energy conversion efficiency of the PTC-TEG-PCM system can be increased by∼500%,while maintaining the solar-to-hydrogen *** advancement of this novel system demonstrated that recycling waste heat from the PTC system and utilizing heat absorption/release capability of PCM for thermoelectric application are effective strategies to improve solar energy *** flexible parameter designing,PTC-TEG-PCM can be applied in various scenarios,offering high efficiency,stability,and sustainability.

关键词： Hybrid solar energy conversion system Photocatalytic overall seawatersplitting Thermoelectric power generation Phase change materials All-day operation

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A refined deviatoric hardening plastic model for sand

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Journal of Rock Mechanics and Geotechnical Engineering 2024年第7期16卷 2813-2821页

作者： Min Wang Tongming qu Yuntian Feng Teng liang liangtong Zhan MOE Key Laboratory of Soft Soils and Geoenvironmental Engineering Zhejiang UniversityHangzhou310058China Department of Civil and Environmental Engineering Hong Kong University of Science and TechnologyKowloon999077Hong KongChina Zienkiewicz Centre for Computational Engineering College of EngineeringSwansea UniversitySwanseaWalesSA18EPUK Center for Hypergravity Experimental and Interdisciplinary Research Zhejiang UniversityHangzhou310058China

The classical deviatoric hardening models are capable of characterizing the mechanical response of granular materials for a broad range of degrees of *** work finds that it has limitations in accurately predicting the volumetric deformation characteristics under a wide range of confining/consolidation *** issue stems from the pressure independent hardening law in the classical deviatoric hardening *** overcome this problem,we propose a refined deviatoric hardening model in which a pressure-dependent hardening law is developed based on experimental *** between numerical results and laboratory triaxial tests indicate that the improved model succeeds in capturing the volumetric deformation behavior under various confining/consolidation pressure conditions for both dense and loose ***,to examine the importance of the improved deviatoric hardening model,it is combined with the bounding surface plasticity theory to investigate the mechanical response of loose sand under complex cyclic loadings and different initial consolidation *** is proved that the proposed pressure-dependent deviatoric hardening law is capable of predicting the volumetric deformation characteristics to a satisfactory degree and plays an important role in the simulation of complex deformations for granular geomaterials.

关键词： Elasto-plastic deformation Isotropic hardening Deviatoric plastic strain Granular material Kinematic hardening Bounding surface

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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

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Leveraging diverse cell-death patterns to predict the clinical outcome of immune checkpoint therapy in lung adenocarcinoma:Based on muti-omics analysis and vitro assay

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Oncology Research 2024年第2期32卷 393-407页

作者： HONGYUAN liang YANQIU LI YONGGANG qu LINGYUN ZHANG Department of Radiology Shengjing Hospital of China Medical UniversityShenyangChina Department of Nephrology The First Affiliated Hospital of China Medical UniversityShenyangChina Department of Clinical Medicine China Medical UniversityShenyangChina Department of Medical Oncology The First Hospital of China Medical UniversityShenyangChina

Advanced LUAD shows limited response to treatment including immune *** the development of sequencing omics,it is urgent to combine high-throughput multi-omics data to identify new immune checkpoint therapeutic response *** GSE72094(n=386)and GSE31210(n=226)gene expression profile data in the GEO database,we identified genes associated with lung adenocarcinoma(LUAD)death using tools such as“edgeR”and“maftools”and visualized the characteristics of these genes using the“circlize”R *** constructed a prognostic model based on death-related genes and optimized the model using LASSO-Cox regression *** calculating the cell death index(CDI)of each individual,we divided LUAD patients into high and low CDI groups and examined the relationship between CDI and overall survival time by principal component analysis(PCA)and Kaplan-Meier *** also used the“ConsensusClusterPlus”tool for unsupervised clustering of LUAD subtypes based on model *** addition,we collected data on the expression of immunomodulatory genes and model genes for each cohort and performed tumor microenvironment *** also used the TIDE algorithm to predict immunotherapy responses in the CDI ***,we studied the effect of PRKCD on the proliferation and migration of LUAD cells through cell culture *** study utilized the TCGA-LUAD cohort(n=493)and identified 2,901 genes that are differentially expressed in patients with *** KEGG and GO enrichment analysis,these genes were found to be involved in a wide range of biological *** study also used univariate Cox regression models and LASSO regression analyses to identify 17 candidate genes that were best associated with mortality prognostic risk *** comparing the overall survival(OS)outcomes of patients with different CDI values,it was found that increased CDI levels were significantly associated with lower OS *** addition,the study used unsupervised cluster analysis to d

关键词： Lung adenocarcinoma Programmed cell death Iron-death Drug sensitivity Cancer therapy

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Current observation and analysis based on mooring systems in the Andaman Sea

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Journal of Oceanology and Limnology 2024年第2期42卷 484-491页

作者： Yimeng WANG Jingsong guo Dapeng qu Zhixin ZHANG Chalermrat SANGMANEE Varintha VASINAMEKHIN Binghuo guo First Institute of Oceanography and Key Laboratory of Marine Science and Numerical ModelingMinistry of Natural ResourcesQingdao 266061China Laboratory for Regional Oceanography and Numerical Modeling Pilot National Laboratory for Marine Science and Technology(Qingdao)Qingdao 266237China Shandong Key Laboratory of Marine Science and Numerical Modeling Qingdao 266061China Phuket Marine Biological Center Department of Marine and Coastal ResourcesPhuket 83000Thailand Marine and Coastal Resources Research&Development Institute Department of Marine and Coastal ResourcesBangkok 10210Thailand

The basic structure and intraseasonal evolution of currents in the southeastern Andaman Sea was analyzed based on data collected in 2017 from two subsurface moorings(C1 and C5).Periodic variation in the upper ocean currents of the Andaman Sea was investigated by combining observational and satellite *** observations show that rapid changes of current speed and direction occurred in May and June,with a significant increase in current velocity at the C1 *** the second half of the year,southward flow dominated at the C1 mooring,and alternating northward and southward flows were evident at the C5 mooring during the same period but the northward flow prevailed in boreal *** addition,analysis of the power spectra of the upper currents revealed that the tidal period at both moorings is primarily semidiurnal with weaker energy than that of the low-frequency *** upper ocean currents at the C1 and C5 moorings exhibited intraseasonal variation of 30-60 d and 120 d,while the zonal current at the C1 mooring exhibited a notable period of approximately 180 *** analysis indicated that the variability of currents in the Andaman Sea is influenced primarily by equatorial Kelvin waves and Rossby wave ***,our results suggest that equatorial Kelvin waves from the eastern Indian Ocean entered the Andaman Sea in the form of Wyrtki Jets and propagated primarily along two distinct pathways during the observation *** addition to coastal boundary Kelvin waves,it was found that a branch of the Wyrtki Jet that directly enters the Andaman Sea and flows northward along the slope of the continental shelf,and reflected Rossby wave packets by topography.

关键词： mooring observation Wyrtki Jet Rossby waves intraseasonal variation

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Modelling the water diversion of a sustainable cover system under humid climates

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Journal of Rock Mechanics and Geotechnical Engineering 2024年第7期16卷 2429-2440页

作者： Haowen guo Charles Wang Wai Ng Qi Zhang Chuanxiang qu Liwen Hu Shenzhen Research Institute of Hong Kong University of Science and Technology Shenzhen518057China Department of Civil and Environmental Engineering The Hong Kong University of Science and TechnologyHong Kong SAR999077China CCCC Fourth Harbor Engineering Institute Co. LtdGuangzhou510230China

Extreme rainfall significantly threatens the safety of the landfill cover system,especially under humid *** study aims to provide design recommendations for a sustainable landfill cover system consisting of a low-permeability soil layer underlying a two-layer capillary barrier for humid ***,the numerical back-analysis was conducted for verification against a series of flume model ***,a parametric study was performed to investigate the effects of inclination angle,particle size and layer thickness on the lateral diversion length(DL)of the three-layer cover system under the 100-year return period rainfall of humid *** results show that the water lateral DL of the cover system can be greatly enhanced by increasing the inclination angle from 3°to 18°.Moreover,the bottom layer of the cover system with a coarser d10 was more susceptible to the impact of the heavy rainfall,while this can be alleviated by increasing the thickness of the bottom layer.A dimensionless number,defined as the ratio of thickness and d_(10) of the bottom layer,is proposed for designing lateral diversion of the three-layer cover system under humid *** preserve the maximum DL,it is suggested that the proposed dimensionless number should be larger than 95 and 110 for the design of rainfall events with 50-year and 100-year return periods for humid climates,respectively.

关键词： Unsaturated soil Recycling Construction waste Three-layer landfill cover Water infiltration

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