Luminescent metal-organic frameworks(MOFs)have garnered significant attention due to their structural tunability and potential applications in solid-state lighting,bioimaging,sensing,anticounterfeiting,and other field...Luminescent metal-organic frameworks(MOFs)have garnered significant attention due to their structural tunability and potential applications in solid-state lighting,bioimaging,sensing,anticounterfeiting,and other fields.Nevertheless,due to the tendency of1,4-benzenedicarboxylic acid(BDC)to rotate within the framework,MOFs composed of it exhibit significant non-radiative energy dissipation and thus impair the emissive properties.In this study,efficient luminescence of MIL-140A nanocrystals(NCs)with BDC rotors as ligands is achieved by pressure treatment strategy.Pressure treatment effectively modulates the pore structure of the framework,enhancing the interactions between the N,N-dimethylformamide vip molecules and the BDC ligands.The enhanced host-vip interaction contributes to the structural rigidity of the MOF,thereby suppressing the rotation-induced excited-state energy loss.As a result,the pressure-treated MIL-140A NCs displayed bright blue-light emission,with the photoluminescence quantum yield increasing from an initial 6.8%to 69.2%.This study developed an effective strategy to improve the luminescence performance of rotor ligand MOFs,offers a new avenue for the rational design and synthesis of MOFs with superior luminescent properties.展开更多
BACKGROUND Calculus bovis(CB),used in traditional Chinese medicine,exhibits anti-tumor effects in various cancer models.It also constitutes an integral component of a compound formulation known as Pien Tze Huang,which...BACKGROUND Calculus bovis(CB),used in traditional Chinese medicine,exhibits anti-tumor effects in various cancer models.It also constitutes an integral component of a compound formulation known as Pien Tze Huang,which is indicated for the treatment of liver cancer.However,its impact on the liver cancer tumor microenvironment,particularly on tumor-associated macrophages(TAMs),is not well understood.AIM To elucidate the anti-liver cancer effect of CB by inhibiting M2-TAM polarization via Wnt/β-catenin pathway modulation.METHODS This study identified the active components of CB using UPLC-Q-TOF-MS,evaluated its anti-neoplastic effects in a nude mouse model,and elucidated the underlying mechanisms via network pharmacology,transcriptomics,and molecular docking.In vitro assays were used to investigate the effects of CB-containing serum on HepG2 cells and M2-TAMs,and Wnt pathway modulation was validated by real-time reverse transcriptase-polymerase chain reaction and Western blot analysis.RESULTS This study identified 22 active components in CB,11 of which were detected in the bloodstream.Preclinical investigations have demonstrated the ability of CB to effectively inhibit liver tumor growth.An integrated approach employing network pharmacology,transcriptomics,and molecular docking implicated the Wnt signaling pathway as a target of the antineoplastic activity of CB by suppressing M2-TAM polarization.In vitro and in vivo experiments further confirmed that CB significantly hinders M2-TAM polarization and suppresses Wnt/β-catenin pathway activation.The inhibitory effect of CB on M2-TAMs was reversed when treated with the Wnt agonist SKL2001,confirming its pathway specificity.CONCLUSION This study demonstrated that CB mediates inhibition of M2-TAM polarization through the Wnt/β-catenin pathway,contributing to the suppression of liver cancer growth.展开更多
Low-dimensional hybrid metal halides exhibit broadband emission and high photoluminescence quantum yield(PLQY), making them promising candidates for the next-generation luminescent materials in lighting applications. ...Low-dimensional hybrid metal halides exhibit broadband emission and high photoluminescence quantum yield(PLQY), making them promising candidates for the next-generation luminescent materials in lighting applications. Here,the emission intensity of(C_(12)H_(24)O_(6))_(2)Na_(2)(H_(2)O)_(3)Cu_(4)I_(6) was strengthened between 9.3 GPa and 17.2 GPa, accompanied by the redshift of emission wavelength. The photoluminescence(PL) of Cu(Ⅰ)-based organometallic halides originates from multiple emission states, which are a metal-to-ligand charge transfer or a halide-to-ligand charge transfer(MLCT/HLCT)excited state and a cluster-centered(CC) excited state. MLCT/HLCT-related emission wavelength redshifts while CCrelated emission wavelength remains unchanged, indicating that the rearrangement of different emission states plays a critical role in the changes of luminescence wavelength. This study not only deepens the understanding of the influence of high pressure on(C_(12)H_(24)O_(6))_(2)Na_(2)(H_(2)O)_(3)Cu_(4)I_(6), but also provides valuable insights into the structure–property relationship of zero-dimensional Cu(Ⅰ)-based organometallic halides.展开更多
The stability of clarified juice is of great importance in the beverage industry and to consumers.Phenolic compounds are considered to be one of the main factors responsible for sediment formation.The aim of this stud...The stability of clarified juice is of great importance in the beverage industry and to consumers.Phenolic compounds are considered to be one of the main factors responsible for sediment formation.The aim of this study is to investigate the changes in the phenolic content in clarified mulberry juice during storage.Hence, separation, identification, quantification, and analysis of the changes in the contents of phenolic compounds, both free and bound forms, in the supernatant and sediments of mulberry juice, were carried out using high performance liquid chromatographic system, equipped with a photo-diode array detector（HPLC-PDA） and HPLC coupled with quadrupole-time of flight mass spectrometric（HPLC-QTOF-MS/MS） techniques.There was an increase in the amount of sediment formed over the period of study.Total phenolic content of supernatant, as well as free phenolic content in the extracts of the precipitate decreased, whereas the bound phenolic content in the sediment increased.Quantitative estimation of individual phenolic compounds indicated high degradation of free anthocyanins in the supernatant and sediment from 938.60 to 2.30 mg/L and 235.60 to 1.74 mg/g, respectively.A decrease in flavonoids in the supernatant was also observed, whereas the contents of bound forms of gallic acid, protocatechuic acid, caffeic acid, and rutin in the sediment increased.Anthocyanins were the most abundant form of phenolics in the sediment, and accounted for 67.2% of total phenolics after 8 weeks of storage.These results revealed that phenolic compounds, particularly anthocyanins, were involved in the formation of sediments in mulberry juice during storage.展开更多
Organic luminescent materials are very sensitive to external stimuli,such as pressure,temperature,and electric field.The luminescent properties of some organic luminescent materials significantly change under high pre...Organic luminescent materials are very sensitive to external stimuli,such as pressure,temperature,and electric field.The luminescent properties of some organic luminescent materials significantly change under high pressure.Some materials may show luminescence discoloration,whereas some may exhibit luminescence enhancement.These properties have many potential applications in anticounterfeiting,force sensor,data recording and storage,and luminescent devices,thereby greatly attracting the attention of scientists.In this review,the progress of research on these materials at high pressure in recent years is summarized.展开更多
Flourishing rare earth superhydrides are a class of recently discovered materials that exhibit near-room-temperature superconductivity at high pressures,ushering in a new era of superconductivity research at high pres...Flourishing rare earth superhydrides are a class of recently discovered materials that exhibit near-room-temperature superconductivity at high pressures,ushering in a new era of superconductivity research at high pressures.Yttrium superhydrides drew the most attention among these superhydrides due to their abundance of stoichiometries and excellent superconductivities.Here,we carried out a comprehensive study of yttrium superhydrides in a wide pressure range of 140 GPa-300 GPa.We successfully synthesized a series of superhydrides with the compositions of YH_(4),YH_(6),YH_(7),and YH_(9),and reported superconducting transition temperatures of 82 K at 167 GPa,218 K at 165 GPa,29 K at 162 GPa,and230 K at 300 GPa,respectively,as evidenced by sharp drops in resistance.The structure and superconductivity of YH_(4) were taken as a representative example and were also examined using x-ray diffraction measurements and the superconductivity suppression under external magnetic fields,respectively.Clathrate YH_(10),a candidate for room-temperature superconductor,was not synthesized within the study pressure and temperature ranges of up to 300 GPa and 2000 K.The current study established a detailed foundation for future research into room-temperature superconductors in polynary yttrium-based superhydrides.展开更多
SiO_(2)is the major mineral substance in the upper mantle of the earth.Therefore,studies of the silica-coated materials under high-pressure are essential to explore the physical and chemical properties of the upper ma...SiO_(2)is the major mineral substance in the upper mantle of the earth.Therefore,studies of the silica-coated materials under high-pressure are essential to explore the physical and chemical properties of the upper mantle.The silica-confined CsPbBr_(3)nanocrystals(NCs)have recently attracted much attention because of the improved photoluminescence(PL)quantum yield,owing to the protection of silica shell.However,it remains considerable interest to further explore the relationship between optical properties and the structure of CsPbBr_(3)@SiO_(2)NCs.We systemically studied the structural and optical properties of the CsPbBr_(3)@SiO_(2)NCs under high pressure by using diamond anvil cell(DAC).The discontinuous changes of PL and absorption spectra occurred at~1.40 GPa.Synchrotron X-ray diffraction(XRD)studies of CsPbBr_(3)@SiO_(2)NCs under high pressure indicated an isostructural phase transformation at about 1.36 GPa,owing to the pressure-induced tilting of the Pb-Br octahedra.The isothermal bulk moduli for two phases are estimated about 60.0 GPa and 19.2 GPa by fitting the equation of state.Besides,the transition pressure point of CsPbBr_(3)@SiO_(2)NCs is slightly higher than that of pristine CsPbBr_(3)NCs,which attributed to the buffer effect of coating silica shell.The results indicate that silica shell is able to enhance the stabilization without changing the relationship between optical properties and structure of CsPbBr_(3)NCs.Our results were fascinated to model the rock metasomatism in the upper mantle and provided a new‘lithoprobe’for detecting the upper mantle.展开更多
Mechanoresponsive luminescent(MRL)materials have drawn extensive concern due to their potential applications in mechanical sensors,memory chips,and security inks;especially these possessing high emission efficiency.In...Mechanoresponsive luminescent(MRL)materials have drawn extensive concern due to their potential applications in mechanical sensors,memory chips,and security inks;especially these possessing high emission efficiency.In this work,we found trans-stilbene crystal exhibited two different pressure-induced emission enhancement(PIEE)behaviors at different pressure areas.The structural characterizations combined with density functional theory calculation indicate that the first emission enhancement was due to the decrease of nonradiation transition by the weaken of energy exchange process between atoms and lattice.And the second emission enhancement was attributed to the strengthen of C-H...C interactions from the non-planarization comformation.The results regarding the mechanoresponsive behavior of trans-stilbene offered a deep insight into PIEE from the structural point of view,which will facilitate the design of and search for high-performance MRL materials.展开更多
The origin and history of the Earth are manifested as the evolutionary processes of chemistry and physics of its interiors,which can be recognized by deciphering the geochemical signals recorded in minerals and rocks....The origin and history of the Earth are manifested as the evolutionary processes of chemistry and physics of its interiors,which can be recognized by deciphering the geochemical signals recorded in minerals and rocks.Deep interiors of the Earth and other rocky planets are under both extreme pressure and temperature,i.e.,approximately 360 gigapascals(GPa)and as high as 7000 K at the center of the Earth.展开更多
The penetration rate of distributed generation is gradually increasing in the distribution system concerned.This is creating new problems and challenges in the planning and operation of the system.The intermittency an...The penetration rate of distributed generation is gradually increasing in the distribution system concerned.This is creating new problems and challenges in the planning and operation of the system.The intermittency and variability of power outputs from numerous distributed renewable generators could significantly jeopardize the secure operation of the distribution system.Therefore,it is necessary to assess the hosting capability for intermittent distributed generation by a distribution system considering operational constraints.This is the subject of this study.An assessment model considering the uncertainty of generation outputs from distributed generators is presented for this purpose.It involves different types of regulation or control functions using on-load tap-changers(OLTCs),reactive power compensation devices,energy storage systems,and the reactive power support of the distributed generators employed.A robust optimization model is then attained It is solved by Bertsimas robust counterpart through GUROBI solver.Finally,the feasibility and efficiency of the proposed method are demonstrated by a modified IEEE 33-bus distribution system.In addition,the effects of the aforementioned regulation or control functions on the enhancement of the hosting capability for intermittent distributed generation are examined.展开更多
Dear Editor,This letter aims to investigate the optimization problem where the decision variable is contained in a closed convex set.By combing the gradient decent-like method with the push-sum algorithm framework,we ...Dear Editor,This letter aims to investigate the optimization problem where the decision variable is contained in a closed convex set.By combing the gradient decent-like method with the push-sum algorithm framework,we design the distributed iterative formulas under the condition that the considered graphs sequence is time-varying and unbalanced.展开更多
Large-volume presses(LVPs)providing large volumes,liquid media,deformation capability,jump compression,and in situ measurements are in great demand for high-pressure research,particularly in the fields of geoscience,c...Large-volume presses(LVPs)providing large volumes,liquid media,deformation capability,jump compression,and in situ measurements are in great demand for high-pressure research,particularly in the fields of geoscience,condensed matter physics,material science,chemistry,and biology.A high-pressure and high-temperature(HPHT)platform with different LVP subsystems,both solid-state and liquid environments,and nonequilibrium subsystems,has been constructed at the Synergetic Extreme Condition User Facility,Jilin University.This article describes the construction of the different subsystems and provides an overview of the capabilities and characteristics of the different HPHT subsystems.A large sample volume(1000 mm^(3))at 20 GPa is achieved through the use of a belt-type apparatus in the solid-state subsystem.HPHT conditions(1.8 GPa and 1000 K)are realized in the liquid subsystem through the use of a piston-cylinder-type LVP with optical diamond windows for in situ spectroscopic measurements.A maximum pressure jump to 10.2 GPa can be reached within 20 ms in the nonequilibrium subsystem with the use of an improved bladder-pressurization jump press.Some typical results obtained with different LVPs are briefly reviewed to illustrate the applications and advantages of these presses.In summary,the platform described here has the potential to contribute greatly to high-pressure research and to innovations in high-pressure technology.展开更多
Solid-state fluorescent multi-color carbon dots(SFM-CDs),prepared using the same precursor(s)without the need for dispersion in a solid matrix,are highly demanded for a wide range of applications.Herein,we report a mi...Solid-state fluorescent multi-color carbon dots(SFM-CDs),prepared using the same precursor(s)without the need for dispersion in a solid matrix,are highly demanded for a wide range of applications.Herein,we report a microwave-assisted strategy for the prepara-tion of SFM-CDs with blue,yellow and red emissions within 5 min from the same precursors.The as-prepared B-CDs,Y-CDs,and R-CDs possessed bright fluorescence at 425 nm,550 nm,and 640 nm,and photoluminescence quantum yields(PLQYs)of 54.68%,17.93%,and 2.88%,respectively.The structure of SFM-CDs consisted of 5-oxo-3,5-dihydro-2H-thiazolo[3,2-a]pyridine-7-carboxylic acid(TPCA)immobilized on the surface of a carbon core,with the size of the carbon core and degree of disulfide crosslinking between CDs both increasing on going from the B-CDs to the R-CDs,as verified by mechanochromic experiments.The excellent solid-state fluorescence performance of the SFM-CDs allowed their utilization as the fluorescent converter layer in multi-color LEDs and white LEDs with a high color rendering index.展开更多
As an extensively used chemical product,cyclic carbonate was generally synthesized by transesterification,or the cycloaddition of epoxides,diols with CO2.To reduce the production costs and expand the raw materials,alk...As an extensively used chemical product,cyclic carbonate was generally synthesized by transesterification,or the cycloaddition of epoxides,diols with CO2.To reduce the production costs and expand the raw materials,alkenyl and alkynyl substrates have caused much attention in the synthesis of cyclic carbonates,such as olefins,allyl alcohols and propargylic alcohols.Based on the alkenyl substrate,the synthetic process involves a continuous reaction of oxidative carboxylation,with epoxide or halohydrin as an intermediate usually.Therefore,peroxides and nucleophiles （halogens or organic bases） are often necessary in the conversion.Using propargylic alcohols to produce a-alkylidene cyclic carbonates,noble metal catalysts play crucial roles in alkynyl activation,and organic bases are considered to assist the intramolecular and intermolecular proton transfer and combine CO2 molecular.As the carboxyl sources in products,inorganic carbonates and organic carboxylic acids also have some applications instead of CO2.In this review,we summarized the synthetic routes of cyclic carbonates from alkenyl and alkynyl substrates in the aspect of catalyst,mechanism and the development tendency.展开更多
Pressure, as a thermodynamic parameter, provides an appropriate method to detect weak intermolecular interactions. The C–H···H–B dihydrogen bond is so weak that the experimental evidence of this inter...Pressure, as a thermodynamic parameter, provides an appropriate method to detect weak intermolecular interactions. The C–H···H–B dihydrogen bond is so weak that the experimental evidence of this interaction is still limited. A combination of in situ high pressure Raman spectra and angle-dispersive X-ray diffraction(ADXRD) experiments was utilized to explore the dihydrogen bonds in dimethylamine borane(DMAB). Both Raman and ADXRD measurements suggested that the crystal structure of DMAB is stable in the pressure region from 1 atm(1 atm=1.01325×10~5 Pa) to 0.54 GPa. The red shift of CH stretching and CH_3 distortion modes gave strong evidence for the existence of C–H···H–B dihydrogen bonds. Further analysis of Raman spectra and Hirshfeld surface confirmed our proposal. This work provided a deeper understanding of dihydrogen bonds.And we wish that high pressure could be applied to identify other unconfirmed hydrogen or dihydrogen bond.展开更多
The interaction between organic and inorganic components in metal hybrid perovskites fundamentally determines the intrinsic optoelectronic performance.However,the underlying interaction sites have still remained elusi...The interaction between organic and inorganic components in metal hybrid perovskites fundamentally determines the intrinsic optoelectronic performance.However,the underlying interaction sites have still remained elusive,especially for those non-hydrogen-bonded hybrid perovskites,thus largely impeding materials precise design with targeted properties.Herein,high pressure is utilized to elucidate the interaction mechanism between organic and inorganic components in the as-synthesized one-dimensional hybrid metal halide(DBU)PbBr_(3)(DBU=1,8-diazabicyclo[5.4.0]undec-7-ene).The interaction sites are identified to be the N from DBU and the Br from inorganic framework by the indicative of enhanced Raman mode under high pressure.The change in interaction strength is indeed derived from the pressure modulation on both distance and spatial arrangement of the nearest Br and N,rather than traditional hydrogen-bonding effect.Furthermore,the enhanced interaction increased charge transfer,resulting in a cyan emission with photoluminescence quantum yields(PLQYs)of 86.6%.The enhanced cyan emission is particularly important for underwater communication due to the much less attenuation in water than at other wavelength emissions.This study provides deep insights into the underlying photophysical mechanism of non-hydrogen-bonded hybrid metal halides and is expected to impart innovative construction with superior performance.展开更多
Chalcogenide quantum dots(QDs)are established as promising materials for white-light-emitting applications because of their wide surface defect emission.However,the limited understanding of the origin of defect emissi...Chalcogenide quantum dots(QDs)are established as promising materials for white-light-emitting applications because of their wide surface defect emission.However,the limited understanding of the origin of defect emission poses challenges in attaining efficient white-light emission.Herein,we sought to introduce high pressure to strengthen the interaction between different types of ligands and QDs,as well as enable in situ observation of surface trap passivation that contributes to emission control.Under pressure,both defect emission and band-edge emission in the CdS QDs could be selectively enhanced by more than an order of magnitude through treatment with X-type and Z-type ligands,respectively.Our findings identified that surface hole traps predominantly contributed to defect emission,whereas nonradiative recombination was primarily associated with surface electron traps.Our goal was to service ambient science through high-pressure research.Thus,based on this proposed mechanism,an energy-saving“neutral”white light with a human-eyefriendly color rendering index of 86 was achieved by tuning the defect emission through further elimination of surface Cd sites.This study endowed high pressure as an efficient tool to elucidate the defect origin of chalcogenide QDs under ambient conditions,paving the way for precise control over white-light emission through materials design application in solid-state lighting.展开更多
The chemical synthesis of functional materials is inseparable from national defense,medical treatment,national economy,and people’s livelihood.Traditional organic and inorganic materials are approaching their perform...The chemical synthesis of functional materials is inseparable from national defense,medical treatment,national economy,and people’s livelihood.Traditional organic and inorganic materials are approaching their performance limit.Therefore,the design and exploitation of novel functional materials are imminent and of significance for sustainable development.This review outlines the current progress and future prospects of chemical synthesis driven by high pressure,including organic and inorganic synthesis,as well as high-pressure phase retention.Based on the latest works,the basic mechanism of high-pressure chemical synthesis and three potential strategies for high-pressure phase harvesting are revealed.Finally,the challenge and outlook of high-pressureguided chemical synthesis are summarized.We sincerely hope that this review will provide guidance for designing high-performance materials by expanding the paths of chemical synthesis,thus greatly exploiting the existing materials world with newly emerging and enhanced functionalities.展开更多
Conformational flexibility is essential to the stimuli-responsive property of organic materials,but achieving the reversible molecular transformation is still challenging in functional materials for the high energy ba...Conformational flexibility is essential to the stimuli-responsive property of organic materials,but achieving the reversible molecular transformation is still challenging in functional materials for the high energy barriers and restriction by intermolecular interactions.Herein,through the incorporation of various steric hindrances into phenothiazine derivatives with different positions and quantities to tune the molecular conformations by adjustable repulsive forces,the folded angles gradually changed from 180°to 90°in 17 compounds.When the angle located at 112°with moderated steric effect,dynamic and reversible transformation of conformations under mechanical force has been achieved for the low energy barriers and mutually regulated molecular motions,resulting in both selfrecoverable and stimuli-responsive phosphorescence properties for the first time.It opened up a new way to realize the self-recovery property of organic materials,which can facilitate the multi-functional property of smart materials with the opened avenue for other fields with inspiration.展开更多
基金supported by the National Key R&D Program of China(Grant No.2023YFA1406200)the National Natural Science Foundation of China(No.12274177 and 12304261)the China Postdoctoral Science Foundation(No.2024M751076)。
文摘Luminescent metal-organic frameworks(MOFs)have garnered significant attention due to their structural tunability and potential applications in solid-state lighting,bioimaging,sensing,anticounterfeiting,and other fields.Nevertheless,due to the tendency of1,4-benzenedicarboxylic acid(BDC)to rotate within the framework,MOFs composed of it exhibit significant non-radiative energy dissipation and thus impair the emissive properties.In this study,efficient luminescence of MIL-140A nanocrystals(NCs)with BDC rotors as ligands is achieved by pressure treatment strategy.Pressure treatment effectively modulates the pore structure of the framework,enhancing the interactions between the N,N-dimethylformamide vip molecules and the BDC ligands.The enhanced host-vip interaction contributes to the structural rigidity of the MOF,thereby suppressing the rotation-induced excited-state energy loss.As a result,the pressure-treated MIL-140A NCs displayed bright blue-light emission,with the photoluminescence quantum yield increasing from an initial 6.8%to 69.2%.This study developed an effective strategy to improve the luminescence performance of rotor ligand MOFs,offers a new avenue for the rational design and synthesis of MOFs with superior luminescent properties.
基金Supported by National Natural Science Foundation of China,No.82074450Education Department of Hunan Province,No.21A0243,No.21B0374,No.22B0397,and No.22B0392+2 种基金Research Project of"Academician Liu Liang Workstation"of Hunan University of Traditional Chinese Medicine,No.21YS003Hunan Administration of Traditional Chinese Medicine,No.B2023001 and No.B2023009Hunan Provincial Natural Science Foundation of China,No.2023JJ40481。
文摘BACKGROUND Calculus bovis(CB),used in traditional Chinese medicine,exhibits anti-tumor effects in various cancer models.It also constitutes an integral component of a compound formulation known as Pien Tze Huang,which is indicated for the treatment of liver cancer.However,its impact on the liver cancer tumor microenvironment,particularly on tumor-associated macrophages(TAMs),is not well understood.AIM To elucidate the anti-liver cancer effect of CB by inhibiting M2-TAM polarization via Wnt/β-catenin pathway modulation.METHODS This study identified the active components of CB using UPLC-Q-TOF-MS,evaluated its anti-neoplastic effects in a nude mouse model,and elucidated the underlying mechanisms via network pharmacology,transcriptomics,and molecular docking.In vitro assays were used to investigate the effects of CB-containing serum on HepG2 cells and M2-TAMs,and Wnt pathway modulation was validated by real-time reverse transcriptase-polymerase chain reaction and Western blot analysis.RESULTS This study identified 22 active components in CB,11 of which were detected in the bloodstream.Preclinical investigations have demonstrated the ability of CB to effectively inhibit liver tumor growth.An integrated approach employing network pharmacology,transcriptomics,and molecular docking implicated the Wnt signaling pathway as a target of the antineoplastic activity of CB by suppressing M2-TAM polarization.In vitro and in vivo experiments further confirmed that CB significantly hinders M2-TAM polarization and suppresses Wnt/β-catenin pathway activation.The inhibitory effect of CB on M2-TAMs was reversed when treated with the Wnt agonist SKL2001,confirming its pathway specificity.CONCLUSION This study demonstrated that CB mediates inhibition of M2-TAM polarization through the Wnt/β-catenin pathway,contributing to the suppression of liver cancer growth.
基金Project supported by the National Key R&D Program of China (Grant No. 2023YFA1406200)the National Natural Science Foundation of China (Grant Nos. 12174144 and 12474009)the Graduate Innovation Fund of Jilin University (Grant No. 2024CX201)。
文摘Low-dimensional hybrid metal halides exhibit broadband emission and high photoluminescence quantum yield(PLQY), making them promising candidates for the next-generation luminescent materials in lighting applications. Here,the emission intensity of(C_(12)H_(24)O_(6))_(2)Na_(2)(H_(2)O)_(3)Cu_(4)I_(6) was strengthened between 9.3 GPa and 17.2 GPa, accompanied by the redshift of emission wavelength. The photoluminescence(PL) of Cu(Ⅰ)-based organometallic halides originates from multiple emission states, which are a metal-to-ligand charge transfer or a halide-to-ligand charge transfer(MLCT/HLCT)excited state and a cluster-centered(CC) excited state. MLCT/HLCT-related emission wavelength redshifts while CCrelated emission wavelength remains unchanged, indicating that the rearrangement of different emission states plays a critical role in the changes of luminescence wavelength. This study not only deepens the understanding of the influence of high pressure on(C_(12)H_(24)O_(6))_(2)Na_(2)(H_(2)O)_(3)Cu_(4)I_(6), but also provides valuable insights into the structure–property relationship of zero-dimensional Cu(Ⅰ)-based organometallic halides.
基金Project supported by the China Agriculture Research System (No.CARS-22-02A)the National Natural Science Foundation of China (No.31501541)+1 种基金the Natural Science Foundation of Guangdong Province (No.2015A030312001)the Science and Technology Program of Guangzhou (No.201510010063), China
文摘The stability of clarified juice is of great importance in the beverage industry and to consumers.Phenolic compounds are considered to be one of the main factors responsible for sediment formation.The aim of this study is to investigate the changes in the phenolic content in clarified mulberry juice during storage.Hence, separation, identification, quantification, and analysis of the changes in the contents of phenolic compounds, both free and bound forms, in the supernatant and sediments of mulberry juice, were carried out using high performance liquid chromatographic system, equipped with a photo-diode array detector（HPLC-PDA） and HPLC coupled with quadrupole-time of flight mass spectrometric（HPLC-QTOF-MS/MS） techniques.There was an increase in the amount of sediment formed over the period of study.Total phenolic content of supernatant, as well as free phenolic content in the extracts of the precipitate decreased, whereas the bound phenolic content in the sediment increased.Quantitative estimation of individual phenolic compounds indicated high degradation of free anthocyanins in the supernatant and sediment from 938.60 to 2.30 mg/L and 235.60 to 1.74 mg/g, respectively.A decrease in flavonoids in the supernatant was also observed, whereas the contents of bound forms of gallic acid, protocatechuic acid, caffeic acid, and rutin in the sediment increased.Anthocyanins were the most abundant form of phenolics in the sediment, and accounted for 67.2% of total phenolics after 8 weeks of storage.These results revealed that phenolic compounds, particularly anthocyanins, were involved in the formation of sediments in mulberry juice during storage.
基金supported by the National Natural Science Foundation of China(NSFC,Nos.21725304 and 11774120)the Chang Jiang Scholars Program of China(No.T2016051)the Fundamental Research Funds for the Central Universities
文摘Organic luminescent materials are very sensitive to external stimuli,such as pressure,temperature,and electric field.The luminescent properties of some organic luminescent materials significantly change under high pressure.Some materials may show luminescence discoloration,whereas some may exhibit luminescence enhancement.These properties have many potential applications in anticounterfeiting,force sensor,data recording and storage,and luminescent devices,thereby greatly attracting the attention of scientists.In this review,the progress of research on these materials at high pressure in recent years is summarized.
基金Project supported by the National Key Research and Development Program of China(Grant Nos.2021YFA1400203 and 2018YFA0305900)the National Natural Science Foundation of China(Grant Nos.52090024,11874175,12074139,12074138,11874176,and 12034009)+1 种基金the Strategic Priority Research Program of Chinese Academy of Sciences(Grant No.XDB33000000)Program for JLU Science and Technology Innovative Research Team(JLUSTIRT)。
文摘Flourishing rare earth superhydrides are a class of recently discovered materials that exhibit near-room-temperature superconductivity at high pressures,ushering in a new era of superconductivity research at high pressures.Yttrium superhydrides drew the most attention among these superhydrides due to their abundance of stoichiometries and excellent superconductivities.Here,we carried out a comprehensive study of yttrium superhydrides in a wide pressure range of 140 GPa-300 GPa.We successfully synthesized a series of superhydrides with the compositions of YH_(4),YH_(6),YH_(7),and YH_(9),and reported superconducting transition temperatures of 82 K at 167 GPa,218 K at 165 GPa,29 K at 162 GPa,and230 K at 300 GPa,respectively,as evidenced by sharp drops in resistance.The structure and superconductivity of YH_(4) were taken as a representative example and were also examined using x-ray diffraction measurements and the superconductivity suppression under external magnetic fields,respectively.Clathrate YH_(10),a candidate for room-temperature superconductor,was not synthesized within the study pressure and temperature ranges of up to 300 GPa and 2000 K.The current study established a detailed foundation for future research into room-temperature superconductors in polynary yttrium-based superhydrides.
基金the National Science Foundation of China(Grant Nos.21725304,11774125,and 21673100)the Chang Jiang Scholars Program of China(Grant No.T2016051)+3 种基金Changbai Mountain Scholars Program(Grant No.2013007)National Defense Science and Technology Key Laboratory Fund(Grant No.6142A0306010917)Jilin Provincial Science&Technology Development Program(Grant No.20190103044JH)Scientific Research Planning Project of the Education Department of Jilin Province(Grant No.JJKH20180118KJ)。
文摘SiO_(2)is the major mineral substance in the upper mantle of the earth.Therefore,studies of the silica-coated materials under high-pressure are essential to explore the physical and chemical properties of the upper mantle.The silica-confined CsPbBr_(3)nanocrystals(NCs)have recently attracted much attention because of the improved photoluminescence(PL)quantum yield,owing to the protection of silica shell.However,it remains considerable interest to further explore the relationship between optical properties and the structure of CsPbBr_(3)@SiO_(2)NCs.We systemically studied the structural and optical properties of the CsPbBr_(3)@SiO_(2)NCs under high pressure by using diamond anvil cell(DAC).The discontinuous changes of PL and absorption spectra occurred at~1.40 GPa.Synchrotron X-ray diffraction(XRD)studies of CsPbBr_(3)@SiO_(2)NCs under high pressure indicated an isostructural phase transformation at about 1.36 GPa,owing to the pressure-induced tilting of the Pb-Br octahedra.The isothermal bulk moduli for two phases are estimated about 60.0 GPa and 19.2 GPa by fitting the equation of state.Besides,the transition pressure point of CsPbBr_(3)@SiO_(2)NCs is slightly higher than that of pristine CsPbBr_(3)NCs,which attributed to the buffer effect of coating silica shell.The results indicate that silica shell is able to enhance the stabilization without changing the relationship between optical properties and structure of CsPbBr_(3)NCs.Our results were fascinated to model the rock metasomatism in the upper mantle and provided a new‘lithoprobe’for detecting the upper mantle.
基金the National Natural Science Foundation of China(Grant Nos.21725304,11774120,and 11904010)the Chang Jiang Scholars Program of China(Grant No.T2016051)+2 种基金Changbai Mountain Scholars Program(Grant No.2013007)the Science and Technology Innovation Program of Shanxi Province,China(Grant Nos.2020L0540 and 2020L0544)Scientific Research Fund of XinZhou Teachers University(Grant No.2019KY04).
文摘Mechanoresponsive luminescent(MRL)materials have drawn extensive concern due to their potential applications in mechanical sensors,memory chips,and security inks;especially these possessing high emission efficiency.In this work,we found trans-stilbene crystal exhibited two different pressure-induced emission enhancement(PIEE)behaviors at different pressure areas.The structural characterizations combined with density functional theory calculation indicate that the first emission enhancement was due to the decrease of nonradiation transition by the weaken of energy exchange process between atoms and lattice.And the second emission enhancement was attributed to the strengthen of C-H...C interactions from the non-planarization comformation.The results regarding the mechanoresponsive behavior of trans-stilbene offered a deep insight into PIEE from the structural point of view,which will facilitate the design of and search for high-performance MRL materials.
文摘The origin and history of the Earth are manifested as the evolutionary processes of chemistry and physics of its interiors,which can be recognized by deciphering the geochemical signals recorded in minerals and rocks.Deep interiors of the Earth and other rocky planets are under both extreme pressure and temperature,i.e.,approximately 360 gigapascals(GPa)and as high as 7000 K at the center of the Earth.
基金the Scientific and Technological Project of SGCC Headquarters entitled“Smart Distribution Network and Ubiquitous Power Internet of Things Integrated Development Collaborative Planning Technology Research”(5400-201956447A-0-0-00).
文摘The penetration rate of distributed generation is gradually increasing in the distribution system concerned.This is creating new problems and challenges in the planning and operation of the system.The intermittency and variability of power outputs from numerous distributed renewable generators could significantly jeopardize the secure operation of the distribution system.Therefore,it is necessary to assess the hosting capability for intermittent distributed generation by a distribution system considering operational constraints.This is the subject of this study.An assessment model considering the uncertainty of generation outputs from distributed generators is presented for this purpose.It involves different types of regulation or control functions using on-load tap-changers(OLTCs),reactive power compensation devices,energy storage systems,and the reactive power support of the distributed generators employed.A robust optimization model is then attained It is solved by Bertsimas robust counterpart through GUROBI solver.Finally,the feasibility and efficiency of the proposed method are demonstrated by a modified IEEE 33-bus distribution system.In addition,the effects of the aforementioned regulation or control functions on the enhancement of the hosting capability for intermittent distributed generation are examined.
基金supported by the Science and Technology Project of State Grid Zhejiang Electric Power CO.,LTD.(5211JY19000X)。
文摘Dear Editor,This letter aims to investigate the optimization problem where the decision variable is contained in a closed convex set.By combing the gradient decent-like method with the push-sum algorithm framework,we design the distributed iterative formulas under the condition that the considered graphs sequence is time-varying and unbalanced.
基金supported by the Major National Science and Technology Infrastructurethe National Natural Science Foundation of China(Grant No.12204254)the National Major Science Facility Synergetic Extreme Condition User Facility Achievement Transformation Platform Construction(Grant No.2021FGWCXNLJSKJ01)。
文摘Large-volume presses(LVPs)providing large volumes,liquid media,deformation capability,jump compression,and in situ measurements are in great demand for high-pressure research,particularly in the fields of geoscience,condensed matter physics,material science,chemistry,and biology.A high-pressure and high-temperature(HPHT)platform with different LVP subsystems,both solid-state and liquid environments,and nonequilibrium subsystems,has been constructed at the Synergetic Extreme Condition User Facility,Jilin University.This article describes the construction of the different subsystems and provides an overview of the capabilities and characteristics of the different HPHT subsystems.A large sample volume(1000 mm^(3))at 20 GPa is achieved through the use of a belt-type apparatus in the solid-state subsystem.HPHT conditions(1.8 GPa and 1000 K)are realized in the liquid subsystem through the use of a piston-cylinder-type LVP with optical diamond windows for in situ spectroscopic measurements.A maximum pressure jump to 10.2 GPa can be reached within 20 ms in the nonequilibrium subsystem with the use of an improved bladder-pressurization jump press.Some typical results obtained with different LVPs are briefly reviewed to illustrate the applications and advantages of these presses.In summary,the platform described here has the potential to contribute greatly to high-pressure research and to innovations in high-pressure technology.
基金supported by the National Natural Science Foundation of China(52122308,21905253,51973200,52203244,21725304)the Natural Science Foundation of Henan Province(202300410372)the China Postdoctoral Science Foundation(2022M712868).
文摘Solid-state fluorescent multi-color carbon dots(SFM-CDs),prepared using the same precursor(s)without the need for dispersion in a solid matrix,are highly demanded for a wide range of applications.Herein,we report a microwave-assisted strategy for the prepara-tion of SFM-CDs with blue,yellow and red emissions within 5 min from the same precursors.The as-prepared B-CDs,Y-CDs,and R-CDs possessed bright fluorescence at 425 nm,550 nm,and 640 nm,and photoluminescence quantum yields(PLQYs)of 54.68%,17.93%,and 2.88%,respectively.The structure of SFM-CDs consisted of 5-oxo-3,5-dihydro-2H-thiazolo[3,2-a]pyridine-7-carboxylic acid(TPCA)immobilized on the surface of a carbon core,with the size of the carbon core and degree of disulfide crosslinking between CDs both increasing on going from the B-CDs to the R-CDs,as verified by mechanochromic experiments.The excellent solid-state fluorescence performance of the SFM-CDs allowed their utilization as the fluorescent converter layer in multi-color LEDs and white LEDs with a high color rendering index.
文摘As an extensively used chemical product,cyclic carbonate was generally synthesized by transesterification,or the cycloaddition of epoxides,diols with CO2.To reduce the production costs and expand the raw materials,alkenyl and alkynyl substrates have caused much attention in the synthesis of cyclic carbonates,such as olefins,allyl alcohols and propargylic alcohols.Based on the alkenyl substrate,the synthetic process involves a continuous reaction of oxidative carboxylation,with epoxide or halohydrin as an intermediate usually.Therefore,peroxides and nucleophiles （halogens or organic bases） are often necessary in the conversion.Using propargylic alcohols to produce a-alkylidene cyclic carbonates,noble metal catalysts play crucial roles in alkynyl activation,and organic bases are considered to assist the intramolecular and intermolecular proton transfer and combine CO2 molecular.As the carboxyl sources in products,inorganic carbonates and organic carboxylic acids also have some applications instead of CO2.In this review,we summarized the synthetic routes of cyclic carbonates from alkenyl and alkynyl substrates in the aspect of catalyst,mechanism and the development tendency.
基金supported by the National Natural Science Foundation of China(21725304,21673100,91227202,11774120,11774125)the Chang Jiang Scholars Program of China(T2016051)+3 种基金Changbai Mountain Scholars Program(2013007)Program for Innovative Research Team(in Science and Technology)in University of Jilin Province and Graduate Innovation Fund of Jilin University(2017050)ADXRD experiments were performed at Beijing Synchrotron Radiation Facility(4W2 beamline)which is supported by Chinese Academy of Sciences(KJCX2-SW-N20,KJCX2-SW-N03)
文摘Pressure, as a thermodynamic parameter, provides an appropriate method to detect weak intermolecular interactions. The C–H···H–B dihydrogen bond is so weak that the experimental evidence of this interaction is still limited. A combination of in situ high pressure Raman spectra and angle-dispersive X-ray diffraction(ADXRD) experiments was utilized to explore the dihydrogen bonds in dimethylamine borane(DMAB). Both Raman and ADXRD measurements suggested that the crystal structure of DMAB is stable in the pressure region from 1 atm(1 atm=1.01325×10~5 Pa) to 0.54 GPa. The red shift of CH stretching and CH_3 distortion modes gave strong evidence for the existence of C–H···H–B dihydrogen bonds. Further analysis of Raman spectra and Hirshfeld surface confirmed our proposal. This work provided a deeper understanding of dihydrogen bonds.And we wish that high pressure could be applied to identify other unconfirmed hydrogen or dihydrogen bond.
基金supported by the National Key R&D Program of China(2023YFA1406200)the National Science Foundation of China(12174144 and 12304014)+2 种基金the Jilin Provincial Science&Technology Development Program(20220101002JC)the Graduate Innovation Fund of Jilin University(2024CX201)the Fundamental Research Funds for the Central Universities.
文摘The interaction between organic and inorganic components in metal hybrid perovskites fundamentally determines the intrinsic optoelectronic performance.However,the underlying interaction sites have still remained elusive,especially for those non-hydrogen-bonded hybrid perovskites,thus largely impeding materials precise design with targeted properties.Herein,high pressure is utilized to elucidate the interaction mechanism between organic and inorganic components in the as-synthesized one-dimensional hybrid metal halide(DBU)PbBr_(3)(DBU=1,8-diazabicyclo[5.4.0]undec-7-ene).The interaction sites are identified to be the N from DBU and the Br from inorganic framework by the indicative of enhanced Raman mode under high pressure.The change in interaction strength is indeed derived from the pressure modulation on both distance and spatial arrangement of the nearest Br and N,rather than traditional hydrogen-bonding effect.Furthermore,the enhanced interaction increased charge transfer,resulting in a cyan emission with photoluminescence quantum yields(PLQYs)of 86.6%.The enhanced cyan emission is particularly important for underwater communication due to the much less attenuation in water than at other wavelength emissions.This study provides deep insights into the underlying photophysical mechanism of non-hydrogen-bonded hybrid metal halides and is expected to impart innovative construction with superior performance.
基金supported by the National Key R&D Program of China(grant no.2023YFA1406200)the Jilin Provincial Science&Technology Development Program,China(grant no.20220101002JC)+2 种基金the National Science Foundation of China(grant no.12174144)Young Elite Scientists Sponsorship Program of the China Association for Science and Technology(CAST,grant no.2022QNRC001)the Fundamental Research Funds for the Central Universities.This work was mainly performed at BL15U1 at the Shanghai Synchrotron Radiation Facility(SSRF).
文摘Chalcogenide quantum dots(QDs)are established as promising materials for white-light-emitting applications because of their wide surface defect emission.However,the limited understanding of the origin of defect emission poses challenges in attaining efficient white-light emission.Herein,we sought to introduce high pressure to strengthen the interaction between different types of ligands and QDs,as well as enable in situ observation of surface trap passivation that contributes to emission control.Under pressure,both defect emission and band-edge emission in the CdS QDs could be selectively enhanced by more than an order of magnitude through treatment with X-type and Z-type ligands,respectively.Our findings identified that surface hole traps predominantly contributed to defect emission,whereas nonradiative recombination was primarily associated with surface electron traps.Our goal was to service ambient science through high-pressure research.Thus,based on this proposed mechanism,an energy-saving“neutral”white light with a human-eyefriendly color rendering index of 86 was achieved by tuning the defect emission through further elimination of surface Cd sites.This study endowed high pressure as an efficient tool to elucidate the defect origin of chalcogenide QDs under ambient conditions,paving the way for precise control over white-light emission through materials design application in solid-state lighting.
基金supported by the National Key R&D Program of China(grant nos.2022YFA1402300,2023YFA1406200,and 2019YFA0708502)the National Science Foundation of China(grant nos.22131006,12174144,12474009,22022101,and 22090041).
文摘The chemical synthesis of functional materials is inseparable from national defense,medical treatment,national economy,and people’s livelihood.Traditional organic and inorganic materials are approaching their performance limit.Therefore,the design and exploitation of novel functional materials are imminent and of significance for sustainable development.This review outlines the current progress and future prospects of chemical synthesis driven by high pressure,including organic and inorganic synthesis,as well as high-pressure phase retention.Based on the latest works,the basic mechanism of high-pressure chemical synthesis and three potential strategies for high-pressure phase harvesting are revealed.Finally,the challenge and outlook of high-pressureguided chemical synthesis are summarized.We sincerely hope that this review will provide guidance for designing high-performance materials by expanding the paths of chemical synthesis,thus greatly exploiting the existing materials world with newly emerging and enhanced functionalities.
基金supported by the National Natural Science Foundation of China(22122504,22235006)Foundation of Hubei Scientific Committee(2022BAA015 and 2022EHB010).
文摘Conformational flexibility is essential to the stimuli-responsive property of organic materials,but achieving the reversible molecular transformation is still challenging in functional materials for the high energy barriers and restriction by intermolecular interactions.Herein,through the incorporation of various steric hindrances into phenothiazine derivatives with different positions and quantities to tune the molecular conformations by adjustable repulsive forces,the folded angles gradually changed from 180°to 90°in 17 compounds.When the angle located at 112°with moderated steric effect,dynamic and reversible transformation of conformations under mechanical force has been achieved for the low energy barriers and mutually regulated molecular motions,resulting in both selfrecoverable and stimuli-responsive phosphorescence properties for the first time.It opened up a new way to realize the self-recovery property of organic materials,which can facilitate the multi-functional property of smart materials with the opened avenue for other fields with inspiration.
