Developing luminescent metal-organic frameworks(MOFs) capable of high-efficiency Fe^(3+)sensing has aroused great attraction in the fields of biology,chemistry,etc.However,previous solvothermal methods are limited by ...Developing luminescent metal-organic frameworks(MOFs) capable of high-efficiency Fe^(3+)sensing has aroused great attraction in the fields of biology,chemistry,etc.However,previous solvothermal methods are limited by organic solvent usage,time consuming,high pressure,and high-energy consumption.Herein,we propose the waste-toMOF strategy towards the scale-up production of La-MOF nanoparticles through the ball milling of recycled poly(-ethylene terephthalate)(PET) bottles and La(NO_(3))_(3)·_(6)H_(2)O.PET goes on alkaline hydrolysis to form 1,4-benzenedicarboxylic acid sodium salt(Na_(2)BDC) and ethylene glycol by ball milling.Subsequently,BDC reacts with La^(3+)to form La-MOF.The as-prepared La-MOF crystal nanoparticles possess a rod-like morphology with the size of few hundred nanometers.Additionally,La-MOF nanoparticles display high selectivity and sensitivity for Fe^(3+)detection.The quenching constant and limit of detection are 5.29×10^(3)(mol·L^(-1))^(-1) and 0.147 μmol·L^(-1),respectively,thus surpassing many advanced Fe^(3+) sensors.According to the result of density functional theory,the high Fe^(3+) detection performance of La-MOF is related to the complexing of Fe^(3+)with La-MOF,which leads to the gradual dissociation of the coordination bond between terephthalic acid and La^(3+).It is anticipated that the mechanochemistry milling-based wasteto-MOF strategy provides a new platform for the massive production of functional MOFs in a green manner.展开更多
Porous metal–organic frameworks(MOFs) have been recently discovered to be efficient catalysts for energy applications and green technologies. Here, we report on a scalable catalytic platform using Cu–based MOFs for ...Porous metal–organic frameworks(MOFs) have been recently discovered to be efficient catalysts for energy applications and green technologies. Here, we report on a scalable catalytic platform using Cu–based MOFs for electrocatalytic alkaline hydrogen evolution reaction. First, the solvothermal synthesis of Cu–BTC MOFs(BTC = 1,3,5–benzenetricarboxylate) at 85 ℃ and a 1:60 ligand–to–solvent ratio allowed for minimizing the chemical consumption. Second, the obtained platform demonstrated enhanced electrochemical performance compared with commercially available Cu–based MOFs, with a potential of –230 versus –232 eV, logarithm of the current density of –3.6 versus –4.2 cm2, and electrochemical surface area of 75 versus 25 cm2per cm2of geometric area, respectively. Morphological and Raman analyses also revealed that the high concentration of defects in the obtained submicron Cu–BTC MOFs can contribute to their improved catalytic performance. Thus, our findings pave the way to the low–cost synthesis of energy–efficient MOF–based catalysts for hydrogen production.展开更多
As activated hepatic stellate cells(aHSCs)play a central role in fibrogenesis,they have become key target cells for antifibrotic treatment.Nevertheless,the therapeutic efficiency is constrained by the exosomes they se...As activated hepatic stellate cells(aHSCs)play a central role in fibrogenesis,they have become key target cells for antifibrotic treatment.Nevertheless,the therapeutic efficiency is constrained by the exosomes they secrete,which are linked to energy metabolism and continuously stimulate the activation of neighboring quiescent hepatic stellate cells(qHSCs).Herein,an intercellular communication interference strategy is designed utilizing paeoniflorin(PF)loaded and hyaluronic acid(HA)coated copper-doped ZIF-8(PF@HA-Cu/ZIF-8,PF@HCZ)to reduce energy-related exosome secretion from aHSCs,thus preserving neighboring qHSCs in a quiescent state.Simultaneously,the released copper and zinc ions disrupt key enzymes involved in glycolysis to reduce bioenergy synthesis in aHSCs,thereby promoting the reversion of aHSCs to a quiescent state and further decreasing exosome secretion.Therefore,PF@HCZ can effectively sustain both aHSCs and qHSCs in a metabolically dormant state to ultimately alleviate liver fibrosis.The study provides an enlightening strategy for interrupting exosome-mediated intercellular communication and remodeling the energy metabolic status of HSCs with boosted antifibrogenic activity.展开更多
Optical clearing of invertebrates,the number of species of which is 20 times greater than that of vertebrates,is of fundamental and applied interest for neuroscience in general.Herein,the optical clearing of invertebr...Optical clearing of invertebrates,the number of species of which is 20 times greater than that of vertebrates,is of fundamental and applied interest for neuroscience in general.Herein,the optical clearing of invertebrates to identify their morphology and neurostructure remains unrealized as of yet.Here,we report on fast(from a few seconds to minutes)and uniform whole-body optical clearing of invertebrates(bivalves,nemertines,annelids,and anomura)of any age and thickness(up to 2 cm)possessing complicated structures and integuments.We developed the protocol unifying dimethyl sulfoxide(DMSO)-based immunostaining of the animals followed by their optical clearing with benzyl alcohol/benzyl benzoate(BABB).Confocal microspectroscopy revealed that the protocol provides an increase of the fluorescence signal by 2 orders of magnitude and decrease of the light scattering by 2 orders of magnitude,thereby accelerating the confocal bioimaging of the whole body.Moreover,by tracking the optical clearing over time with 0.3 s resolution,we revealed that the clearing process is described by the Gompertz growth function,allowing us to determine the physical mechanism of the clearing and its optical parameters.Thereby,we were able to identify in detail and to describe previously unknown neurostructures of different invertebrate animals,paving the way to discovery in neuroscience.展开更多
基金financially supported by the National Natural Science Foundation of China (Nos.52373099,51903099 and 22102059)the 100 Talents Program of Hubei Provincial Government,Huazhong University of Science and Technology (Nos.3004013134 and 2021XXJS036)+4 种基金the Innovation and Talent Recruitment Base of New Energy Chemistry and Device (No.B21003)the Opening Project (No.KFKT2304) of the Key Laboratory of Polymer Processing Engineering (South China University of Technology)Ministry of Education,the Open Research Fund of Key Laboratory of Material Chemistry for Energy Conversion and Storage(HUST)Ministry of Education (Nos.2022JYBKF01 and 2022JYBKF05)the National Innovation and Entrepreneurship Training Program for College Students (Nos.202310487109 and202310487110)。
文摘Developing luminescent metal-organic frameworks(MOFs) capable of high-efficiency Fe^(3+)sensing has aroused great attraction in the fields of biology,chemistry,etc.However,previous solvothermal methods are limited by organic solvent usage,time consuming,high pressure,and high-energy consumption.Herein,we propose the waste-toMOF strategy towards the scale-up production of La-MOF nanoparticles through the ball milling of recycled poly(-ethylene terephthalate)(PET) bottles and La(NO_(3))_(3)·_(6)H_(2)O.PET goes on alkaline hydrolysis to form 1,4-benzenedicarboxylic acid sodium salt(Na_(2)BDC) and ethylene glycol by ball milling.Subsequently,BDC reacts with La^(3+)to form La-MOF.The as-prepared La-MOF crystal nanoparticles possess a rod-like morphology with the size of few hundred nanometers.Additionally,La-MOF nanoparticles display high selectivity and sensitivity for Fe^(3+)detection.The quenching constant and limit of detection are 5.29×10^(3)(mol·L^(-1))^(-1) and 0.147 μmol·L^(-1),respectively,thus surpassing many advanced Fe^(3+) sensors.According to the result of density functional theory,the high Fe^(3+) detection performance of La-MOF is related to the complexing of Fe^(3+)with La-MOF,which leads to the gradual dissociation of the coordination bond between terephthalic acid and La^(3+).It is anticipated that the mechanochemistry milling-based wasteto-MOF strategy provides a new platform for the massive production of functional MOFs in a green manner.
基金This work was supported by Russian Science Foundation(22-73-10069“Design and application of fl exible Metal organic frameworks for photonics devices,”the chemical part and structural analysis of developed MOFs)The of stability MOFs was conducted under the fi nancial support of the Ministry of Science and Higher Education of the Russian Federation as part of the World-Class Research Center program:Advanced Digital Technologies(contract No.075-15-2022-311 dated 20.04.2022)The authors thank the Engineering Centre of Saint Petersburg State Institute of Technology for PXRD analysis.
文摘Porous metal–organic frameworks(MOFs) have been recently discovered to be efficient catalysts for energy applications and green technologies. Here, we report on a scalable catalytic platform using Cu–based MOFs for electrocatalytic alkaline hydrogen evolution reaction. First, the solvothermal synthesis of Cu–BTC MOFs(BTC = 1,3,5–benzenetricarboxylate) at 85 ℃ and a 1:60 ligand–to–solvent ratio allowed for minimizing the chemical consumption. Second, the obtained platform demonstrated enhanced electrochemical performance compared with commercially available Cu–based MOFs, with a potential of –230 versus –232 eV, logarithm of the current density of –3.6 versus –4.2 cm2, and electrochemical surface area of 75 versus 25 cm2per cm2of geometric area, respectively. Morphological and Raman analyses also revealed that the high concentration of defects in the obtained submicron Cu–BTC MOFs can contribute to their improved catalytic performance. Thus, our findings pave the way to the low–cost synthesis of energy–efficient MOF–based catalysts for hydrogen production.
基金supported by the National Natural Science of China(82273873 and 31971106,China)the Youth Science and Technology Talent Program by Tianjin(QN20230215,China)+2 种基金the National Key Research and Development Program of China(2020YFC1512304 and 2020YFC1512301,China)the Tianjin Natural Science Foundation(24JCZDJC01110 China)the Major Special Projects(0402080005,China).
文摘As activated hepatic stellate cells(aHSCs)play a central role in fibrogenesis,they have become key target cells for antifibrotic treatment.Nevertheless,the therapeutic efficiency is constrained by the exosomes they secrete,which are linked to energy metabolism and continuously stimulate the activation of neighboring quiescent hepatic stellate cells(qHSCs).Herein,an intercellular communication interference strategy is designed utilizing paeoniflorin(PF)loaded and hyaluronic acid(HA)coated copper-doped ZIF-8(PF@HA-Cu/ZIF-8,PF@HCZ)to reduce energy-related exosome secretion from aHSCs,thus preserving neighboring qHSCs in a quiescent state.Simultaneously,the released copper and zinc ions disrupt key enzymes involved in glycolysis to reduce bioenergy synthesis in aHSCs,thereby promoting the reversion of aHSCs to a quiescent state and further decreasing exosome secretion.Therefore,PF@HCZ can effectively sustain both aHSCs and qHSCs in a metabolically dormant state to ultimately alleviate liver fibrosis.The study provides an enlightening strategy for interrupting exosome-mediated intercellular communication and remodeling the energy metabolic status of HSCs with boosted antifibrogenic activity.
基金supported by the Russian Science Foundation(Grant No.21-74-30004(clearance)and 22-14-00245(immunostainings)).
文摘Optical clearing of invertebrates,the number of species of which is 20 times greater than that of vertebrates,is of fundamental and applied interest for neuroscience in general.Herein,the optical clearing of invertebrates to identify their morphology and neurostructure remains unrealized as of yet.Here,we report on fast(from a few seconds to minutes)and uniform whole-body optical clearing of invertebrates(bivalves,nemertines,annelids,and anomura)of any age and thickness(up to 2 cm)possessing complicated structures and integuments.We developed the protocol unifying dimethyl sulfoxide(DMSO)-based immunostaining of the animals followed by their optical clearing with benzyl alcohol/benzyl benzoate(BABB).Confocal microspectroscopy revealed that the protocol provides an increase of the fluorescence signal by 2 orders of magnitude and decrease of the light scattering by 2 orders of magnitude,thereby accelerating the confocal bioimaging of the whole body.Moreover,by tracking the optical clearing over time with 0.3 s resolution,we revealed that the clearing process is described by the Gompertz growth function,allowing us to determine the physical mechanism of the clearing and its optical parameters.Thereby,we were able to identify in detail and to describe previously unknown neurostructures of different invertebrate animals,paving the way to discovery in neuroscience.
