Achieving increasingly finely targeted drug delivery to organs,tissues,cells,and even to intracellular biomacromolecules is one of the core goals of nanomedicines.As the delivery destination is refined to cellular and...Achieving increasingly finely targeted drug delivery to organs,tissues,cells,and even to intracellular biomacromolecules is one of the core goals of nanomedicines.As the delivery destination is refined to cellular and subcellular targets,it is essential to explore the delivery of nanomedicines at the molecular level.However,due to the lack of technical methods,the molecular mechanism of the intracellular delivery of nanomedicines remains unclear to date.Here,we develop an enzyme-induced proximity labeling technology in nanoparticles(nano-EPL)for the real-time monitoring of proteins that interact with intracellular nanomedicines.Poly(lactic-co-glycolic acid)nanoparticles coupled with horseradish peroxidase(HRP)were fabricated as a model(HRP(+)-PNPs)to evaluate the molecular mechanism of nano delivery in macrophages.By adding the labeling probe biotin-phenol and the catalytic substrate H_(2)O_(2)at different time points in cellular delivery,nano-EPL technology was validated for the real-time in situ labeling of proteins interacting with nanoparticles.Nano-EPL achieves the dynamic molecular profiling of 740 proteins to map the intracellular delivery of HRP(+)-PNPs in macrophages over time.Based on dynamic clustering analysis of these proteins,we further discovered that different organelles,including endosomes,lysosomes,the endoplasmic reticulum,and the Golgi apparatus,are involved in delivery with distinct participation timelines.More importantly,the engagement of these organelles differentially affects the drug delivery efficiency,reflecting the spatial–temporal heterogeneity of nano delivery in cells.In summary,these findings highlight a significant methodological advance toward understanding the molecular mechanisms involved in the intracellular delivery of nanomedicines.展开更多
The degradation and mineralization of aniline(AN) using ozone combined with Fenton reagent(O_3/Fenton) in a rotating packed bed(RPB) was proposed in this study, and the process(RPB-O_3/Fenton) was compared with conven...The degradation and mineralization of aniline(AN) using ozone combined with Fenton reagent(O_3/Fenton) in a rotating packed bed(RPB) was proposed in this study, and the process(RPB-O_3/Fenton) was compared with conventional O_3/Fenton in a stirred tank reactor(STR-O_3/Fenton) or single ozonation in an RPB(RPB-O_3). Effects of high gravity factor, H_2O_2 dosage, H_2O_2 dosing method and initial p H on the AN mineralization efficiency were investigated in the RPB-O_3/Fenton process. In addition, the behavior of Fe(II) was monitored at different H2 O2 dosing methods and p H values. Finally, the optimal operation conditions were determined with high gravity factor of100, initial pH of 5, Fe(II) concentration of 0.8 mmol·L^(-1) and H_2O_2 dosage of 2.5 ml. Under these conditions, for aniline wastewater at the volume of 1 L and concentration of 200 mg·L^(-1), a fast and thorough decay of AN was conducted in 10 min, and the TOC removal efficiency reached 89% in 60 min. The main intermediates of p-benzoquinone, nitrobenzene, maleic acid and oxalic acid were identified by liquid chromatography/mass spectroscopy(LC/MS), and the degradation pathways of AN in RPB-O_3/Fenton system were proposed based on experimental evidence. It could be envisioned that high-gravity technology combined with O_3/Fenton processes would be promising in the rapid and efficient mineralization of wastewater.展开更多
The hydrogen evolution reaction(HER)of molybdenum disulfide(MoS_(2))is limited in alkaline and acid solution because the active sites are on the finite edge with extended basal plane remaining inert.Herein,we activate...The hydrogen evolution reaction(HER)of molybdenum disulfide(MoS_(2))is limited in alkaline and acid solution because the active sites are on the finite edge with extended basal plane remaining inert.Herein,we activated the interfacial S sites by coupling with Ru nanoparticles on the inert basal plane of MoS_(2)nanosheets.The density functional theory(DFT)calculation and experimental results show that the interfacial S electronic structure was modulated.And the results of∆G H*demonstrate that the adsorption of H on the MoS_(2)was also optimized.With the advantage of interfacial S sites activation,the Ru-MoS_(2)needs only overpotential of 110 and 98 mV to achieve 10 mA·cm^(–2)in both 0.5 M H_(2)SO_(4)and ^(1) M KOH solution,respectively.This strategy paves a new way for activating the basal plane of other transition metal sulfide electrocatalysts for improving the HER performance.展开更多
The electrocatalytic hydrogen evolution reaction(HER)is one of the most promising ways for low-cost hydrogen production in the future.In this work,hetero S atoms were introduced into the MoO2 to enhance the catalytic ...The electrocatalytic hydrogen evolution reaction(HER)is one of the most promising ways for low-cost hydrogen production in the future.In this work,hetero S atoms were introduced into the MoO2 to enhance the catalytic activity by simultaneously adjusting electron structure,engineering lattice defect,and increasing oxygen vacancies.And the S doped MoO2 nanosheets with proper S doping amount show the enhanced performance for HER.The optimized catalyst shows a small onset overpotential as low as 120 mV,a low overpotential of 176 mV at the current density of 10 mA/cm^2 which is decreased 166 mV compared to that of the pristine MoO2 nanosheets,a low Tafel slope of 57 mV/decade,and a high turnover frequency of 0.13 H2/s per active site at 150 mV.This finding proposes an effective strategy to prepare nonprecious metal oxide catalyst for enhancing HER performance by rationally doping hetero atoms.展开更多
Neutrophils are traditionally considered as first responders to infection and provide antimicrobial host defense. However, recent advances indicate that neutrophils are also critically involved in the modulation of ho...Neutrophils are traditionally considered as first responders to infection and provide antimicrobial host defense. However, recent advances indicate that neutrophils are also critically involved in the modulation of host immune environments by dynamically adopting distinct functional states. Functionally diverse neutrophil subsets are increasingly recognized as critical components mediating host pathophysiology. Despite its emerging significance, molecular mechanisms as well as functional relevance of dynamically programmed neutrophils remain to be better defined. The increasing complexity of neutrophil functions may require integrative studies that address programming dynamics of neutrophils and their pathophysiological relevance. This review aims to provide an update on the emerging topics of neutrophil programming dynamics as well as their functional relevance in diseases.展开更多
Implant-related infection is one of the most catastrophic complications after surgery,since it may trigger osteomyelitis and necessitate reoperation,increasing the pain suffered by and the burden placed on the patient...Implant-related infection is one of the most catastrophic complications after surgery,since it may trigger osteomyelitis and necessitate reoperation,increasing the pain suffered by and the burden placed on the patient.Producing a new alloy with an antibacterial effect for use as a biomedical material is an urgent requirement.In this article,Ti-6 Al-4 V-5 Cu was synthesized under two different heat treatment schemes(solution temperatures of 850℃and 950℃).Through comprehensive observation of the microstructure,phase,copper ion release,biocompatibility,corrosion resistance and antibacterial effect in vitro and in vivo,it was determined that cell viability and corrosion resistance of Ti-6 Al-4 V-5 Cu was better than Ti-6 Al-4 V.More importantly,the obtained alloy,especially samples treated at 850℃,showed prominent antibacterial ability.Meanwhile,we also found that the main antibacterial mechanism of the alloy was contact sterilization via the extensive precipitation of Ti_(2)Cu instead of Cu ion release,and the content,surface area of Ti_(2)Cu could affect the antibacterial effect.These findings provide a very promising scheme by which to balance the biocompatibility and antibacterial effect of Ti-based,Cu-bearing alloys,which could improve their performance in orthopedic and dental applications.展开更多
基金supported by Natural Science Foundation of Beijing Municipality(L212013)National Key Research and Development Program of China(No.2022YFA1206104)+2 种基金AI+Health Collaborative Innovation Cultivation Project(Z211100003521002)National Natural Science Foundation of China(81971718,82073786,81872809,U20A20412,81821004)Beijing Natural Science Foundation(7222020).
文摘Achieving increasingly finely targeted drug delivery to organs,tissues,cells,and even to intracellular biomacromolecules is one of the core goals of nanomedicines.As the delivery destination is refined to cellular and subcellular targets,it is essential to explore the delivery of nanomedicines at the molecular level.However,due to the lack of technical methods,the molecular mechanism of the intracellular delivery of nanomedicines remains unclear to date.Here,we develop an enzyme-induced proximity labeling technology in nanoparticles(nano-EPL)for the real-time monitoring of proteins that interact with intracellular nanomedicines.Poly(lactic-co-glycolic acid)nanoparticles coupled with horseradish peroxidase(HRP)were fabricated as a model(HRP(+)-PNPs)to evaluate the molecular mechanism of nano delivery in macrophages.By adding the labeling probe biotin-phenol and the catalytic substrate H_(2)O_(2)at different time points in cellular delivery,nano-EPL technology was validated for the real-time in situ labeling of proteins interacting with nanoparticles.Nano-EPL achieves the dynamic molecular profiling of 740 proteins to map the intracellular delivery of HRP(+)-PNPs in macrophages over time.Based on dynamic clustering analysis of these proteins,we further discovered that different organelles,including endosomes,lysosomes,the endoplasmic reticulum,and the Golgi apparatus,are involved in delivery with distinct participation timelines.More importantly,the engagement of these organelles differentially affects the drug delivery efficiency,reflecting the spatial–temporal heterogeneity of nano delivery in cells.In summary,these findings highlight a significant methodological advance toward understanding the molecular mechanisms involved in the intracellular delivery of nanomedicines.
基金Supported by the National Natural Science Foundations of China(U1610106)Shanxi Excellent Talent Science and Technology Innovation Project(201705D211011)+1 种基金Specialized Research Fund for Sanjin Scholars Program of Shanxi ProvinceNorth University of China Fund for Distinguished Young Scholars
文摘The degradation and mineralization of aniline(AN) using ozone combined with Fenton reagent(O_3/Fenton) in a rotating packed bed(RPB) was proposed in this study, and the process(RPB-O_3/Fenton) was compared with conventional O_3/Fenton in a stirred tank reactor(STR-O_3/Fenton) or single ozonation in an RPB(RPB-O_3). Effects of high gravity factor, H_2O_2 dosage, H_2O_2 dosing method and initial p H on the AN mineralization efficiency were investigated in the RPB-O_3/Fenton process. In addition, the behavior of Fe(II) was monitored at different H2 O2 dosing methods and p H values. Finally, the optimal operation conditions were determined with high gravity factor of100, initial pH of 5, Fe(II) concentration of 0.8 mmol·L^(-1) and H_2O_2 dosage of 2.5 ml. Under these conditions, for aniline wastewater at the volume of 1 L and concentration of 200 mg·L^(-1), a fast and thorough decay of AN was conducted in 10 min, and the TOC removal efficiency reached 89% in 60 min. The main intermediates of p-benzoquinone, nitrobenzene, maleic acid and oxalic acid were identified by liquid chromatography/mass spectroscopy(LC/MS), and the degradation pathways of AN in RPB-O_3/Fenton system were proposed based on experimental evidence. It could be envisioned that high-gravity technology combined with O_3/Fenton processes would be promising in the rapid and efficient mineralization of wastewater.
基金the National Natural Science Foundation of China(Nos.51871078 and 52071119)Heilongjiang Science Foundation(No.E201808).
文摘The hydrogen evolution reaction(HER)of molybdenum disulfide(MoS_(2))is limited in alkaline and acid solution because the active sites are on the finite edge with extended basal plane remaining inert.Herein,we activated the interfacial S sites by coupling with Ru nanoparticles on the inert basal plane of MoS_(2)nanosheets.The density functional theory(DFT)calculation and experimental results show that the interfacial S electronic structure was modulated.And the results of∆G H*demonstrate that the adsorption of H on the MoS_(2)was also optimized.With the advantage of interfacial S sites activation,the Ru-MoS_(2)needs only overpotential of 110 and 98 mV to achieve 10 mA·cm^(–2)in both 0.5 M H_(2)SO_(4)and ^(1) M KOH solution,respectively.This strategy paves a new way for activating the basal plane of other transition metal sulfide electrocatalysts for improving the HER performance.
基金supported by the Research Project of the Key Laboratory of Functional Materials Physics and Chemistry of the Ministry of Education(2017005)the National Natural Science Foundation of China(Nos.51571072 and 51871078)Heilongjiang Science Foundation(No.E2018028).
文摘The electrocatalytic hydrogen evolution reaction(HER)is one of the most promising ways for low-cost hydrogen production in the future.In this work,hetero S atoms were introduced into the MoO2 to enhance the catalytic activity by simultaneously adjusting electron structure,engineering lattice defect,and increasing oxygen vacancies.And the S doped MoO2 nanosheets with proper S doping amount show the enhanced performance for HER.The optimized catalyst shows a small onset overpotential as low as 120 mV,a low overpotential of 176 mV at the current density of 10 mA/cm^2 which is decreased 166 mV compared to that of the pristine MoO2 nanosheets,a low Tafel slope of 57 mV/decade,and a high turnover frequency of 0.13 H2/s per active site at 150 mV.This finding proposes an effective strategy to prepare nonprecious metal oxide catalyst for enhancing HER performance by rationally doping hetero atoms.
文摘Neutrophils are traditionally considered as first responders to infection and provide antimicrobial host defense. However, recent advances indicate that neutrophils are also critically involved in the modulation of host immune environments by dynamically adopting distinct functional states. Functionally diverse neutrophil subsets are increasingly recognized as critical components mediating host pathophysiology. Despite its emerging significance, molecular mechanisms as well as functional relevance of dynamically programmed neutrophils remain to be better defined. The increasing complexity of neutrophil functions may require integrative studies that address programming dynamics of neutrophils and their pathophysiological relevance. This review aims to provide an update on the emerging topics of neutrophil programming dynamics as well as their functional relevance in diseases.
基金financially supported by the Harbin Medical University Graduate Research Innovation Fund[201801140]。
文摘Implant-related infection is one of the most catastrophic complications after surgery,since it may trigger osteomyelitis and necessitate reoperation,increasing the pain suffered by and the burden placed on the patient.Producing a new alloy with an antibacterial effect for use as a biomedical material is an urgent requirement.In this article,Ti-6 Al-4 V-5 Cu was synthesized under two different heat treatment schemes(solution temperatures of 850℃and 950℃).Through comprehensive observation of the microstructure,phase,copper ion release,biocompatibility,corrosion resistance and antibacterial effect in vitro and in vivo,it was determined that cell viability and corrosion resistance of Ti-6 Al-4 V-5 Cu was better than Ti-6 Al-4 V.More importantly,the obtained alloy,especially samples treated at 850℃,showed prominent antibacterial ability.Meanwhile,we also found that the main antibacterial mechanism of the alloy was contact sterilization via the extensive precipitation of Ti_(2)Cu instead of Cu ion release,and the content,surface area of Ti_(2)Cu could affect the antibacterial effect.These findings provide a very promising scheme by which to balance the biocompatibility and antibacterial effect of Ti-based,Cu-bearing alloys,which could improve their performance in orthopedic and dental applications.
