Thermodynamic/dynamic modeling of liquid immiscibility in silicates is seriously hindered due to lack of in situ investigation on the structural evolution of the melt.In this work,atomic-scale structural evolution of ...Thermodynamic/dynamic modeling of liquid immiscibility in silicates is seriously hindered due to lack of in situ investigation on the structural evolution of the melt.In this work,atomic-scale structural evolution of a classic binary silicate immiscible system,SiO2–TiO2,is tracked by in situ high energy X-ray diffraction(HE-XRD).It is found that both the configuration of[SiO]and the polymerization between them are closely coupled with embedment and extraction of the metallic cations(Ti^4+).[SiO]monomer goes through deficit-oxygen and excess-polymerization before liquid–liquid separation and enables self-healing after liquid–liquid separation,which challenges the traditional cognition that[SiO4]monomer is immutable.Ti4+cations with tetrahedral oxygen-coordination first participate in the network construction before liquid separation.The four-fold Ti–O bond is broken during liquid separation,which may facilitate the movement of Ti4+across the Si–O network to form TiO2-rich nodules.The structural features of nodules were also investigated and they were found highly analogous to that of molten TiO2,which implies a parallel crystallization behavior in the two circumstances.Our results shed light on the structural evolution scenario in liquid immiscibility at atomic scale,which will contribute to constructing a complete thermodynamic/dynamic framework describing the silicate liquid immiscibility systems beyond current models.展开更多
Background:Silica nanoparticles(SiNPs),commonly utilized in industrial and biomedical fields,are known to provoke pulmonary inflammation by elevating cyclooxygenase-2(COX-2)levels in human pulmonary alveolar epithelia...Background:Silica nanoparticles(SiNPs),commonly utilized in industrial and biomedical fields,are known to provoke pulmonary inflammation by elevating cyclooxygenase-2(COX-2)levels in human pulmonary alveolar epithelial cells(HPAEpiCs).Salvianolic acid A(SAA),a water-soluble polyphenol extracted from Salvia miltiorrhiza(Danshen),possesses well-documented antioxidant and anti-inflammatory activities.Nevertheless,its potential to counteract SiNP-induced inflammatory responses in the lung has not been thoroughly explored.Objective:This study aimed to evaluate the protective role and mechanistic actions of SAA against SiNP-triggered inflammation in both cellular and animal models.Methods:HPAEpiCs were pre-incubated with SAA prior to SiNP exposure to investigate changes in COX-2 expression and prostaglandin E2(PGE2)secretion.A murine model of SiNP-induced lung inflammation was used for in vivo validation.Key inflammatory signaling proteins,including c-Src,PKCα,p42/p44MAPK,and NF-κB p65,were analyzed for phosphorylation status.NF-κB promoter activity was also assessed.Pharmacological inhibitors and siRNA-mediated silencing were employed to verify the signaling cascade responsible for COX-2 regulation.Results:SAA treatment markedly suppressed SiNP-induced upregulation of COX-2 and PGE2 in bothHPAEpiCs andmouse lung tissues.SAA also reduced the activation(phosphorylation)of c-Src,PKCα,p42/p44 MAPK,and NF-κB p65,alongside diminishing NF-κB transcriptional activity.Functional studies using inhibitors and gene silencing further supported the involvement of these pathways inmediating the observed anti-inflammatory effect.Conclusion:By concurrently targeting several upstream pro-inflammatory signaling pathways,SAA demonstrates robust potential in alleviating SiNP-induced lung inflammation.These results highlight SAA as a promising candidate for therapeutic intervention in environmentally triggered respiratory conditions.展开更多
Point source CO_(2) capture(PSCC)is crucial for decarbonizing various industrial sectors,while direct air capture(DAC)holds promise for removing CO_(2) directly from the air.Sorbents play a critical role in both techn...Point source CO_(2) capture(PSCC)is crucial for decarbonizing various industrial sectors,while direct air capture(DAC)holds promise for removing CO_(2) directly from the air.Sorbents play a critical role in both technologies,with their performances,efficiency,cost,etc.,largely depending on which type is used(physical or chemical).Solid amine sorbents(SAS)employed in the chemical adsorption of CO_(2) are suitable for both PSCC and DAC.SAS offer significant advantages over liquid amines such as monoethanolamine(MEA),due to their ability to perform cyclic adsorption–desorption with much lower energy requirement.The environmental concern associated with MEA can be mitigated by SAS.Support materials have a significantly important role in stabilizing amine and enhancing stability and kinetics;varieties of support materials have been screened at a laboratory scale.One promising support material is a silica gel(SG),which is commercially available and attractive for designing cost-effective sorbents for large-scale CO_(2) capture.Various impregnation methods such as physical adsorption and covalent functionalization have been employed to functionalize silica surfaces with amines.This review provided a comprehensive critical analysis of SG-based SAS for CO_(2) capture.We discussed and evaluated them in terms of their adsorption capacity,adsorption,and desorption conditions,and the kinetics involved in these processes.Finally,we proposed a few recommendations for further development of low-cost,lower carbon footprint SAS for large-scale deployment of CO_(2) capture technology.展开更多
A Ti_(3)SiC_(2)-modified high-silica oxygen/phenolic aerogel composite with excellent oxidation resistance and high-temperature performance was prepared.The experimental results show that the obtained composite has si...A Ti_(3)SiC_(2)-modified high-silica oxygen/phenolic aerogel composite with excellent oxidation resistance and high-temperature performance was prepared.The experimental results show that the obtained composite has significantly improved oxidation resistance.When the addition amount of Ti_(3)SiC_(2)is 75%,the carbonization volume shrinkage rate of the composite after aerobic static combustion is only 5.95%.At the same time,the LAR and MAR after 30 seconds of oxyacetylene ablation under a heat flux density of 1.5 MW/m2 are 0.0307 mm/s and 0.0149 g/s,respectively.The compressive strength after aerobic static combustion at 1000℃is up to 20.43%of that before aerobic static combustion,which is 1.99 times that of the unfilled material,significantly improving the high-temperature mechanical properties of the composite.展开更多
V2O5/WO3‐TiO2 and V2O5/WO3‐TiO2‐SiO2 catalysts were prepared by a wetness impregnation method, and both the catalysts were hydrothermally aged at 750℃ in 10 vol%H2O/air for 24 h. The catalysts were evaluated for N...V2O5/WO3‐TiO2 and V2O5/WO3‐TiO2‐SiO2 catalysts were prepared by a wetness impregnation method, and both the catalysts were hydrothermally aged at 750℃ in 10 vol%H2O/air for 24 h. The catalysts were evaluated for NOx conversion using NH3 as the reductant. Hydrothermal ageing decreased the NOx conversion of V2O5/WO3‐TiO2 catalyst severely over the entire measured tem‐perature range. Interestingly, the NH3‐SCR activity of the silica‐modified catalyst at 220–480℃ is enhanced after ageing. The catalysts were characterized by X‐ray diffraction, nitrogen adsorption, X‐ray fluorescence, Raman spectroscopy, H2 temperature‐programmed reduction, and NH3 temper‐ature‐programmed desorption. The addition of silica inhibited the phase transition from anatase to rutile titania, growth of TiO2 crystallite size and shrinkage of catalyst surface area. Consequently, the vanadia species remained highly dispersed and the hydrothermal stability of the V2O5/WO3‐TiO2 catalyst was significantly improved.展开更多
基金supported by the National Natural Science Foundation of China-Excellent Young Scholars(No.51922068)the National Key Research and Development Program(No.2017YFA0403800)+1 种基金the National Natural Science Foundation of China(Nos.51727802,51821001 and 51971138)Shanghai Pujiang Program(No.19PJ1404400)。
文摘Thermodynamic/dynamic modeling of liquid immiscibility in silicates is seriously hindered due to lack of in situ investigation on the structural evolution of the melt.In this work,atomic-scale structural evolution of a classic binary silicate immiscible system,SiO2–TiO2,is tracked by in situ high energy X-ray diffraction(HE-XRD).It is found that both the configuration of[SiO]and the polymerization between them are closely coupled with embedment and extraction of the metallic cations(Ti^4+).[SiO]monomer goes through deficit-oxygen and excess-polymerization before liquid–liquid separation and enables self-healing after liquid–liquid separation,which challenges the traditional cognition that[SiO4]monomer is immutable.Ti4+cations with tetrahedral oxygen-coordination first participate in the network construction before liquid separation.The four-fold Ti–O bond is broken during liquid separation,which may facilitate the movement of Ti4+across the Si–O network to form TiO2-rich nodules.The structural features of nodules were also investigated and they were found highly analogous to that of molten TiO2,which implies a parallel crystallization behavior in the two circumstances.Our results shed light on the structural evolution scenario in liquid immiscibility at atomic scale,which will contribute to constructing a complete thermodynamic/dynamic framework describing the silicate liquid immiscibility systems beyond current models.
基金supported by the National Science and Technology Council,Taiwan[Grant number:NSTC111-2320-B-030-013]as well as the Chang Gung University of Science Foundation,Taiwan[Grant number:ZRRPF6N0011].
文摘Background:Silica nanoparticles(SiNPs),commonly utilized in industrial and biomedical fields,are known to provoke pulmonary inflammation by elevating cyclooxygenase-2(COX-2)levels in human pulmonary alveolar epithelial cells(HPAEpiCs).Salvianolic acid A(SAA),a water-soluble polyphenol extracted from Salvia miltiorrhiza(Danshen),possesses well-documented antioxidant and anti-inflammatory activities.Nevertheless,its potential to counteract SiNP-induced inflammatory responses in the lung has not been thoroughly explored.Objective:This study aimed to evaluate the protective role and mechanistic actions of SAA against SiNP-triggered inflammation in both cellular and animal models.Methods:HPAEpiCs were pre-incubated with SAA prior to SiNP exposure to investigate changes in COX-2 expression and prostaglandin E2(PGE2)secretion.A murine model of SiNP-induced lung inflammation was used for in vivo validation.Key inflammatory signaling proteins,including c-Src,PKCα,p42/p44MAPK,and NF-κB p65,were analyzed for phosphorylation status.NF-κB promoter activity was also assessed.Pharmacological inhibitors and siRNA-mediated silencing were employed to verify the signaling cascade responsible for COX-2 regulation.Results:SAA treatment markedly suppressed SiNP-induced upregulation of COX-2 and PGE2 in bothHPAEpiCs andmouse lung tissues.SAA also reduced the activation(phosphorylation)of c-Src,PKCα,p42/p44 MAPK,and NF-κB p65,alongside diminishing NF-κB transcriptional activity.Functional studies using inhibitors and gene silencing further supported the involvement of these pathways inmediating the observed anti-inflammatory effect.Conclusion:By concurrently targeting several upstream pro-inflammatory signaling pathways,SAA demonstrates robust potential in alleviating SiNP-induced lung inflammation.These results highlight SAA as a promising candidate for therapeutic intervention in environmentally triggered respiratory conditions.
基金financial support from Business Finland 8205/31/2022the Magnus Ehrnrooth Foundation for financial support.
文摘Point source CO_(2) capture(PSCC)is crucial for decarbonizing various industrial sectors,while direct air capture(DAC)holds promise for removing CO_(2) directly from the air.Sorbents play a critical role in both technologies,with their performances,efficiency,cost,etc.,largely depending on which type is used(physical or chemical).Solid amine sorbents(SAS)employed in the chemical adsorption of CO_(2) are suitable for both PSCC and DAC.SAS offer significant advantages over liquid amines such as monoethanolamine(MEA),due to their ability to perform cyclic adsorption–desorption with much lower energy requirement.The environmental concern associated with MEA can be mitigated by SAS.Support materials have a significantly important role in stabilizing amine and enhancing stability and kinetics;varieties of support materials have been screened at a laboratory scale.One promising support material is a silica gel(SG),which is commercially available and attractive for designing cost-effective sorbents for large-scale CO_(2) capture.Various impregnation methods such as physical adsorption and covalent functionalization have been employed to functionalize silica surfaces with amines.This review provided a comprehensive critical analysis of SG-based SAS for CO_(2) capture.We discussed and evaluated them in terms of their adsorption capacity,adsorption,and desorption conditions,and the kinetics involved in these processes.Finally,we proposed a few recommendations for further development of low-cost,lower carbon footprint SAS for large-scale deployment of CO_(2) capture technology.
基金Funded by by the Wuhan Science and Technology Project(No.2024010702030141)。
文摘A Ti_(3)SiC_(2)-modified high-silica oxygen/phenolic aerogel composite with excellent oxidation resistance and high-temperature performance was prepared.The experimental results show that the obtained composite has significantly improved oxidation resistance.When the addition amount of Ti_(3)SiC_(2)is 75%,the carbonization volume shrinkage rate of the composite after aerobic static combustion is only 5.95%.At the same time,the LAR and MAR after 30 seconds of oxyacetylene ablation under a heat flux density of 1.5 MW/m2 are 0.0307 mm/s and 0.0149 g/s,respectively.The compressive strength after aerobic static combustion at 1000℃is up to 20.43%of that before aerobic static combustion,which is 1.99 times that of the unfilled material,significantly improving the high-temperature mechanical properties of the composite.
基金supported by the National Natural Science Foundation of China (51372137)the National High Technology Research and Development Program of China (863 Program,2015AA034603)~~
文摘V2O5/WO3‐TiO2 and V2O5/WO3‐TiO2‐SiO2 catalysts were prepared by a wetness impregnation method, and both the catalysts were hydrothermally aged at 750℃ in 10 vol%H2O/air for 24 h. The catalysts were evaluated for NOx conversion using NH3 as the reductant. Hydrothermal ageing decreased the NOx conversion of V2O5/WO3‐TiO2 catalyst severely over the entire measured tem‐perature range. Interestingly, the NH3‐SCR activity of the silica‐modified catalyst at 220–480℃ is enhanced after ageing. The catalysts were characterized by X‐ray diffraction, nitrogen adsorption, X‐ray fluorescence, Raman spectroscopy, H2 temperature‐programmed reduction, and NH3 temper‐ature‐programmed desorption. The addition of silica inhibited the phase transition from anatase to rutile titania, growth of TiO2 crystallite size and shrinkage of catalyst surface area. Consequently, the vanadia species remained highly dispersed and the hydrothermal stability of the V2O5/WO3‐TiO2 catalyst was significantly improved.
