Manganese oxides are regarded as one of the most promising cathode materials in rechargeable aqueous Zn-ion batteries(ZIBs)because of the low price and high security.However,the practical application of Mn2O3 in ZIBs ...Manganese oxides are regarded as one of the most promising cathode materials in rechargeable aqueous Zn-ion batteries(ZIBs)because of the low price and high security.However,the practical application of Mn2O3 in ZIBs is still plagued by the low specific capacity and poor rate capability.Herein,highly crystalline Mn2O3 materials with interconnected mesostructures and controllable pore sizes are obtained via a ligand-assisted self-assembly process and used as high-performance electrode materials for reversible aqueous ZIBs.The coordination degree between Mn2+and citric acid ligand plays a crucial role in the formation of the mesostructure,and the pore sizes can be easily tuned from 3.2 to 7.3 nm.Ascribed to the unique feature of nanoporous architectures,excellent zinc-storage performance can be achieved in ZIBs during charge/discharge processes.The Mn2O3 electrode exhibits high reversible capacity(233 mAh g−1 at 0.3 A g−1),superior rate capability(162 mAh g−1 retains at 3.08 A g−1)and remarkable cycling durability over 3000 cycles at a high current rate of 3.08 A g−1.Moreover,the corresponding electrode reaction mechanism is studied in depth according to a series of analytical methods.These results suggest that rational design of the nanoporous architecture for electrode materials can effectively improve the battery performance.展开更多
Surface modification by metal ion has been considered a promising strategy to enhance the photocatalytic activity by extending optical response and improving charge separation and transportation.Here,univalent copper ...Surface modification by metal ion has been considered a promising strategy to enhance the photocatalytic activity by extending optical response and improving charge separation and transportation.Here,univalent copper species were modified on ZnIn_(2)S_(4)photocatalyst via an in-situ photodeposition method,exhibiting a much higher H2evolution rate of 41.10±3.43 mmol g^(-1)h^(-1)and an impressive apparent quantum efficiency(AQE)of 20.81%at 420±15 nm.Our characterizations indicate that the surface modification by copper species can broaden light utilization as well as promote charge separation and transportation.Besides,the density functional theory(DFT)results further exhibit that the energy levels(LUMO and HOMO)for copper-surface modified ZnIn_(2)S_(4)present spatial separation,locating on the Zn-S and In-S layers,respectively,which can suppress the recombination of electron and hole and thus achieves higher photocatalytic H2evolution efficiency.展开更多
Colonoscopic polypectomy is extremely effective in protecting against colorectal cancers,and recognition of adenomas by colonoscopy is of paramount importance in preventing colorectal cancer(CRC)and CRC-associated mor...Colonoscopic polypectomy is extremely effective in protecting against colorectal cancers,and recognition of adenomas by colonoscopy is of paramount importance in preventing colorectal cancer(CRC)and CRC-associated mortality.Incomplete polyp resection(IPR)occurs routinely in medical practice following polypectomy.We conducted a comprehensive literature search to identify studies that reported on the potential risk factors for IPR using MEDLINE,EMBASE,and PubMed.Publication time was limited between January 2004 and July 2021.Our search revealed assessments of the position,morphology,and histologic variation of the polypsdas well as the relevant skills that may interfere with IPR.The included studies showed that colonic polyps with a diameter>20 mm and proximal in location should be dealt with cautiously.For smaller polyps,cold-snare polypectomy appeared to be the most effective method used to accomplish comprehensive polyp removal.In addition,endoscopist experience in narrow-band imaging in polyp detection were also associated with IPR.Therefore,polypectomy should be performed cautiously if the polyp growth is expected to be cancerous and situated in the proximal portion of the colon or rectum,and modalities should be standardized so as to lower the potential risk for IPR.展开更多
The phenomenon of strong metal-support interaction(SMSI)observed in supported metal catalysts,usually accompanied by the formation of the encapsulation layer on metal nanoparticles,has attracted extensive research att...The phenomenon of strong metal-support interaction(SMSI)observed in supported metal catalysts,usually accompanied by the formation of the encapsulation layer on metal nanoparticles,has attracted extensive research attention due to its significance in heterogeneous catalysis.Notably,great progress has been made in recent years in investigating SMSI by in situ transmission electron microscopy(TEM),along with an enhanced comprehension of the underlying mechanisms governing SMSI formation.This emerging topic summarizes recent progress utilizing in situ TEM to study the interaction between metal and support and the relationship between the structure and performance of the supported catalyst under reaction conditions.A brief perspective about the use of in situ TEM for further study of SMSI is also presented,showing prospects in this field that will stimulate further upsurging research in promoting the catalytic efficiency of supported catalysts.展开更多
Recycling spent lithium-ion batteries is integral to today's low-carbon environmental protection efforts.The concept of direct regeneration,acknowledged for its environmental sustainability,economic viability,and ...Recycling spent lithium-ion batteries is integral to today's low-carbon environmental protection efforts.The concept of direct regeneration,acknowledged for its environmental sustainability,economic viability,and consistent performance of recycled materials,is gaining prominence.This study presents an efficient and nondestructive approach by utilizing an ultrafast microwave technology to directly regenerate spent lithium cobaltate(LCO)cathode materials.In contrast to conventional furnacebased processes,this method significantly reduces the regeneration timeframe.By subjecting the spent LCO mixed with lithium sources to three microwave heating cycles(at approximately 1,350 K),LCO regeneration is achieved,yielding a specific capacity of 140.8 mAh g^(-1)(0.2 C)with a robust cycle stability.With further environmental and economic benefits,the ultrafast microwave technology holds scientific promise for directly regenerating cathode materials,while establishing competitiveness for industrial applications.展开更多
Mechanochemistry has been recognized as an efficient and sustainable methodology to provide a unique driven force and reaction environments under ambient and neat conditions for the construction of functionalized mate...Mechanochemistry has been recognized as an efficient and sustainable methodology to provide a unique driven force and reaction environments under ambient and neat conditions for the construction of functionalized materials possessing promising properties.Among them,highly porous conjugated scaffolds with attractive electronic conductivities and high surface areas are one of the representative categories exhibiting diverse taskspecific applications,especially in electrochemical energy storage.In recent years,the mechanochemistry-driven procedures have been deployed to construct conjugated scaffolds with engineered structures and properties leveraging the tunability in chemical structures of building blocks and polymerization capability of diverse catalysts.Therefore,a thorough review of related works is required to gain an in-depth understanding of the mechanochemical synthesis procedure and property-performance relationship of the as-produced conjugated scaffolds.Herein,the mechanochemistry-driven construction of conjugated porous networks(CPNs),the carbon-based materials(e.g.,graphite and graphyne),and carbon supported single atom catalysts(CS-SACs)are discussed and summarized.The electrochemical performance of the afforded conductive scaffolds as electrode materials in supercapacitors and alkali-ion batteries is elucidated.Finally,the challenges and potential opportunities related to the construction of conjugated scaffolds driven by mechanochemistry are also discussed and concluded.展开更多
Drilling plays a significant role in the history of human civilization.The exploration of greater depths,extreme environments,or hazardous areas calls for more energy-efficient and high levels of autonomous drilling t...Drilling plays a significant role in the history of human civilization.The exploration of greater depths,extreme environments,or hazardous areas calls for more energy-efficient and high levels of autonomous drilling technologies with reduced cost and improved safety.Meanwhile,nature presents numerous biological boring examples that can be a source of inspiration to renovate our current drilling technologies.This paper reviews both man-made and biological drilling strategies and quantifies their performance by the dimensionless specific drilling energy and the rate of penetration.The results highlight that rotary drilling(including tunnel boring machines)remains the most popular method for subsurface drilling due to its advanced technical status and fewer environmental concerns.For harder rocks,the specific energy of rotary drilling increases dramatically,while percussion drilling requires nearly the same if not lower specific energy but with compromised bit durability that can significantly slow down the drilling operation.Innovative drilling technologies developed and tested in the laboratory still demand improved energy efficiency and penetration rate to be competitive.Bio-boring by natural organisms mostly outperforms man-made drilling technologies in terms of energy efficiency,penetration rate,or both.Studying the underlying mechanisms of bio-boring and translating such knowledge into developing innovative drilling technologies are of significance to subsurface construction and exploration.展开更多
Since Haruta et al. discovered that small gold nanoparticles finely dispersed on certain metal oxide supports can exhibit surprisingly high activity in CO oxidation below room temperature, heterogeneous catalysis by s...Since Haruta et al. discovered that small gold nanoparticles finely dispersed on certain metal oxide supports can exhibit surprisingly high activity in CO oxidation below room temperature, heterogeneous catalysis by supported gold nanoparticles has attracted tremendous attention. The majority of publications deal with the preparation and characterization of conventional gold catalysts (e.g., Au/TiO2), the use of gold catalysts in various catalytic reactions, as well as elucidation of the nature of the active sites and reaction mechanisms. In this overview, we highlight the development of novel supported gold catalysts from a materials perspective. Examples, mostly from those reported by our group, are given concerning the development of simple gold catalysts with single metal-support interfaces and heterostructured gold catalysts with complicated interfacial structures. Catalysts in the first category include active Au/SiO2 and Au/metal phosphate catalysts, and those in the second category include catalysts prepared by pre-modification of supports before loading gold, by post-modification of supported gold catalysts, or by simultaneous dispersion of gold and an inorganic component onto a support. CO oxidation has generally been employed as a probe reaction to screen the activities of these catalysts. These novel gold catalysts not only provide possibilities for applied catalysis, but also furnish grounds for fundamental research.展开更多
Monodisperse Au nanoparticles(NPs)have been synthesized at room temperature via a burst nucleation of Au upon injection of the reducing agent t-butylamine-borane complex into a 1,2,3,4-tetrahydronaphthalene solution o...Monodisperse Au nanoparticles(NPs)have been synthesized at room temperature via a burst nucleation of Au upon injection of the reducing agent t-butylamine-borane complex into a 1,2,3,4-tetrahydronaphthalene solution of HAuCl4·3H2O in the presence of oleylamine.The as-synthesized Au NPs show size-dependent surface plasmonic properties between 520 and 530 nm.They adopt an icosahedral shape and are polycrystalline with multiple-twinned structures.When deposited on a graphitized porous carbon support,the NPs are highly active for CO oxidation,showing 100%CO conversion at-45°C.展开更多
High-entropy alloy nanoparticles(HEA-NPs)are highly underutilized in heterogeneous catalysis due to the absence of a reliable,sustainable,and facile synthetic method.Herein,we report a facile synthesis of HEA nanocata...High-entropy alloy nanoparticles(HEA-NPs)are highly underutilized in heterogeneous catalysis due to the absence of a reliable,sustainable,and facile synthetic method.Herein,we report a facile synthesis of HEA nanocatalysts realized via an ultrasounddriven wet chemistry method promoted by alcoholic ionic liquids(AILs).Owing to the intrinsic reducing ability of the hydroxyl group,AILs were synthesized and utilized as environmentally friendly alternatives to conventional reducing agents and volatile organic solvents in the synthetic process.Under high-intensity ultrasound irradiation,Au^(3+),Pd^(2+),Pt^(2+),Rh^(3+),and Ru^(3+)ions were coreduced and transformed into single-phase HEA(AuPdPtRhRu)nanocrystals without calcination.Characterization results reveal that the as-synthesized nanocrystals are composed of elements of Au,Pd,Pt,Rh,and Ru as expected.Compared to the monometallic counterparts such as Pd-NPs,the carbon-supported HEA nanocatalysts show superior catalytic performance for selective hydrogenation of phenol to cyclohexanone in terms of yield and selectivity.Our synthetic strategy provides an improved and facile methodology for the sustainable synthesis of multicomponent alloys for catalysis and other applications.展开更多
Ferritin stores and releases iron ions in mammals.It is globally important as a drug nanocarrier.This is because of its unique hollow-spherical structure,desirable stability and biological properties.Novel drug-loadin...Ferritin stores and releases iron ions in mammals.It is globally important as a drug nanocarrier.This is because of its unique hollow-spherical structure,desirable stability and biological properties.Novel drug-loading approaches plus various functionalization approaches have been developed to improve ferritin in response to differing demands in disease treatments.Here,we critically review ferritin drug delivery and evaluate its diverse drug-loading and functionalization approaches,we:(1)Introduce basic structural and property information related to ferritin as a drug nanocarrier;(2)Contrast in detail the different means to load drugs and the selection of drug loading means;(3)Discuss multiple ferritin functionalization approaches,together with related advantages and potential risks;and,(4)Compare ferritin with alternative,commonly-used drug nanocarriers.We conclude that despite that no drugs based on ferritin are commercially available,the market potential for it is significant,and evaluate future research directions.Findings from this work will be of immediate benefit and interest to a wide range of researchers and manufacturers for drug delivery using ferritin.展开更多
Fluorinated porous organic networks(F-PONs)have demonstrated unique properties and applications,but approaches capable of affording F-PONs with high fluorine content and robust nanoporous architecture under metal-free...Fluorinated porous organic networks(F-PONs)have demonstrated unique properties and applications,but approaches capable of affording F-PONs with high fluorine content and robust nanoporous architecture under metal-free and easy handling conditions are still rarely reported.Herein,using polydivinylbenzene(PDVB)as an easily available precursor,a novel and straightforward approach was developed to afford F-PONs via a dehydrative Friedel-Crafts reaction using perfluorinated benzylic alcohols as the cross-linking agent promoted by Bronsted acid(trifluoromethanesulfonic acid).The afforded material(F-PDVB)featured high fluorine content(22 at.%),large surface area(771 m^(2)·g^(-1)),and good chemical/thermal stability,rendering them as promising candidates for the adsorption of CO_(2),hydrocarbons,fluorocarbons,and chlorofluorocarbons,with weight capacities up to 520 wt.%being achieved.This simple methodology can be extended to fabricate fluorinated hyper-crosslinked polymers(F-HCPs)from rigid aromatic monomers.The progress made in this work will open new opportunities to further expand the involvement of fluorinated materials in large scale applications.展开更多
Designing metal compounds based on their structure and chemical composition is essential in achieving desirable performance in methane oxidation,because of the synergistic effect between different metal elements.Herei...Designing metal compounds based on their structure and chemical composition is essential in achieving desirable performance in methane oxidation,because of the synergistic effect between different metal elements.Herein,a bimetallic Ru-Pt catalyst on TiO_(2) support(RuPt-O/TiO_(2)) was prepared by in situ reduction followed by calcination in air.Compared with monometallic catalysts(Ru-O/TiO_(2) and Pt-O/TiO_(2)),the synergistic effect of mixed metals endowed bimetallic catalysts with excellent stability and outstanding performance in methane oxidation,with a reaction rate of 13.9×10^(-5)mol^(-1)_(CH_(4))·g^(-1)_(Ru+Pt)·s^(-1)at 303℃.The varied characterization results revealed that among the bimetallic catalysts,RuO_(2)was epitaxially grown on the TiO_(2) substrate owing to lattice matching between them,and part of the PtO_(x) adhered to the RuO_(2) surface,in addition to a single PtO_(x) nanoparticle with 4 nm in size.Consequently,Pt mainly existed in the form of Pt2+and Pt4+and a small amount of zero valence in the bimetallic catalyst,prompting the adsorption and activation of methane as the first and rate-controlling step for CH_(4) oxidation.More importantly,the RuO_(2) species provided additional oxygen species to facilitate the redox cycle of the PtO_(x) species.This study opens a new route for structurally designing promising catalysts for CH4oxidation.展开更多
Objective:Securidaca inappendiculata is a medicinal plant frequently used in the treatment of inflammatory diseases in south China.In this study,we aimed to explore its bioactive constituent which contributes to the a...Objective:Securidaca inappendiculata is a medicinal plant frequently used in the treatment of inflammatory diseases in south China.In this study,we aimed to explore its bioactive constituent which contributes to the anti-inflammatory activity.Methods:Polyphenol-enriched and polyphenol-deprived fractions(PRF and PDF,respectively)were separated from the ethanolic extract by HPD300 macroporous resin-based method,and their antiinflammatory activities were investigated on a lipopolysaccharide(LPS)-induced acute lung injury(ALI)model in rats.The possible mechanism of action in alleviating acute inflammation was studied using RAW264.7 cells.Results:Both Folin-Ciocalteu and^(1)H nuclear magnetic resonance(NMR)analyses showed that polyphenolic content in PRF was approximately 10 times higher than that of PDF,and this observation reflected in their antioxidative capacities.PRF but not PDF significantly decreased the level of malondialdehyde,suppressed the expression of nicotinamide phosphoribosyltransferase(NAMPT)protein,and improved the severity of ALI in rats.PRF at 10μg/mL effectively downregulated the expression of proteins NAMPT,HMGB1,TLR4,and p-p65,and scavenged the intracellular reactive oxygen species(ROS)in LPS-primed RAW264.7 cells.N-acetyl-L-cysteine exhibited similar inhibitory effects on ROS production and NAMPT-mediated TLR4/NF-κB activation in vitro,whereas nicotinamide mononucleotide antagonized all the changes induced by PRF during cotreatments.Conclusion:As an antioxidant,PRF exhibited potent anti-inflammatory activity under both in vivo and in vitro conditions by downregulating NAMPT and TLR4/NF-κB.Accordingly,polyphenols were identified as important bioactive constituents in S.inappendiculata targeting oxidative stress-sensitive proinflammatory pathways.展开更多
Titanium dioxide(TiO2)has a long history of application in blood contact materials,but it often suffers from insufficient anticoagulant properties.Recently,we have revealed the photocatalytic effect of TiO2 also induc...Titanium dioxide(TiO2)has a long history of application in blood contact materials,but it often suffers from insufficient anticoagulant properties.Recently,we have revealed the photocatalytic effect of TiO2 also induces anticoagulant properties.However,for long-term vascular implant devices such as vascular stents,besides anticoagulation,also anti-inflammatory,anti-hyperplastic properties,and the ability to support endothelial repair,are desired.To meet these requirements,here,we immobilized silver nanoparticles(AgNPs)on the surface of TiO2 nanotubes(TiO2-NTs)to obtain a composite material with enhanced photo-induced anticoagulant property and improvement of the other requested properties.The photo-functionalized TiO2-NTs showed protein-fouling resistance,causing the anticoagulant property and the ability to suppress cell adhesion.The immobilized AgNPs increased the photocatalytic activity of TiO2-NTs to enhances its photo-induced anticoagulant property.The AgNP density was optimized to endow the TiO2-NTs with anti-inflammatory property,a strong inhibitory effect on smooth muscle cells(SMCs),and low toxicity to endothelial cells(ECs).The in vivo test indicated that the photofunctionalized composite material achieved outstanding biocompatibility in vasculature via the synergy of photo-functionalized TiO2-NTs and the multifunctional AgNPs,and therefore has enormous potential in the field of cardiovascular implant devices.Our research could be a useful reference for further designing of multifunctional TiO2 materials with high vascular biocompatibility.展开更多
基金the Young Thousand Talented Program and the National Natural Science Foundation of China (21671073 and 21621001)the “111” Project of the Ministry of Education of China (B17020)Program for JLU Science and Technology Innovative Research Team
文摘Manganese oxides are regarded as one of the most promising cathode materials in rechargeable aqueous Zn-ion batteries(ZIBs)because of the low price and high security.However,the practical application of Mn2O3 in ZIBs is still plagued by the low specific capacity and poor rate capability.Herein,highly crystalline Mn2O3 materials with interconnected mesostructures and controllable pore sizes are obtained via a ligand-assisted self-assembly process and used as high-performance electrode materials for reversible aqueous ZIBs.The coordination degree between Mn2+and citric acid ligand plays a crucial role in the formation of the mesostructure,and the pore sizes can be easily tuned from 3.2 to 7.3 nm.Ascribed to the unique feature of nanoporous architectures,excellent zinc-storage performance can be achieved in ZIBs during charge/discharge processes.The Mn2O3 electrode exhibits high reversible capacity(233 mAh g−1 at 0.3 A g−1),superior rate capability(162 mAh g−1 retains at 3.08 A g−1)and remarkable cycling durability over 3000 cycles at a high current rate of 3.08 A g−1.Moreover,the corresponding electrode reaction mechanism is studied in depth according to a series of analytical methods.These results suggest that rational design of the nanoporous architecture for electrode materials can effectively improve the battery performance.
基金financially supported by the National Natural Science Funds for Distinguished Young Scholars(51725201)the International(Regional)Cooperation and Exchange Projects of the National Natural Science Foundation of China(51920105003)+4 种基金the Innovation Program of Shanghai Municipal Education Commission(E00014)the Science and Technology Commission of Shanghai Municipality(21DZ1207101)the National Natural Science Foundation of China(21902048)the Shanghai Engineering Research Center of Hierarchical Nanomaterials(18DZ2252400)Additional support was provided by the Feringa Nobel Prize Scientist Joint Research Center。
文摘Surface modification by metal ion has been considered a promising strategy to enhance the photocatalytic activity by extending optical response and improving charge separation and transportation.Here,univalent copper species were modified on ZnIn_(2)S_(4)photocatalyst via an in-situ photodeposition method,exhibiting a much higher H2evolution rate of 41.10±3.43 mmol g^(-1)h^(-1)and an impressive apparent quantum efficiency(AQE)of 20.81%at 420±15 nm.Our characterizations indicate that the surface modification by copper species can broaden light utilization as well as promote charge separation and transportation.Besides,the density functional theory(DFT)results further exhibit that the energy levels(LUMO and HOMO)for copper-surface modified ZnIn_(2)S_(4)present spatial separation,locating on the Zn-S and In-S layers,respectively,which can suppress the recombination of electron and hole and thus achieves higher photocatalytic H2evolution efficiency.
基金supported by the National Natural Science Foundation of China(No.81703076 and No.82072628).
文摘Colonoscopic polypectomy is extremely effective in protecting against colorectal cancers,and recognition of adenomas by colonoscopy is of paramount importance in preventing colorectal cancer(CRC)and CRC-associated mortality.Incomplete polyp resection(IPR)occurs routinely in medical practice following polypectomy.We conducted a comprehensive literature search to identify studies that reported on the potential risk factors for IPR using MEDLINE,EMBASE,and PubMed.Publication time was limited between January 2004 and July 2021.Our search revealed assessments of the position,morphology,and histologic variation of the polypsdas well as the relevant skills that may interfere with IPR.The included studies showed that colonic polyps with a diameter>20 mm and proximal in location should be dealt with cautiously.For smaller polyps,cold-snare polypectomy appeared to be the most effective method used to accomplish comprehensive polyp removal.In addition,endoscopist experience in narrow-band imaging in polyp detection were also associated with IPR.Therefore,polypectomy should be performed cautiously if the polyp growth is expected to be cancerous and situated in the proximal portion of the colon or rectum,and modalities should be standardized so as to lower the potential risk for IPR.
基金the support from the National Natural Science Foundation of China(22376062)the Science and Technology Commission of Shanghai Municipality(22ZR1415700)+1 种基金Shanghai Rising-star Program(20QA1402400)and the Fundamental Research Funds for the Central Universities,Additional support was provided by the Frontiers Science Center for Materiobiology and Dynamic Chemistry and the Feringa Nobel Prize Scientist Joint Research Center at East China University of Science and Technology。
文摘The phenomenon of strong metal-support interaction(SMSI)observed in supported metal catalysts,usually accompanied by the formation of the encapsulation layer on metal nanoparticles,has attracted extensive research attention due to its significance in heterogeneous catalysis.Notably,great progress has been made in recent years in investigating SMSI by in situ transmission electron microscopy(TEM),along with an enhanced comprehension of the underlying mechanisms governing SMSI formation.This emerging topic summarizes recent progress utilizing in situ TEM to study the interaction between metal and support and the relationship between the structure and performance of the supported catalyst under reaction conditions.A brief perspective about the use of in situ TEM for further study of SMSI is also presented,showing prospects in this field that will stimulate further upsurging research in promoting the catalytic efficiency of supported catalysts.
基金supported by the startup funding of Shanghai Jiao Tong Universitythe National Natural Science Foundation of Chinathe Ministry of Higher Education of Malaysia for the Fundamental Research Grant(FRGS/1/2022/STG05/UM/02/3)to Woo Haw Jiunn。
文摘Recycling spent lithium-ion batteries is integral to today's low-carbon environmental protection efforts.The concept of direct regeneration,acknowledged for its environmental sustainability,economic viability,and consistent performance of recycled materials,is gaining prominence.This study presents an efficient and nondestructive approach by utilizing an ultrafast microwave technology to directly regenerate spent lithium cobaltate(LCO)cathode materials.In contrast to conventional furnacebased processes,this method significantly reduces the regeneration timeframe.By subjecting the spent LCO mixed with lithium sources to three microwave heating cycles(at approximately 1,350 K),LCO regeneration is achieved,yielding a specific capacity of 140.8 mAh g^(-1)(0.2 C)with a robust cycle stability.With further environmental and economic benefits,the ultrafast microwave technology holds scientific promise for directly regenerating cathode materials,while establishing competitiveness for industrial applications.
基金supported by the U.S.Department of Energy,Office of Science,Basic Energy Sciences,Materials Sciences,and Engineering Division
文摘Mechanochemistry has been recognized as an efficient and sustainable methodology to provide a unique driven force and reaction environments under ambient and neat conditions for the construction of functionalized materials possessing promising properties.Among them,highly porous conjugated scaffolds with attractive electronic conductivities and high surface areas are one of the representative categories exhibiting diverse taskspecific applications,especially in electrochemical energy storage.In recent years,the mechanochemistry-driven procedures have been deployed to construct conjugated scaffolds with engineered structures and properties leveraging the tunability in chemical structures of building blocks and polymerization capability of diverse catalysts.Therefore,a thorough review of related works is required to gain an in-depth understanding of the mechanochemical synthesis procedure and property-performance relationship of the as-produced conjugated scaffolds.Herein,the mechanochemistry-driven construction of conjugated porous networks(CPNs),the carbon-based materials(e.g.,graphite and graphyne),and carbon supported single atom catalysts(CS-SACs)are discussed and summarized.The electrochemical performance of the afforded conductive scaffolds as electrode materials in supercapacitors and alkali-ion batteries is elucidated.Finally,the challenges and potential opportunities related to the construction of conjugated scaffolds driven by mechanochemistry are also discussed and concluded.
基金supported by the National Science Foundation Engineering Research Center for Bio-mediated and Bio-inspired Geotechnics(EEC-1449501).
文摘Drilling plays a significant role in the history of human civilization.The exploration of greater depths,extreme environments,or hazardous areas calls for more energy-efficient and high levels of autonomous drilling technologies with reduced cost and improved safety.Meanwhile,nature presents numerous biological boring examples that can be a source of inspiration to renovate our current drilling technologies.This paper reviews both man-made and biological drilling strategies and quantifies their performance by the dimensionless specific drilling energy and the rate of penetration.The results highlight that rotary drilling(including tunnel boring machines)remains the most popular method for subsurface drilling due to its advanced technical status and fewer environmental concerns.For harder rocks,the specific energy of rotary drilling increases dramatically,while percussion drilling requires nearly the same if not lower specific energy but with compromised bit durability that can significantly slow down the drilling operation.Innovative drilling technologies developed and tested in the laboratory still demand improved energy efficiency and penetration rate to be competitive.Bio-boring by natural organisms mostly outperforms man-made drilling technologies in terms of energy efficiency,penetration rate,or both.Studying the underlying mechanisms of bio-boring and translating such knowledge into developing innovative drilling technologies are of significance to subsurface construction and exploration.
文摘Since Haruta et al. discovered that small gold nanoparticles finely dispersed on certain metal oxide supports can exhibit surprisingly high activity in CO oxidation below room temperature, heterogeneous catalysis by supported gold nanoparticles has attracted tremendous attention. The majority of publications deal with the preparation and characterization of conventional gold catalysts (e.g., Au/TiO2), the use of gold catalysts in various catalytic reactions, as well as elucidation of the nature of the active sites and reaction mechanisms. In this overview, we highlight the development of novel supported gold catalysts from a materials perspective. Examples, mostly from those reported by our group, are given concerning the development of simple gold catalysts with single metal-support interfaces and heterostructured gold catalysts with complicated interfacial structures. Catalysts in the first category include active Au/SiO2 and Au/metal phosphate catalysts, and those in the second category include catalysts prepared by pre-modification of supports before loading gold, by post-modification of supported gold catalysts, or by simultaneous dispersion of gold and an inorganic component onto a support. CO oxidation has generally been employed as a probe reaction to screen the activities of these catalysts. These novel gold catalysts not only provide possibilities for applied catalysis, but also furnish grounds for fundamental research.
基金by NSF/DMR 0606264 and a GAANN fellowship(Y.Lee).
文摘Monodisperse Au nanoparticles(NPs)have been synthesized at room temperature via a burst nucleation of Au upon injection of the reducing agent t-butylamine-borane complex into a 1,2,3,4-tetrahydronaphthalene solution of HAuCl4·3H2O in the presence of oleylamine.The as-synthesized Au NPs show size-dependent surface plasmonic properties between 520 and 530 nm.They adopt an icosahedral shape and are polycrystalline with multiple-twinned structures.When deposited on a graphitized porous carbon support,the NPs are highly active for CO oxidation,showing 100%CO conversion at-45°C.
基金supported by the Division of Chemical Sciences,Geosciences,and Biosciences,Office of Basic Energy Sciences,US Department of Energy.
文摘High-entropy alloy nanoparticles(HEA-NPs)are highly underutilized in heterogeneous catalysis due to the absence of a reliable,sustainable,and facile synthetic method.Herein,we report a facile synthesis of HEA nanocatalysts realized via an ultrasounddriven wet chemistry method promoted by alcoholic ionic liquids(AILs).Owing to the intrinsic reducing ability of the hydroxyl group,AILs were synthesized and utilized as environmentally friendly alternatives to conventional reducing agents and volatile organic solvents in the synthetic process.Under high-intensity ultrasound irradiation,Au^(3+),Pd^(2+),Pt^(2+),Rh^(3+),and Ru^(3+)ions were coreduced and transformed into single-phase HEA(AuPdPtRhRu)nanocrystals without calcination.Characterization results reveal that the as-synthesized nanocrystals are composed of elements of Au,Pd,Pt,Rh,and Ru as expected.Compared to the monometallic counterparts such as Pd-NPs,the carbon-supported HEA nanocatalysts show superior catalytic performance for selective hydrogenation of phenol to cyclohexanone in terms of yield and selectivity.Our synthetic strategy provides an improved and facile methodology for the sustainable synthesis of multicomponent alloys for catalysis and other applications.
基金funded by joint PhD Scholarship Scheme of the University of Adelaide and Institute of Process EngineeringChinese Academy of Sciences+1 种基金the National Natural Science Foundation of China(Grant No.21576267)Beijing Natural Science Foundation(Grant Number 2162041).
文摘Ferritin stores and releases iron ions in mammals.It is globally important as a drug nanocarrier.This is because of its unique hollow-spherical structure,desirable stability and biological properties.Novel drug-loading approaches plus various functionalization approaches have been developed to improve ferritin in response to differing demands in disease treatments.Here,we critically review ferritin drug delivery and evaluate its diverse drug-loading and functionalization approaches,we:(1)Introduce basic structural and property information related to ferritin as a drug nanocarrier;(2)Contrast in detail the different means to load drugs and the selection of drug loading means;(3)Discuss multiple ferritin functionalization approaches,together with related advantages and potential risks;and,(4)Compare ferritin with alternative,commonly-used drug nanocarriers.We conclude that despite that no drugs based on ferritin are commercially available,the market potential for it is significant,and evaluate future research directions.Findings from this work will be of immediate benefit and interest to a wide range of researchers and manufacturers for drug delivery using ferritin.
基金Project supported by the National Science Fund for Distinguished Young Scholars(No.51625805),Chinathe Program of China Scholarships Council(No.201706320096)+2 种基金the Zhejiang Provincial Key Research Project of China(No.2015C03021)the Engineering Research Center Program of the US National Science Foundation(No.EEC-1449501)the US DOE/NETL Gas Hydrate Research Program
基金supported financially by the Division of Chemical Sciences,Geosciences,and Biosciences,Office of Basic Energy Sciences,US Department of Energy.
文摘Fluorinated porous organic networks(F-PONs)have demonstrated unique properties and applications,but approaches capable of affording F-PONs with high fluorine content and robust nanoporous architecture under metal-free and easy handling conditions are still rarely reported.Herein,using polydivinylbenzene(PDVB)as an easily available precursor,a novel and straightforward approach was developed to afford F-PONs via a dehydrative Friedel-Crafts reaction using perfluorinated benzylic alcohols as the cross-linking agent promoted by Bronsted acid(trifluoromethanesulfonic acid).The afforded material(F-PDVB)featured high fluorine content(22 at.%),large surface area(771 m^(2)·g^(-1)),and good chemical/thermal stability,rendering them as promising candidates for the adsorption of CO_(2),hydrocarbons,fluorocarbons,and chlorofluorocarbons,with weight capacities up to 520 wt.%being achieved.This simple methodology can be extended to fabricate fluorinated hyper-crosslinked polymers(F-HCPs)from rigid aromatic monomers.The progress made in this work will open new opportunities to further expand the involvement of fluorinated materials in large scale applications.
基金financially supported by National Natural Science Foundation of China(Nos.21922602,22076047 and U21A20326)Shanghai Science and Technology Innovation Action Plan(No.20dz1204200)the Fundamental Research Funds for the Central Universities。
文摘Designing metal compounds based on their structure and chemical composition is essential in achieving desirable performance in methane oxidation,because of the synergistic effect between different metal elements.Herein,a bimetallic Ru-Pt catalyst on TiO_(2) support(RuPt-O/TiO_(2)) was prepared by in situ reduction followed by calcination in air.Compared with monometallic catalysts(Ru-O/TiO_(2) and Pt-O/TiO_(2)),the synergistic effect of mixed metals endowed bimetallic catalysts with excellent stability and outstanding performance in methane oxidation,with a reaction rate of 13.9×10^(-5)mol^(-1)_(CH_(4))·g^(-1)_(Ru+Pt)·s^(-1)at 303℃.The varied characterization results revealed that among the bimetallic catalysts,RuO_(2)was epitaxially grown on the TiO_(2) substrate owing to lattice matching between them,and part of the PtO_(x) adhered to the RuO_(2) surface,in addition to a single PtO_(x) nanoparticle with 4 nm in size.Consequently,Pt mainly existed in the form of Pt2+and Pt4+and a small amount of zero valence in the bimetallic catalyst,prompting the adsorption and activation of methane as the first and rate-controlling step for CH_(4) oxidation.More importantly,the RuO_(2) species provided additional oxygen species to facilitate the redox cycle of the PtO_(x) species.This study opens a new route for structurally designing promising catalysts for CH4oxidation.
基金supported by National Natural Science Foundation of China(81603388,81973828 and 81173596)Major Project of Natural Science Foundation of the Department of Education of Anhui province(KJ2019ZD32)+1 种基金Funding of"Peak"Training Program for Scientific Research of Yijishan Hospital,Wannan Medical College(GF2019J01)Key Project of Natural Science Foundation of Anhui Province for College Scholar(KJ2019A0416 and KJ2018A0249)。
文摘Objective:Securidaca inappendiculata is a medicinal plant frequently used in the treatment of inflammatory diseases in south China.In this study,we aimed to explore its bioactive constituent which contributes to the anti-inflammatory activity.Methods:Polyphenol-enriched and polyphenol-deprived fractions(PRF and PDF,respectively)were separated from the ethanolic extract by HPD300 macroporous resin-based method,and their antiinflammatory activities were investigated on a lipopolysaccharide(LPS)-induced acute lung injury(ALI)model in rats.The possible mechanism of action in alleviating acute inflammation was studied using RAW264.7 cells.Results:Both Folin-Ciocalteu and^(1)H nuclear magnetic resonance(NMR)analyses showed that polyphenolic content in PRF was approximately 10 times higher than that of PDF,and this observation reflected in their antioxidative capacities.PRF but not PDF significantly decreased the level of malondialdehyde,suppressed the expression of nicotinamide phosphoribosyltransferase(NAMPT)protein,and improved the severity of ALI in rats.PRF at 10μg/mL effectively downregulated the expression of proteins NAMPT,HMGB1,TLR4,and p-p65,and scavenged the intracellular reactive oxygen species(ROS)in LPS-primed RAW264.7 cells.N-acetyl-L-cysteine exhibited similar inhibitory effects on ROS production and NAMPT-mediated TLR4/NF-κB activation in vitro,whereas nicotinamide mononucleotide antagonized all the changes induced by PRF during cotreatments.Conclusion:As an antioxidant,PRF exhibited potent anti-inflammatory activity under both in vivo and in vitro conditions by downregulating NAMPT and TLR4/NF-κB.Accordingly,polyphenols were identified as important bioactive constituents in S.inappendiculata targeting oxidative stress-sensitive proinflammatory pathways.
基金the National Natural Science Foundation of China(nos.31870958,31700821,and 81771988).
文摘Titanium dioxide(TiO2)has a long history of application in blood contact materials,but it often suffers from insufficient anticoagulant properties.Recently,we have revealed the photocatalytic effect of TiO2 also induces anticoagulant properties.However,for long-term vascular implant devices such as vascular stents,besides anticoagulation,also anti-inflammatory,anti-hyperplastic properties,and the ability to support endothelial repair,are desired.To meet these requirements,here,we immobilized silver nanoparticles(AgNPs)on the surface of TiO2 nanotubes(TiO2-NTs)to obtain a composite material with enhanced photo-induced anticoagulant property and improvement of the other requested properties.The photo-functionalized TiO2-NTs showed protein-fouling resistance,causing the anticoagulant property and the ability to suppress cell adhesion.The immobilized AgNPs increased the photocatalytic activity of TiO2-NTs to enhances its photo-induced anticoagulant property.The AgNP density was optimized to endow the TiO2-NTs with anti-inflammatory property,a strong inhibitory effect on smooth muscle cells(SMCs),and low toxicity to endothelial cells(ECs).The in vivo test indicated that the photofunctionalized composite material achieved outstanding biocompatibility in vasculature via the synergy of photo-functionalized TiO2-NTs and the multifunctional AgNPs,and therefore has enormous potential in the field of cardiovascular implant devices.Our research could be a useful reference for further designing of multifunctional TiO2 materials with high vascular biocompatibility.
基金supported by the National Key Research and Development Program of China (2020YFB1505802)the National Natural Science Foundation of China (21931009 and 21721001)+2 种基金the Fundamental Research Funds for the Central Universities (20720210016 and 20720210104)the China Postdoctoral Science Foundation (2020M671939)Additional support was provided by Feringa Nobel Prize Scientist Joint Research Center。