Available online two new Ni_(8)Mo_(8) bimetallic coordination clusters,[Ni_(4)(TC4A)]_(2)[(Mo_5~VMo_(3)~ⅥO_(24))(PO_(4))](+Solvent)(Ni_(8)PMo_(8),H_(4)TC4A=p-tert-butylthiacalix[4]arene) and[Ni_(4)(TC4A)]_(2)[(Mo_5~V...Available online two new Ni_(8)Mo_(8) bimetallic coordination clusters,[Ni_(4)(TC4A)]_(2)[(Mo_5~VMo_(3)~ⅥO_(24))(PO_(4))](+Solvent)(Ni_(8)PMo_(8),H_(4)TC4A=p-tert-butylthiacalix[4]arene) and[Ni_(4)(TC4A)]_(2)[(Mo_5~VMo_(3)~ⅥO_(24))(OH)(CO_(3))](+Solvent)(Ni_(8)Mo_(8)),were synthesized by solvothermal method and structurally characterized by single-crystal X-ray diffraction,powder X-ray diffraction,FT-IR spectroscopy,and TGA experiments,respectively.The usage of H_(3)PMo_(12)O_(40) as source for Ni_(8)PMo_(8) resulted a sandwich like structure built from two Ni_(4)-thiacalix[4]arene units and a Mo_(8) polyoxometalate with inner spaces of PO_(4)^(3-).Ni_(8)Mo_(8) with the similar structure to that of Ni_(8)PMo_(8) is from H_(2)MoO_(4) starting reagent with OH^(-)and CO_(3)^(2-)anions encapsulated in the center.The two clusters can be directly loaded on carbon paper and utilized as working electrodes which showed distinguishable performances for glucose detection and oxidation.This work provides a better understanding of the structure-property relationships in using substituted polyoxometalates for electrochemical applications and is helpful for building calixarene-based or polyoxometalatebased functional materials.展开更多
The biosynthesized gold/activated carbon catalysts for glucose oxidation were prepared with Cacumen platycladi leaves extract,and activated carbon （AC） was modified with hydrochloric acid and nitric acid to modify i...The biosynthesized gold/activated carbon catalysts for glucose oxidation were prepared with Cacumen platycladi leaves extract,and activated carbon （AC） was modified with hydrochloric acid and nitric acid to modify its surface chemistry and used as supports.The catalysts with acid-treated AC exhibited improving activity for the selective oxidation of glucose,when compared to that with untreated one.In order to investigate the influence of the acid treatment for the catalysts performance,the surface chemical properties of AC were characterized by BrunauerEmmett-Teller surface area characterization,Boehm titration,X-ray photoelectron spectroscopy and Fourier transform infrared spectroscopy,respectively.The dispersion of AuNPs on AC was observed by transmission electron microscopy and X-ray diffraction.The results indicated that the catalysts with acid treated supports showed improved dispersion than that of untreated one,which may be the result that the supports significantly increase the surface functional groups and remove the ash after acid treatment.展开更多
Meeting the continuous glucose monitoring requirements of individuals necessitates the research and development of sensors with high sensitivity and stability.In this study,a straightforward strategy was proposed for ...Meeting the continuous glucose monitoring requirements of individuals necessitates the research and development of sensors with high sensitivity and stability.In this study,a straightforward strategy was proposed for synthesizing ultra-thin oxygen-rich graphitized carbon nanosheets(denoted as GCS-O).These nanosheets are obtained by calcining a topologically two-dimensional indium-based coordination polymer.Subsequently,the growth of FeNi Prussian blue analogue(PBA)on GCS-O effectively introduces active sites and increases the nitrogen content within the carbonaceous matrix.The resulting FeNi-PBA/GCS-O composite exhibits excellent glucose sensing performance with a broad linear range of 1 to 1300μmol·L^(-1).Meanwhile,it also achieves a high sensitivity of 2496μA·mmol^(-1)·L·cm^(-2),a limit of detection of 100nmol·L^(-1)(S/N=3),and commendable long-term durability.The relatively simple synthesis process,exceptional sensitivity,and satisfactory electrochemical sensing performance of FeNi-PBA/GCS-O open up new directions for biosensor applications.展开更多
In this study the catalytic properties of gold nanoparticles in electro-oxidation process of glucose, were investigated, taking into account, an influence of catalyst composition. Graphene oxide was applied and for el...In this study the catalytic properties of gold nanoparticles in electro-oxidation process of glucose, were investigated, taking into account, an influence of catalyst composition. Graphene oxide was applied and for electro-oxidation studies of glucose, cyclic voltamperometry was used. It was found that an application of graphene oxide sheets during catalyst synthesis have an influence on gold nanoparticles (AuNPs) size and size distribution. It was confirmed that the application of composite catalyst consisting of graphane-AuNPs significantly changes electro-oxidation of glucose shifting the potential of oxidation to higher positive values and increasing oxidation current.展开更多
Hydrogen production coupled with small molecule oxidation derived by renewable energy power has been widely studied as an effective method to reduce energy consumption and prepare added value production.Here,the coppe...Hydrogen production coupled with small molecule oxidation derived by renewable energy power has been widely studied as an effective method to reduce energy consumption and prepare added value production.Here,the copper-cobalt phosphide with a multilevel structure has been designed based on the hard and soft acids and bases theory.The nanocone composed of lamellas presented a sharp tip,which a positive effect on the mass transfer enhanced by a local electric field,and the nanolamellas contain CoP/Cu_(3)P interface provide the highly selective active site for the gluconic acid(GNA)synthesis and hydrogen evolution.The catalyst can drive hydrogen evolution at 5 A·cm^(-2)up to 437 h without active decay,and the electrocatalytic glucose oxidation at anode presents high efficiency due to Cu(I)introduction and the synergetic effect between interfaces.Density functional theory(DFT)calculation shows that water splitting more readily occurs at the CoP,which provides adsorbed H and-OH for hydrogen evolution and glucose oxidation,respectively,and glucose adsorption more readily occurs at the Cu_(3)P,which presents lower conversion energy for high value-added GNA.Efficient hydrogen evolution and glucose conversion indicate its high intrinsic activity and synergetic effect.This work provides a special interface construction strategy for the catalytic conversion of hydrogen and small molecules.展开更多
In this work, nitric oxide （NO） release coatings designed for intravenous amperometric glucose sensors are optimized through the use ofa polylactic acid （PLA） layer doped with a lipophilic diazeniumdiolated specie...In this work, nitric oxide （NO） release coatings designed for intravenous amperometric glucose sensors are optimized through the use ofa polylactic acid （PLA） layer doped with a lipophilic diazeniumdiolated species that releases NO through a proton-driven mechanism. An Elast-Eon E2As polyurethane coating is used to both moderate NO release from the sensor surface and increase the sensor＇s linear detection range toward glucose. These sensors were evaluated for thromboresistance and in vivo glucose performance through implantation in rabbit veins. By maintaining NO flux on a similar scale to endogenous endothelial cells, implanted glucose sensors exhibited reduced surface clot formation which enables more accurate quantitative glucose measurements continuously. An in vivo time trace of implanted venous sensors demonstrated glucose values that correlated well with the discrete measurements of blood samples on a benchtop point-of-care sensor-based instrument. The raw measured currents from the implanted glucose sensors over 7 h time periods were converted to glucose concentration through use of both a one-point in vivo calibration and a calibration curve obtained in vitro within a bovine serum solution. Control sensors, assembled without NO release functionality, exhibit distinctive surface clotting over the 7 h in vivo implantation period.展开更多
Research on metal-organic framework(MOF)-based non-enzymatic glucose sensors usually ignores the impact of the surface reconstruction degree of MOF on the activity of catalyzing glucose oxidation.In this work,we choos...Research on metal-organic framework(MOF)-based non-enzymatic glucose sensors usually ignores the impact of the surface reconstruction degree of MOF on the activity of catalyzing glucose oxidation.In this work,we choose zeolitic imidazolate framework-67(ZIF-67),which is commonly used in glucose sensing,as a representative to investigate the influence of reconstruction degree on its structure and glucose catalytic performance.By employing the electrochemical activation strategy,the activity of ZIF-67 in catalyzing glucose gradually increased with the prolongation of the activation time,reaching the optimum after 2 h activation.The detection sensitivity of the activated ZIF-67 was 19 times higher than that of the initial ZIF-67,and the limit of detection(LOD)was lowered from 7 to 0.4μM.Our findings demonstrate that the oxidation degree of ZIF-67 deepened rapidly with continuously activation and was basically reconstructed to CoOOH after 2 h activation,accompanied by a morphological change from cuboctahedral to flower-like.Simultaneously,theoretical investigation revealed that ZIF-67 is not suitable as a stable glucose sensor electrode since the adsorbed glucose molecules hasten the dissociation of ligands and the breaking of Co-N bond in ZIF-67.Therefore,our work has important implications for the rational design of next-generation MOF-based glucose sensors.展开更多
Cupric oxide （CuO） and copper-cuprous oxide （Cu-Cu2O） nanoparticles were prepared by a simple hydrothermal method for the synthesis of diethyi carbonate （DEC） from ethanol. During these syntheses, varying NaOH a...Cupric oxide （CuO） and copper-cuprous oxide （Cu-Cu2O） nanoparticles were prepared by a simple hydrothermal method for the synthesis of diethyi carbonate （DEC） from ethanol. During these syntheses, varying NaOH and glucose concentrations were applied to explore and pinpoint the active species. It was found that PdCl2/CuO and PdCI2/Cu-Cu2O both catalysts exhibited good thermal stability and morphology. The results of catalytic tests showed that the catalysts prepared with 5 mol/L NaOH show superior catalytic performances because of their lower extent of agglomeration. It is noteworthy that the PdC12/Cu-Cu2O catalysts were the most active, especially the PdCl2/Cu-Cu2O catalyst prepared with 10 mmol glucose and having a higher Cu2O concentration. In Pd（ll）-Cu（II） （PdCl2/CuO） catalysts, there is an induction period, during which Pd（II） is reduced to Pd（0）, that must occur prior to electron transfer between Pd and Cu, and this can slow the catalytic reaction. To further pinpoint the active species, PdCl2/Cu-Cu2O catalysts with different Cu2O contents were prepared by controlling the dosages of glucose. The maximum DEC yield obtained with these catalysts was 151.9 mg.g-1.h-1, corresponding to an ethanol conversion of 7.2% and 97.9% DEC selectivity on an ethanol basis. Therefore, it was concluded that Cu＋ was the active species in this catalytic system, possibly because a higher proportion of Cu＋ reduces the Pd2＋ concentration and limits the CO oxidation side reaction, thus increasing DEC selectivity. In addition, Cu＋ promotes electron transfer between Pd and Cu without an induction period, which could also promote the catalytic activity.展开更多
The effect of the reduction method on the catalytic properties of palladium catalysts supported on activated carbon for the oxidation of D-glucose was examined.The reduction methods investigated include argon glow dis...The effect of the reduction method on the catalytic properties of palladium catalysts supported on activated carbon for the oxidation of D-glucose was examined.The reduction methods investigated include argon glow discharge plasma reduction at room temperature,reduction by flowing hydrogen at elevated temperature,and reduction by formaldehyde at room temperature.The plasma-reduced catalyst shows the smallest metal particles with a narrow size distribution that leads to a much higher activity.The catalyst characteristics show that the plasma reduction increases the amount of oxygen-containing functional groups,which significantly enhances the hydrophilic property of the activated carbon and improves the dispersion of the metal.展开更多
Since its creation,single-molecule optical imaging has revolutionized the study of catalytic processes,yet its application largely relies on probing fluorogenic reactions.To overcome this limitation,we propose the Flu...Since its creation,single-molecule optical imaging has revolutionized the study of catalytic processes,yet its application largely relies on probing fluorogenic reactions.To overcome this limitation,we propose the Fluorogenic Linkage Integration for Nonfluorescent Transformation(FLINT)approach,an imaging method to resolve nonfluorogenic reactions at the single-molecule level.Using glucose oxidation as a model reaction,we coupled this nonfluorogenic reaction with a fluorogenic Amplex Red(AR)→resorufin(RF)transformation to create a cascading reaction.This integration allowed us to monitor single-turnover events and extract key kinetic parameters for glucose oxidation despite their being invisible under the optical microscope.Our ensemble measurements combining cyclic voltammetry and fluorescence spectroscopy confirmed the cascade reaction mechanism and revealed first-order kinetics for both elementary reaction steps.At the single-molecule level,turnover time analysis provided detailed information on the reaction kinetics,distinguishing the relatively fast glucose oxidation from slower AR oxidation.We further confirmed the validity of the FLINT approach by comparing the catalytic performances of 5 nm gold nanoparticles(AuNPs)against that of 18×52 nm gold nanorods(AuNRs)and AuNP@DNA coronazymes.Furthermore,FLINT was used to evaluate the chiral selectivity of D-and L-glucose on coronazymes,suggesting the potential application of FLINT in enantioselective reactions.The FLINT approach is a significant advancement in single-molecule imaging as it enables the study of nonfluorogenic reactions with high spatiotemporal resolution.展开更多
Background Studies have shown that complications in type 1 diabetes mellitus （T1DM） in children are mainly due to oxidative stress （OS）. Lipid peroxidation is the main marker of OS and iso-prostaglandin is a relia...Background Studies have shown that complications in type 1 diabetes mellitus （T1DM） in children are mainly due to oxidative stress （OS）. Lipid peroxidation is the main marker of OS and iso-prostaglandin is a reliable biomarker of lipid peroxidation in type 2 diabetes mellitus （T2DM）. However, there have been few studies on OS in T1DM children with hyperglycemia and glucose fluctuations.展开更多
Water electrolysis is one of the most promising approaches for producing hydrogen.However,it has been hindered by the sluggishness of the anodic oxygen evolution reaction.In this work,we fabricated Ru-Co-Mn trimetalli...Water electrolysis is one of the most promising approaches for producing hydrogen.However,it has been hindered by the sluggishness of the anodic oxygen evolution reaction.In this work,we fabricated Ru-Co-Mn trimetallic alloy nanoparticles on N-doped carbon support(RuCoMn@NC)via the pyrolysis-adsorption-pyrolysis process using ZIF-67 as a precursor.The RuCoMn@NC catalyst exhibited excellent electrocatalytic performance for the hydrogen evolution reaction(HER)over a wide range of pH and glucose oxidation reaction in alkaline media.It showed exceptional HER activity in alkaline medium,superior to that of the commercial Pt/C catalyst(20 wt%),and good electrochemical stability.Further,a two-electrode alkaline electrolyzer pairing RuCoMn@NC as both cathode and anode was employed,and only a cell voltage of 1.63 V was required to attain a current density of 10 mA cm^(-2)in glucose electrolysis,which is about 270 mV lower than that in the overall water-splitting electrolyzer.This paper provides a promising method for developing efficiently bifunctional electrocatalysts driving redox electrocatalysis,and it would be beneficial to energy-saving electrolytic H_(2) production.展开更多
基金supported by the National Natural Science Foundation of China(No.91961110)。
文摘Available online two new Ni_(8)Mo_(8) bimetallic coordination clusters,[Ni_(4)(TC4A)]_(2)[(Mo_5~VMo_(3)~ⅥO_(24))(PO_(4))](+Solvent)(Ni_(8)PMo_(8),H_(4)TC4A=p-tert-butylthiacalix[4]arene) and[Ni_(4)(TC4A)]_(2)[(Mo_5~VMo_(3)~ⅥO_(24))(OH)(CO_(3))](+Solvent)(Ni_(8)Mo_(8)),were synthesized by solvothermal method and structurally characterized by single-crystal X-ray diffraction,powder X-ray diffraction,FT-IR spectroscopy,and TGA experiments,respectively.The usage of H_(3)PMo_(12)O_(40) as source for Ni_(8)PMo_(8) resulted a sandwich like structure built from two Ni_(4)-thiacalix[4]arene units and a Mo_(8) polyoxometalate with inner spaces of PO_(4)^(3-).Ni_(8)Mo_(8) with the similar structure to that of Ni_(8)PMo_(8) is from H_(2)MoO_(4) starting reagent with OH^(-)and CO_(3)^(2-)anions encapsulated in the center.The two clusters can be directly loaded on carbon paper and utilized as working electrodes which showed distinguishable performances for glucose detection and oxidation.This work provides a better understanding of the structure-property relationships in using substituted polyoxometalates for electrochemical applications and is helpful for building calixarene-based or polyoxometalatebased functional materials.
文摘The biosynthesized gold/activated carbon catalysts for glucose oxidation were prepared with Cacumen platycladi leaves extract,and activated carbon （AC） was modified with hydrochloric acid and nitric acid to modify its surface chemistry and used as supports.The catalysts with acid-treated AC exhibited improving activity for the selective oxidation of glucose,when compared to that with untreated one.In order to investigate the influence of the acid treatment for the catalysts performance,the surface chemical properties of AC were characterized by BrunauerEmmett-Teller surface area characterization,Boehm titration,X-ray photoelectron spectroscopy and Fourier transform infrared spectroscopy,respectively.The dispersion of AuNPs on AC was observed by transmission electron microscopy and X-ray diffraction.The results indicated that the catalysts with acid treated supports showed improved dispersion than that of untreated one,which may be the result that the supports significantly increase the surface functional groups and remove the ash after acid treatment.
基金financially supported by the National Natural Science Foundation of China(No.21601137)Natural Science Foundation of Zhejiang Province(No.LQ16B010003)+2 种基金Basic Science and Technology Research Project of Wenzhou,Zhejiang Province(No.H20220001)the Special Basic Cooperative Research Programs of Yunnan Provincial Undergraduate Universities Association(No.202101BA070001-042)the Yunnan Province Young and Middle-aged Academic and Technical Leaders Reserve Talent Project(202105AC 160060)。
文摘Meeting the continuous glucose monitoring requirements of individuals necessitates the research and development of sensors with high sensitivity and stability.In this study,a straightforward strategy was proposed for synthesizing ultra-thin oxygen-rich graphitized carbon nanosheets(denoted as GCS-O).These nanosheets are obtained by calcining a topologically two-dimensional indium-based coordination polymer.Subsequently,the growth of FeNi Prussian blue analogue(PBA)on GCS-O effectively introduces active sites and increases the nitrogen content within the carbonaceous matrix.The resulting FeNi-PBA/GCS-O composite exhibits excellent glucose sensing performance with a broad linear range of 1 to 1300μmol·L^(-1).Meanwhile,it also achieves a high sensitivity of 2496μA·mmol^(-1)·L·cm^(-2),a limit of detection of 100nmol·L^(-1)(S/N=3),and commendable long-term durability.The relatively simple synthesis process,exceptional sensitivity,and satisfactory electrochemical sensing performance of FeNi-PBA/GCS-O open up new directions for biosensor applications.
基金The authors gratefully acknowledge for financial support from AGH University of Science and Technology(con-tract No.11.11.180.373.2011)and European Grant No.POIG.01.01.02.-00-015/09-00.
文摘In this study the catalytic properties of gold nanoparticles in electro-oxidation process of glucose, were investigated, taking into account, an influence of catalyst composition. Graphene oxide was applied and for electro-oxidation studies of glucose, cyclic voltamperometry was used. It was found that an application of graphene oxide sheets during catalyst synthesis have an influence on gold nanoparticles (AuNPs) size and size distribution. It was confirmed that the application of composite catalyst consisting of graphane-AuNPs significantly changes electro-oxidation of glucose shifting the potential of oxidation to higher positive values and increasing oxidation current.
基金supported by the National Nature Science Foundation of China(No.22269021)Tianshan Talent Project of Xinjiang Uygur Autonomous Region(No.2023TSYCQNTJ0039)the Open project of Key Laboratory in Xinjiang Uygur Autonomous Region of China(No.2023D04027).
文摘Hydrogen production coupled with small molecule oxidation derived by renewable energy power has been widely studied as an effective method to reduce energy consumption and prepare added value production.Here,the copper-cobalt phosphide with a multilevel structure has been designed based on the hard and soft acids and bases theory.The nanocone composed of lamellas presented a sharp tip,which a positive effect on the mass transfer enhanced by a local electric field,and the nanolamellas contain CoP/Cu_(3)P interface provide the highly selective active site for the gluconic acid(GNA)synthesis and hydrogen evolution.The catalyst can drive hydrogen evolution at 5 A·cm^(-2)up to 437 h without active decay,and the electrocatalytic glucose oxidation at anode presents high efficiency due to Cu(I)introduction and the synergetic effect between interfaces.Density functional theory(DFT)calculation shows that water splitting more readily occurs at the CoP,which provides adsorbed H and-OH for hydrogen evolution and glucose oxidation,respectively,and glucose adsorption more readily occurs at the Cu_(3)P,which presents lower conversion energy for high value-added GNA.Efficient hydrogen evolution and glucose conversion indicate its high intrinsic activity and synergetic effect.This work provides a special interface construction strategy for the catalytic conversion of hydrogen and small molecules.
文摘In this work, nitric oxide （NO） release coatings designed for intravenous amperometric glucose sensors are optimized through the use ofa polylactic acid （PLA） layer doped with a lipophilic diazeniumdiolated species that releases NO through a proton-driven mechanism. An Elast-Eon E2As polyurethane coating is used to both moderate NO release from the sensor surface and increase the sensor＇s linear detection range toward glucose. These sensors were evaluated for thromboresistance and in vivo glucose performance through implantation in rabbit veins. By maintaining NO flux on a similar scale to endogenous endothelial cells, implanted glucose sensors exhibited reduced surface clot formation which enables more accurate quantitative glucose measurements continuously. An in vivo time trace of implanted venous sensors demonstrated glucose values that correlated well with the discrete measurements of blood samples on a benchtop point-of-care sensor-based instrument. The raw measured currents from the implanted glucose sensors over 7 h time periods were converted to glucose concentration through use of both a one-point in vivo calibration and a calibration curve obtained in vitro within a bovine serum solution. Control sensors, assembled without NO release functionality, exhibit distinctive surface clotting over the 7 h in vivo implantation period.
基金the National Natural Science Foundation of China(Nos.22102128 and 22279097)the Fundamental Research Funds for the Central Universities(No.WUT:2022IVA168).
文摘Research on metal-organic framework(MOF)-based non-enzymatic glucose sensors usually ignores the impact of the surface reconstruction degree of MOF on the activity of catalyzing glucose oxidation.In this work,we choose zeolitic imidazolate framework-67(ZIF-67),which is commonly used in glucose sensing,as a representative to investigate the influence of reconstruction degree on its structure and glucose catalytic performance.By employing the electrochemical activation strategy,the activity of ZIF-67 in catalyzing glucose gradually increased with the prolongation of the activation time,reaching the optimum after 2 h activation.The detection sensitivity of the activated ZIF-67 was 19 times higher than that of the initial ZIF-67,and the limit of detection(LOD)was lowered from 7 to 0.4μM.Our findings demonstrate that the oxidation degree of ZIF-67 deepened rapidly with continuously activation and was basically reconstructed to CoOOH after 2 h activation,accompanied by a morphological change from cuboctahedral to flower-like.Simultaneously,theoretical investigation revealed that ZIF-67 is not suitable as a stable glucose sensor electrode since the adsorbed glucose molecules hasten the dissociation of ligands and the breaking of Co-N bond in ZIF-67.Therefore,our work has important implications for the rational design of next-generation MOF-based glucose sensors.
基金supported by the National Natural Science Foundation of China(21106054)~~
文摘Cupric oxide （CuO） and copper-cuprous oxide （Cu-Cu2O） nanoparticles were prepared by a simple hydrothermal method for the synthesis of diethyi carbonate （DEC） from ethanol. During these syntheses, varying NaOH and glucose concentrations were applied to explore and pinpoint the active species. It was found that PdCl2/CuO and PdCI2/Cu-Cu2O both catalysts exhibited good thermal stability and morphology. The results of catalytic tests showed that the catalysts prepared with 5 mol/L NaOH show superior catalytic performances because of their lower extent of agglomeration. It is noteworthy that the PdC12/Cu-Cu2O catalysts were the most active, especially the PdCl2/Cu-Cu2O catalyst prepared with 10 mmol glucose and having a higher Cu2O concentration. In Pd（ll）-Cu（II） （PdCl2/CuO） catalysts, there is an induction period, during which Pd（II） is reduced to Pd（0）, that must occur prior to electron transfer between Pd and Cu, and this can slow the catalytic reaction. To further pinpoint the active species, PdCl2/Cu-Cu2O catalysts with different Cu2O contents were prepared by controlling the dosages of glucose. The maximum DEC yield obtained with these catalysts was 151.9 mg.g-1.h-1, corresponding to an ethanol conversion of 7.2% and 97.9% DEC selectivity on an ethanol basis. Therefore, it was concluded that Cu＋ was the active species in this catalytic system, possibly because a higher proportion of Cu＋ reduces the Pd2＋ concentration and limits the CO oxidation side reaction, thus increasing DEC selectivity. In addition, Cu＋ promotes electron transfer between Pd and Cu without an induction period, which could also promote the catalytic activity.
基金supported by the National Natural Science Foundation of China (20990223)
文摘The effect of the reduction method on the catalytic properties of palladium catalysts supported on activated carbon for the oxidation of D-glucose was examined.The reduction methods investigated include argon glow discharge plasma reduction at room temperature,reduction by flowing hydrogen at elevated temperature,and reduction by formaldehyde at room temperature.The plasma-reduced catalyst shows the smallest metal particles with a narrow size distribution that leads to a much higher activity.The catalyst characteristics show that the plasma reduction increases the amount of oxygen-containing functional groups,which significantly enhances the hydrophilic property of the activated carbon and improves the dispersion of the metal.
基金the National Science Foundation(NSF)(No.CHE2247709)for grant supportH.M.acknowledges the National Institute of Health(NIH)(No.R01 CA252827).
文摘Since its creation,single-molecule optical imaging has revolutionized the study of catalytic processes,yet its application largely relies on probing fluorogenic reactions.To overcome this limitation,we propose the Fluorogenic Linkage Integration for Nonfluorescent Transformation(FLINT)approach,an imaging method to resolve nonfluorogenic reactions at the single-molecule level.Using glucose oxidation as a model reaction,we coupled this nonfluorogenic reaction with a fluorogenic Amplex Red(AR)→resorufin(RF)transformation to create a cascading reaction.This integration allowed us to monitor single-turnover events and extract key kinetic parameters for glucose oxidation despite their being invisible under the optical microscope.Our ensemble measurements combining cyclic voltammetry and fluorescence spectroscopy confirmed the cascade reaction mechanism and revealed first-order kinetics for both elementary reaction steps.At the single-molecule level,turnover time analysis provided detailed information on the reaction kinetics,distinguishing the relatively fast glucose oxidation from slower AR oxidation.We further confirmed the validity of the FLINT approach by comparing the catalytic performances of 5 nm gold nanoparticles(AuNPs)against that of 18×52 nm gold nanorods(AuNRs)and AuNP@DNA coronazymes.Furthermore,FLINT was used to evaluate the chiral selectivity of D-and L-glucose on coronazymes,suggesting the potential application of FLINT in enantioselective reactions.The FLINT approach is a significant advancement in single-molecule imaging as it enables the study of nonfluorogenic reactions with high spatiotemporal resolution.
文摘Background Studies have shown that complications in type 1 diabetes mellitus （T1DM） in children are mainly due to oxidative stress （OS）. Lipid peroxidation is the main marker of OS and iso-prostaglandin is a reliable biomarker of lipid peroxidation in type 2 diabetes mellitus （T2DM）. However, there have been few studies on OS in T1DM children with hyperglycemia and glucose fluctuations.
基金supported by the National Natural Science Foundation of China(52072035,51631001,21801015,51902023 and 51872030)the Fundamental Research Funds for the Central Universities(2017CX01003)+1 种基金Beijing Institute of Technology Research Fund Program for Young Scholarsthe Joint R&D Plan of Hong Kong,Macao,Taiwan,and Beijing(Z191100001619002).
文摘Water electrolysis is one of the most promising approaches for producing hydrogen.However,it has been hindered by the sluggishness of the anodic oxygen evolution reaction.In this work,we fabricated Ru-Co-Mn trimetallic alloy nanoparticles on N-doped carbon support(RuCoMn@NC)via the pyrolysis-adsorption-pyrolysis process using ZIF-67 as a precursor.The RuCoMn@NC catalyst exhibited excellent electrocatalytic performance for the hydrogen evolution reaction(HER)over a wide range of pH and glucose oxidation reaction in alkaline media.It showed exceptional HER activity in alkaline medium,superior to that of the commercial Pt/C catalyst(20 wt%),and good electrochemical stability.Further,a two-electrode alkaline electrolyzer pairing RuCoMn@NC as both cathode and anode was employed,and only a cell voltage of 1.63 V was required to attain a current density of 10 mA cm^(-2)in glucose electrolysis,which is about 270 mV lower than that in the overall water-splitting electrolyzer.This paper provides a promising method for developing efficiently bifunctional electrocatalysts driving redox electrocatalysis,and it would be beneficial to energy-saving electrolytic H_(2) production.
