Prussian blue nanoparticles (PB NPs) have exhibited favorable anti-inflammatory effects in animal models,and have been proved to mimic three antioxidant enzymes: peroxidase,catalase,and superoxide dismutase.Whereas th...Prussian blue nanoparticles (PB NPs) have exhibited favorable anti-inflammatory effects in animal models,and have been proved to mimic three antioxidant enzymes: peroxidase,catalase,and superoxide dismutase.Whereas the oxidase-like activity of PB NPs has not been demonstrated.In this work,PB NPs with outstanding oxidase-like activity were demonstrated by virtue of the colorimetric substrate o-phenylenediamine (OPD).Interestingly,based on the oxidase-like activity,PB NPs can also catalytically oxidize vitamin B1 (VB1) to strongly fluorescent product in the physiological environment without the addition of other oxidants.Considering that VB1 has no toxicity and carcinogenicity comparing with OPD,a novel PB NPs-VB1 fluorescent sensor was further developed for simple,nontoxic,and rapid detection of ascorbic acid (AA) in foods and alkaline phosphatase (ALP) in human serum samples by taking advantage of the reduction of PB NPs to Prussian White by AA or enzymatic hydrolysate of ALP and ascorbic acid 2-phosphate (AA2P);leading to the decrease of fluorescence intensity.The extremely low detection limits of 44 nmol/L for AA and 72 mU/L for ALP as well as the excellent applicability in real samples were both obtained.Therefore,we envision that such a novel fluorescent probe would be potentially applied in the food analysis and clinic diagnosis fields.展开更多
The rational control of the active site of metal-organic frameworks(MOFs)derived nanomaterials is essential to build efficient bifunctional oxygen reduction/evolution reaction(ORR/OER)catalysts.Accordingly,through des...The rational control of the active site of metal-organic frameworks(MOFs)derived nanomaterials is essential to build efficient bifunctional oxygen reduction/evolution reaction(ORR/OER)catalysts.Accordingly,through designing and constructing a Co_(3)O_(4)-Co heterostructure embedded in Co,N co-doped carbon polyhedra derived(Co_(3)O_(4)-Co@NC)from the in-situ compositions of ZIF-67 and cobalt nanocrystals synthesized by the strategy of in-situ NaBH4 reduction,the dual-active site(Co_(3)O_(4)-Co and Co-N_(x))is synchronously realized in a MOFs derived nanomaterials.The formed Co_(3)O_(4)-Co@NC shows excellent bifunctional electrocatalytic activity with ultra-small potential gap(ΔE=E_(j=10)(OER)–E_(1/2)(ORR))of 0.72 V,which surpasses the commercial Pt/C and RuO_(2) catalysts.The theory calculation results reveal that the excellent bifunctional electrocatalytic activity can be attributed to the charge redistribution of Co of Co-N_(x) induced by the synergistic effects of well-tuned active sites of Co_(3)O_(4)-Co nanoparticle and Co-N_(x),thus optimizing the rate-determining step of the desorption of O_(2)^(*)intermediate in ORR and OH^(*)intermediate in OER.The rechargeable Zn-air batteries with our bifunctional catalysts exhibit superior performance as well as high cycling stability.This simple-effective optimization strategy offers prospects for tuning the active site of MOF derived bifunctional catalyst in electrochemical energy devices.展开更多
基金supported by the National Natural Science Foundation of China (No.22104103)the Program of Sichuan Department of Science and Technology,China (No.2022ZYFG0312)the Foundation of Sichuan Normal University,China (No.XJ20210223).
文摘Prussian blue nanoparticles (PB NPs) have exhibited favorable anti-inflammatory effects in animal models,and have been proved to mimic three antioxidant enzymes: peroxidase,catalase,and superoxide dismutase.Whereas the oxidase-like activity of PB NPs has not been demonstrated.In this work,PB NPs with outstanding oxidase-like activity were demonstrated by virtue of the colorimetric substrate o-phenylenediamine (OPD).Interestingly,based on the oxidase-like activity,PB NPs can also catalytically oxidize vitamin B1 (VB1) to strongly fluorescent product in the physiological environment without the addition of other oxidants.Considering that VB1 has no toxicity and carcinogenicity comparing with OPD,a novel PB NPs-VB1 fluorescent sensor was further developed for simple,nontoxic,and rapid detection of ascorbic acid (AA) in foods and alkaline phosphatase (ALP) in human serum samples by taking advantage of the reduction of PB NPs to Prussian White by AA or enzymatic hydrolysate of ALP and ascorbic acid 2-phosphate (AA2P);leading to the decrease of fluorescence intensity.The extremely low detection limits of 44 nmol/L for AA and 72 mU/L for ALP as well as the excellent applicability in real samples were both obtained.Therefore,we envision that such a novel fluorescent probe would be potentially applied in the food analysis and clinic diagnosis fields.
基金The authors acknowledge support from the National Natural Science Foundation of China(No.21875039)Minjiang Professorship(XRC-1677)+1 种基金Fujian province’s high level innovative and entrepreneurial talents(No.50012709)the Open Project Program of the State Key Laboratory of Photocatalysis on Energy and Environment(No.SKLPEE-201814),Fuzhou University.
文摘The rational control of the active site of metal-organic frameworks(MOFs)derived nanomaterials is essential to build efficient bifunctional oxygen reduction/evolution reaction(ORR/OER)catalysts.Accordingly,through designing and constructing a Co_(3)O_(4)-Co heterostructure embedded in Co,N co-doped carbon polyhedra derived(Co_(3)O_(4)-Co@NC)from the in-situ compositions of ZIF-67 and cobalt nanocrystals synthesized by the strategy of in-situ NaBH4 reduction,the dual-active site(Co_(3)O_(4)-Co and Co-N_(x))is synchronously realized in a MOFs derived nanomaterials.The formed Co_(3)O_(4)-Co@NC shows excellent bifunctional electrocatalytic activity with ultra-small potential gap(ΔE=E_(j=10)(OER)–E_(1/2)(ORR))of 0.72 V,which surpasses the commercial Pt/C and RuO_(2) catalysts.The theory calculation results reveal that the excellent bifunctional electrocatalytic activity can be attributed to the charge redistribution of Co of Co-N_(x) induced by the synergistic effects of well-tuned active sites of Co_(3)O_(4)-Co nanoparticle and Co-N_(x),thus optimizing the rate-determining step of the desorption of O_(2)^(*)intermediate in ORR and OH^(*)intermediate in OER.The rechargeable Zn-air batteries with our bifunctional catalysts exhibit superior performance as well as high cycling stability.This simple-effective optimization strategy offers prospects for tuning the active site of MOF derived bifunctional catalyst in electrochemical energy devices.