Self-aggregation and sluggish transport kinetics of cathode materials would usually lead to the poor electrochemical performance for aqueous zinc-ion batteries(AZIBs).In this work,we report the construction of C@VO_(2...Self-aggregation and sluggish transport kinetics of cathode materials would usually lead to the poor electrochemical performance for aqueous zinc-ion batteries(AZIBs).In this work,we report the construction of C@VO_(2) composite via anti-aggregation growth and hierarchical porous carbon encapsulation.Both of the morphology of composite and pore structure of carbon layer can be regulated by tuning the adding amount of glucose.When acting as cathode applied for AZIBs,the C@VO_(2)-3:3 composite can deliver a high capacity of 281 m Ah g^(-1) at 0.2 A g^(-1).Moreover,such cathode also exhibits a remarkably rate capability and cyclic stability,which can release a specific capacity of 195 m Ah g^(-1) at 5 A g^(-1) with the capacity retention of 95.4%after 1000 cycles.Besides that,the evolution including the crystal structure,valence state and transport kinetics upon cycling were also deeply investigated.In conclusion,benefited from the synergistic effect of anti-aggregation morphology and hierarchical porous carbon encapsulation,the building of such C@VO_(2) composite can be highly expected to enhance the ion accessible site,boost the transport kinetics and thus performing a superior storage performance.Such design concept can be applied for other kinds of electrode materials and accelerating the development of highperformance AZIBs.展开更多
Fading mechanism of tin dioxide （SnO2） electrodes in lithium ion batteries has attracted much attentions, which is of great importance for the battery applications. In this paper, electrochemical lithiation-delithia...Fading mechanism of tin dioxide （SnO2） electrodes in lithium ion batteries has attracted much attentions, which is of great importance for the battery applications. In this paper, electrochemical lithiation-delithiation cycles of individual SnO2 nanowires were conducted in situ in a high-resolution transmission electron microscopy （TEM）. Major changes in volume with expan- sions of 170%~300% on SnO2 nanowire electrodes were observed during the first lithiation process in electrochemical cycling, including conversion reaction of SnO2 precursor to Li20 matrix and active lithium host Sn, and alloying of Sn with Li to form brittle Li-Sn alloy. SnO2 nanowire electrodes were inclined to suffer from thermal runaway condition in the first two cycles. During cycling, morphology and composition evolution of SnO2 nanowire electrodes were recorded. Cyclic lithiation and del- ithiation of the electrode demonstrated the phase transition between Lii3Sn5 and Sn. Metallic Sn clusters were formed and their sizes enlarged with increasing cycle times. Detrimental aggregation of Sn clusters caused pulverization in SnO2 nanowire elec- trodes, which broke the conduction and transport path for electrons and lithium ions. The real-time in situ TEM revealed fading mechanism provides important guidelines for the viable design of the SnO2 nanowire electrodes in lithium ion batteries.展开更多
Although humans have spent exactly 100 years combating Alzheimer’s disease (AD), the molecular mechanisms of AD remain unclear. Owing to the rapid growth of the oldest age groups of the popula-tion and the continuous...Although humans have spent exactly 100 years combating Alzheimer’s disease (AD), the molecular mechanisms of AD remain unclear. Owing to the rapid growth of the oldest age groups of the popula-tion and the continuous increase of the incidence of AD, it has become one of the crucial problems to modern sciences. It would be impossible to prevent or reverse AD at the root without elucidating its molecular mechanisms. From the point of view of metal-amyloid-β peptide (Aβ) interactions, we review the molecular mechanisms of AD, mainly including Cu2+ and Zn2+ inducing the aggregation of Aβ, cata-lysing the production of active oxygen species from Aβ, as well as interacting with the ion-channel-like structures of Aβ. Moreover, the development of therapeutic drugs on the basis of metal-Aβ interactions is also briefly introduced. With the increasingly rapid progress of the molecular mechanisms of AD, we are now entering a new dawn that promises the delivery of revolutionary developments for the control of dementias.展开更多
Extensive application of nuclear energy has caused widespread environmental uranium contamination.New detection approaches without complicated sample pretreatment and precision instruments are in demand for on-site an...Extensive application of nuclear energy has caused widespread environmental uranium contamination.New detection approaches without complicated sample pretreatment and precision instruments are in demand for on-site and in-time determination of uranyl ions in environmental monitoring, especially in an emergency situation. In this work, a simple and effective fluorescent sensor(Z)-N’-hydroxy-4-(1,2,2-triphenylvinyl)benzimidamide(TPE-A) with aggregation-induced emission(AIE) character was established and studied. It could realize to detect UO_(2)2+via quenching the fluorescence of its aggregation-induced emission, with good selectivity and sensitivity. Such strategy shows a wide linear range from 5.0 × 10^(-8)mol/L to 4.5 × 10^(-7)mol/L(R^(2)= 0.9988) with exceptional sensitivity reaching 4.7 × 10^(-9)mol/L, which is far below the limit for uranium in drinking water(30 μg/L, ca. 1.1 × 10-7mol/L) stipulated by the WHO.A response time less than four minutes make it rapid for uranyl ion measurement. It was applied for detection of uranyl ion in spiked river water samples with recoveries in the range of 98.7%-104.0%, comparable to those obtained by ICP-MS. With the advantages of portable apparatus, rapid detection process and high sensitivity, TPE-A can serve as a promising fluorescent sensor for the detection of UO_(2)2+in environmental water samples.展开更多
Colloidal particles,heterogeneous mixture with various organic components and continuous molecular weight(MW)distribution,is omnipresent in lake sediments and substantially influence the retention,transportation,and f...Colloidal particles,heterogeneous mixture with various organic components and continuous molecular weight(MW)distribution,is omnipresent in lake sediments and substantially influence the retention,transportation,and fate of contaminants in lake ecosystem.We sampled and extracted sedimentary colloids from different ecology regions in Taihu Lake,Jiangsu,East China,in June 2020,and they were further separated into four different particle size ranges by tangent ultrafiltration,and the properties of colloids were studied in various methods,including zeta potential analysis,transmission electron micrograph images(TEM),Fourier transformation infrared(FTIR),and 3D fluorescence.Results show that the surface of the colloids is covered with organic macromolecular substances,such as humuslike substances and protein-like substances.There were significant differences in molecular weight and fraction content of colloids in the sediments from macrophyte-dominant(MD)area and algae-dominant(AD)area in the lake.Colloids from MD area are mainly composed of humic acid,protein,and fulvic acid;the content of fulvic acid is lower than that of humic acid and protein.The humic acid exists mainly in small molecular weight(10-100 kDa),protein exists in mainly large molecular weight colloids(0.45-1μm).Colloids from AD area are mainly composed of humic acid,and mainly distributed in the molecular weight(10 kDa-0.45μm).The presence of humic acid inhibits effectively the agglomeration of the colloids.Especially,the stability of colloids is closely related to the molecular weight,with low molecular weight from MD area show higher stability.The existence of humic acid in colloids increases the electrostatic repulsion between colloidal particles,which can effectively inhibit the agglomeration of colloids,thus enhancing the stability of colloids.Furthermore,both monovalent and divalent electrolytes enhance colloidal aggregation,and the low-molecular-weight(LMW)colloid fraction exhibits higher stability efficiency than the high-molecular-weight(HM展开更多
Ferric and ferrous ion plays critical roles in bioprocesses,their influences in many fields have not been fully explored due to the lack of methods for quantification of ferric and ferrous ions in biological system or...Ferric and ferrous ion plays critical roles in bioprocesses,their influences in many fields have not been fully explored due to the lack of methods for quantification of ferric and ferrous ions in biological system or complex matrix.In this study,an M13 bacteriophage(phage) was engineered for use as a sensor for ferric and ferrous ions via the display of a tyrosine residue on the P8 coat protein.The interaction between the specific phenol group of tyrosine and Fe^(3+)./ Fe^(2+).was used as the sensor.Transmission electron microscopy showed aggregation of the tyrosine-displaying phages after incubation with Fe^(3+) and Fe^(2+).The aggregated phages infected the host bacterium inefficiently.This phenomenon could be utilized for detection of ferric and ferrous ions.For ferric ions,a calibration curve ranging from 200 nmol/L to 8 μmol/L with a detection limit of 58 nmol/L was acquired.For ferrous ions,a calibration curve ranging from 800 nmol/L to 8μmol/L with a detection limit of 641.7 nmol/L was acquired.The assay was specific for Fe^((3+)) and Fe^((2+)) when tested against Ni^(2+),Pb^(2+),Zn^(2+),Mn^(2+),Co^(2+),Ca^(2+),Cu^(2+),Cr^(3+),Ba^(2+),and K^+.The tyrosine displaying phage to Fe^(3+) and Fe^(2+) interaction would have plenty of room in application to biomatenals and bionanotechnology.展开更多
More and more nanomaterials enter the environment along with their production, application and deposal. They may alter the biological effect of pollutants already existing in the real environment by different interact...More and more nanomaterials enter the environment along with their production, application and deposal. They may alter the biological effect of pollutants already existing in the real environment by different interactions. Therefore efforts should also be paid to investigate the combined toxicity of nanomaterials and pollutants. Herein, we studied the combined toxicity of oxi- dized multi-walled carbon nanotubes （O-MWCNTs） and zinc ions on ceils. It is found that cytotoxicity of the combined O-MWCNTs and zinc ions elevates significantly, compared with O-MWCNTs or zinc ions alone. This result comes from the assays of cell morphology, cell viability and proliferation, cell membrane integrity, mitochondrial membrane potential and cell apoptosis. Mechanism studies indicate that O-MWCNTs absorb zinc ions and form slight aggregation. These enhance remark- ably the cellular uptake of O-MWCNTs, and thus induce the death of cells by bringing in more zinc ions into cells. Our study indicates that the existence of nanomaterials could change the bioconsequence of other pollutants and emphasizes the im- portance of the combined toxicity research in the presence of nanomaterials.展开更多
Copper ions can promote amyloid diseases that are associated with amyloid peptides, such as type 2 diabetes(T2D),Alzheimer's disease(AD), Parkinson's disease(PD), and amyotrophic lateral sclerosis(ALS). Howeve...Copper ions can promote amyloid diseases that are associated with amyloid peptides, such as type 2 diabetes(T2D),Alzheimer's disease(AD), Parkinson's disease(PD), and amyotrophic lateral sclerosis(ALS). However, the underlying molecular mechanism remains obscure. Here we present that Cu^(2+)is able to specifically bind to the backbone of T2D related human islet amyloid polypeptide(hIAPP) by forming a ring structure, which causes the reduction of Cu^(2+)to Cu^(+) to produce reactive oxygen species(ROS) and the modulation of hIAPP aggregation. Nuclear magnetic resonance spectroscopy showed that Cu^(2+)bound to the backbone of a turn region, His18-Ser21, which is critical for hIAPP aggregation.Ab initio calculations and x-ray absorption fine structure analyses revealed that Cu^(2+)simultaneously bound with both the amide nitrogen and carbonyl oxygen on the peptide backbone, resulting in a ring structure, and causing the reduction of Cu^(2+)to Cu^(+) to form a hIAPP-Cu^(+) complex. 2′,7′-dichlorodihydrofluorescin diacetate fluorescence measurements further indicated that this complex led to enhanced ROS levels in rat insulinoma cells. Additionally, thioflavin T fluorescence and atomic force microscopy measurements denoted that the backbone-Cu ring structure largely modulated hIAPP aggregation,including the inhibition of hIAPP fibrillation and the promotion of peptide oligomerization. These findings shed new light on the molecular mechanism of Cu^(2+)-induced amyloid toxicity involving both the enhancement of ROS and the modulation of hIAPP aggregation.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.51774203)the Shenzhen Science and Technology Program(Nos.JCYJ20200109105801725)。
文摘Self-aggregation and sluggish transport kinetics of cathode materials would usually lead to the poor electrochemical performance for aqueous zinc-ion batteries(AZIBs).In this work,we report the construction of C@VO_(2) composite via anti-aggregation growth and hierarchical porous carbon encapsulation.Both of the morphology of composite and pore structure of carbon layer can be regulated by tuning the adding amount of glucose.When acting as cathode applied for AZIBs,the C@VO_(2)-3:3 composite can deliver a high capacity of 281 m Ah g^(-1) at 0.2 A g^(-1).Moreover,such cathode also exhibits a remarkably rate capability and cyclic stability,which can release a specific capacity of 195 m Ah g^(-1) at 5 A g^(-1) with the capacity retention of 95.4%after 1000 cycles.Besides that,the evolution including the crystal structure,valence state and transport kinetics upon cycling were also deeply investigated.In conclusion,benefited from the synergistic effect of anti-aggregation morphology and hierarchical porous carbon encapsulation,the building of such C@VO_(2) composite can be highly expected to enhance the ion accessible site,boost the transport kinetics and thus performing a superior storage performance.Such design concept can be applied for other kinds of electrode materials and accelerating the development of highperformance AZIBs.
基金supported by the National Basic Research Program of China("973" project)(Grant Nos.2012CB933003,2013CB932601)the National Natural Science Foundation of China(Grant No.11027402)
文摘Fading mechanism of tin dioxide （SnO2） electrodes in lithium ion batteries has attracted much attentions, which is of great importance for the battery applications. In this paper, electrochemical lithiation-delithiation cycles of individual SnO2 nanowires were conducted in situ in a high-resolution transmission electron microscopy （TEM）. Major changes in volume with expan- sions of 170%~300% on SnO2 nanowire electrodes were observed during the first lithiation process in electrochemical cycling, including conversion reaction of SnO2 precursor to Li20 matrix and active lithium host Sn, and alloying of Sn with Li to form brittle Li-Sn alloy. SnO2 nanowire electrodes were inclined to suffer from thermal runaway condition in the first two cycles. During cycling, morphology and composition evolution of SnO2 nanowire electrodes were recorded. Cyclic lithiation and del- ithiation of the electrode demonstrated the phase transition between Lii3Sn5 and Sn. Metallic Sn clusters were formed and their sizes enlarged with increasing cycle times. Detrimental aggregation of Sn clusters caused pulverization in SnO2 nanowire elec- trodes, which broke the conduction and transport path for electrons and lithium ions. The real-time in situ TEM revealed fading mechanism provides important guidelines for the viable design of the SnO2 nanowire electrodes in lithium ion batteries.
基金Supported by the National Natural Science Foundation of China (Grant Nos. 30470408 and 20637010)the Youth Foundation of Science and Technology of Shanxi Province (Grant No. 2006021009)
文摘Although humans have spent exactly 100 years combating Alzheimer’s disease (AD), the molecular mechanisms of AD remain unclear. Owing to the rapid growth of the oldest age groups of the popula-tion and the continuous increase of the incidence of AD, it has become one of the crucial problems to modern sciences. It would be impossible to prevent or reverse AD at the root without elucidating its molecular mechanisms. From the point of view of metal-amyloid-β peptide (Aβ) interactions, we review the molecular mechanisms of AD, mainly including Cu2+ and Zn2+ inducing the aggregation of Aβ, cata-lysing the production of active oxygen species from Aβ, as well as interacting with the ion-channel-like structures of Aβ. Moreover, the development of therapeutic drugs on the basis of metal-Aβ interactions is also briefly introduced. With the increasingly rapid progress of the molecular mechanisms of AD, we are now entering a new dawn that promises the delivery of revolutionary developments for the control of dementias.
基金the financial support received from the National Natural Science Foundation of China (No. 21702193)China Academy of Engineering Physics (Nos. TP03201601, TP02201711 and JMJJ20190101)。
文摘Extensive application of nuclear energy has caused widespread environmental uranium contamination.New detection approaches without complicated sample pretreatment and precision instruments are in demand for on-site and in-time determination of uranyl ions in environmental monitoring, especially in an emergency situation. In this work, a simple and effective fluorescent sensor(Z)-N’-hydroxy-4-(1,2,2-triphenylvinyl)benzimidamide(TPE-A) with aggregation-induced emission(AIE) character was established and studied. It could realize to detect UO_(2)2+via quenching the fluorescence of its aggregation-induced emission, with good selectivity and sensitivity. Such strategy shows a wide linear range from 5.0 × 10^(-8)mol/L to 4.5 × 10^(-7)mol/L(R^(2)= 0.9988) with exceptional sensitivity reaching 4.7 × 10^(-9)mol/L, which is far below the limit for uranium in drinking water(30 μg/L, ca. 1.1 × 10-7mol/L) stipulated by the WHO.A response time less than four minutes make it rapid for uranyl ion measurement. It was applied for detection of uranyl ion in spiked river water samples with recoveries in the range of 98.7%-104.0%, comparable to those obtained by ICP-MS. With the advantages of portable apparatus, rapid detection process and high sensitivity, TPE-A can serve as a promising fluorescent sensor for the detection of UO_(2)2+in environmental water samples.
基金Supported by the National Natural Science Foundation of China(Nos.42007332,51979137)the Natural Science Foundation of Jiangsu Province(No.20KJB610001)。
文摘Colloidal particles,heterogeneous mixture with various organic components and continuous molecular weight(MW)distribution,is omnipresent in lake sediments and substantially influence the retention,transportation,and fate of contaminants in lake ecosystem.We sampled and extracted sedimentary colloids from different ecology regions in Taihu Lake,Jiangsu,East China,in June 2020,and they were further separated into four different particle size ranges by tangent ultrafiltration,and the properties of colloids were studied in various methods,including zeta potential analysis,transmission electron micrograph images(TEM),Fourier transformation infrared(FTIR),and 3D fluorescence.Results show that the surface of the colloids is covered with organic macromolecular substances,such as humuslike substances and protein-like substances.There were significant differences in molecular weight and fraction content of colloids in the sediments from macrophyte-dominant(MD)area and algae-dominant(AD)area in the lake.Colloids from MD area are mainly composed of humic acid,protein,and fulvic acid;the content of fulvic acid is lower than that of humic acid and protein.The humic acid exists mainly in small molecular weight(10-100 kDa),protein exists in mainly large molecular weight colloids(0.45-1μm).Colloids from AD area are mainly composed of humic acid,and mainly distributed in the molecular weight(10 kDa-0.45μm).The presence of humic acid inhibits effectively the agglomeration of the colloids.Especially,the stability of colloids is closely related to the molecular weight,with low molecular weight from MD area show higher stability.The existence of humic acid in colloids increases the electrostatic repulsion between colloidal particles,which can effectively inhibit the agglomeration of colloids,thus enhancing the stability of colloids.Furthermore,both monovalent and divalent electrolytes enhance colloidal aggregation,and the low-molecular-weight(LMW)colloid fraction exhibits higher stability efficiency than the high-molecular-weight(HM
基金funded by the National Natural Science Foundation of China (No. 31300829)Natural Science Foundation of Hubei Province of China (No. 2014CFC1117)Open Research Fund Program of the State Key Laboratory of Virology of China (No. 2015IOV002)
文摘Ferric and ferrous ion plays critical roles in bioprocesses,their influences in many fields have not been fully explored due to the lack of methods for quantification of ferric and ferrous ions in biological system or complex matrix.In this study,an M13 bacteriophage(phage) was engineered for use as a sensor for ferric and ferrous ions via the display of a tyrosine residue on the P8 coat protein.The interaction between the specific phenol group of tyrosine and Fe^(3+)./ Fe^(2+).was used as the sensor.Transmission electron microscopy showed aggregation of the tyrosine-displaying phages after incubation with Fe^(3+) and Fe^(2+).The aggregated phages infected the host bacterium inefficiently.This phenomenon could be utilized for detection of ferric and ferrous ions.For ferric ions,a calibration curve ranging from 200 nmol/L to 8 μmol/L with a detection limit of 58 nmol/L was acquired.For ferrous ions,a calibration curve ranging from 800 nmol/L to 8μmol/L with a detection limit of 641.7 nmol/L was acquired.The assay was specific for Fe^((3+)) and Fe^((2+)) when tested against Ni^(2+),Pb^(2+),Zn^(2+),Mn^(2+),Co^(2+),Ca^(2+),Cu^(2+),Cr^(3+),Ba^(2+),and K^+.The tyrosine displaying phage to Fe^(3+) and Fe^(2+) interaction would have plenty of room in application to biomatenals and bionanotechnology.
基金supported by the National Basic Research Program of China (2011CB933402)the National Natural Science Foundation of China (21371117, 31571024)
文摘More and more nanomaterials enter the environment along with their production, application and deposal. They may alter the biological effect of pollutants already existing in the real environment by different interactions. Therefore efforts should also be paid to investigate the combined toxicity of nanomaterials and pollutants. Herein, we studied the combined toxicity of oxi- dized multi-walled carbon nanotubes （O-MWCNTs） and zinc ions on ceils. It is found that cytotoxicity of the combined O-MWCNTs and zinc ions elevates significantly, compared with O-MWCNTs or zinc ions alone. This result comes from the assays of cell morphology, cell viability and proliferation, cell membrane integrity, mitochondrial membrane potential and cell apoptosis. Mechanism studies indicate that O-MWCNTs absorb zinc ions and form slight aggregation. These enhance remark- ably the cellular uptake of O-MWCNTs, and thus induce the death of cells by bringing in more zinc ions into cells. Our study indicates that the existence of nanomaterials could change the bioconsequence of other pollutants and emphasizes the im- portance of the combined toxicity research in the presence of nanomaterials.
基金Project supported by the National Natural Science Foundation of China (Grant Nos. 12074208 and 11375256)the Natural Science Foundation of Jiangsu Province (Grant No. BK20200176)+2 种基金the Natural Science Foundation of Jiangsu Higher Education Institutions of China (Grant Nos. 20KJB140020 and 19KJB140005)Fundamental Research Project from Changzhou Science and Technology (Grant No. CJ20200029)the Jiangsu Province High-level Innovative and Entrepreneurial Talents Introduction Plan。
文摘Copper ions can promote amyloid diseases that are associated with amyloid peptides, such as type 2 diabetes(T2D),Alzheimer's disease(AD), Parkinson's disease(PD), and amyotrophic lateral sclerosis(ALS). However, the underlying molecular mechanism remains obscure. Here we present that Cu^(2+)is able to specifically bind to the backbone of T2D related human islet amyloid polypeptide(hIAPP) by forming a ring structure, which causes the reduction of Cu^(2+)to Cu^(+) to produce reactive oxygen species(ROS) and the modulation of hIAPP aggregation. Nuclear magnetic resonance spectroscopy showed that Cu^(2+)bound to the backbone of a turn region, His18-Ser21, which is critical for hIAPP aggregation.Ab initio calculations and x-ray absorption fine structure analyses revealed that Cu^(2+)simultaneously bound with both the amide nitrogen and carbonyl oxygen on the peptide backbone, resulting in a ring structure, and causing the reduction of Cu^(2+)to Cu^(+) to form a hIAPP-Cu^(+) complex. 2′,7′-dichlorodihydrofluorescin diacetate fluorescence measurements further indicated that this complex led to enhanced ROS levels in rat insulinoma cells. Additionally, thioflavin T fluorescence and atomic force microscopy measurements denoted that the backbone-Cu ring structure largely modulated hIAPP aggregation,including the inhibition of hIAPP fibrillation and the promotion of peptide oligomerization. These findings shed new light on the molecular mechanism of Cu^(2+)-induced amyloid toxicity involving both the enhancement of ROS and the modulation of hIAPP aggregation.
