Photocatalytic CO_(2)reduction to produce high value-added carbon-based fuel has been proposed as a promising approach to mitigate global warming issues.However,the conversion efficiency and product selectivity are st...Photocatalytic CO_(2)reduction to produce high value-added carbon-based fuel has been proposed as a promising approach to mitigate global warming issues.However,the conversion efficiency and product selectivity are still low due to the sluggish dynamics of transfer processes involved in proton-assisted multi-electron reactions.Lowering the formation energy barriers of intermediate products is an effective method to enhance the selectivity and productivity of final products.In this study,we aim to regulate the surface electronic structure of Bi_(2)WO_(6)by doping surface chlorine atoms to achieve effective photocatalytic CO_(2)reduction.Surface Cl atoms can enhance the absorption ability of light,affect its energy band structure and promote charge separation.Combined with DFT calculations,it is revealed that surface Cl atoms can not only change the surface charge distribution which affects the competitive adsorption of H_(2)O and CO_(2),but also lower the formation energy barrier of intermediate products to generate more intermediate*COOH,thus facilitating CO production.Overall,this study demonstrates a promising surface halogenation strategy to enhance the photocatalytic CO_(2)reduction activity of a layered structure Bi-based catalyst.展开更多
Heart failure(HF)is a clinical hallmark of cardiovascular syndrome leading to substantial morbidity,repeated hospitalization,and enormous healthcare expenditure.As elderly populations continue to increase,biomarker-gu...Heart failure(HF)is a clinical hallmark of cardiovascular syndrome leading to substantial morbidity,repeated hospitalization,and enormous healthcare expenditure.As elderly populations continue to increase,biomarker-guided diagnosis and treatment for age-related cardiac decline have become essential.Accumulating evidence demonstrates that N-terminal proBNP(NT-proBNP)can provide a unique window into the diagnosis and risk stratification with HF.Herein,a simple yet robust aptasensor is developed for on-site recognizing the NT-proBNP by its targeting aptamer,thus achieving the accurate diagnosis of HF.This aptasensing system is prepared by absorbing the fluorophore-labeled aptamer strand onto the graphene oxide(GO),leading to efficient quenching without possible off-site signal leakage.The aptamer strand can specifically identify target NT-proBNP molecules via a versatile conformational transformation,resulting in the desorption of the aptamer-NTproBNP complexes from GO and re-generation fluorescence signal,thus allowing sensitive detection of NT-proBNP in 37 clinical blood samples.Taking advantage of the high specificity of aptamer-guaranteed recognitions of NT-proBNP,this aptasensor system readily achieves better diagnostic performance for HF than commercially adopted chemiluminescence immunoassay(Siemens,CLIA)in hospitals in terms of accuracy(89.2%vs 83.8%),specificity(89.5%vs 84.2%),and positive predictive value(88.9%vs 83.3%).This work provides a stable option for the diagnosis and treatment of elderly HF-related diseases inclinics.展开更多
纳米酶的催化活性很大程度上依赖于纳米材料自身的晶体结构和理化性质.本研究可控合成了三种具有不同晶体结构的羟基氧化铁(α-FeOOH、β-FeOOH、γ-FeOOH)纳米晶,并系统研究了其类过氧化物酶活性的差异及其机制.结果表明,相比另外两种...纳米酶的催化活性很大程度上依赖于纳米材料自身的晶体结构和理化性质.本研究可控合成了三种具有不同晶体结构的羟基氧化铁(α-FeOOH、β-FeOOH、γ-FeOOH)纳米晶,并系统研究了其类过氧化物酶活性的差异及其机制.结果表明,相比另外两种晶体结构,γ-FeOOH具有更高的类过氧化物酶活性,其催化常数分别是α-FeOOH和β-FeOOH的2.0和2.6倍,这归因于γ-FeOOH表面的Fe^(2+)/Fe^(3+)高于α-FeOOH和β-FeOOH.进一步基于γ-FeOOH的优异类过氧化物酶活性,以维生素B1为底物,本文建立了一种快速、高灵敏、高选择性的荧光新方法用于Hg^(2+)检测,其检测范围为10~100 nM,检出限为2 n M,并成功应用于日用化妆品中Hg^(2+)的含量测定.这项工作为通过调控晶体结构获得高效催化活性的酶模拟物提供了有效途径,并基于纳米酶催化原理开发了一种检测Hg^(2+)的新方法.展开更多
基金supported by the National Natural Science Foundation of China(Grant No.51708078)Natural Science Foundation of Chongqing(Grant No.CSTB2022NSCQ-MSX0815)+2 种基金Science and Technology Research Program of Chongqing Municipal Education Commission(Grant No.KJQN202200542)the Chongqing Innovative Research Group Project(Grant No.CXQT21015)Foundation of Chongqing Normal University(22XLB022).
文摘Photocatalytic CO_(2)reduction to produce high value-added carbon-based fuel has been proposed as a promising approach to mitigate global warming issues.However,the conversion efficiency and product selectivity are still low due to the sluggish dynamics of transfer processes involved in proton-assisted multi-electron reactions.Lowering the formation energy barriers of intermediate products is an effective method to enhance the selectivity and productivity of final products.In this study,we aim to regulate the surface electronic structure of Bi_(2)WO_(6)by doping surface chlorine atoms to achieve effective photocatalytic CO_(2)reduction.Surface Cl atoms can enhance the absorption ability of light,affect its energy band structure and promote charge separation.Combined with DFT calculations,it is revealed that surface Cl atoms can not only change the surface charge distribution which affects the competitive adsorption of H_(2)O and CO_(2),but also lower the formation energy barrier of intermediate products to generate more intermediate*COOH,thus facilitating CO production.Overall,this study demonstrates a promising surface halogenation strategy to enhance the photocatalytic CO_(2)reduction activity of a layered structure Bi-based catalyst.
基金supported by the National Natural Science Foundation of China(81972020 and 22204012)Chongqing Innovation Research Group Project(CXQT21015)+2 种基金Natural Science Foundation of Chongqing(cstc2021ycjh-bgzxm0113 and CSTB2022NSCQ-MSX0466)Startup Founds of Chongqing Normal University(22XLB010)supported by the Chongqing YouthExpert Studio.
文摘Heart failure(HF)is a clinical hallmark of cardiovascular syndrome leading to substantial morbidity,repeated hospitalization,and enormous healthcare expenditure.As elderly populations continue to increase,biomarker-guided diagnosis and treatment for age-related cardiac decline have become essential.Accumulating evidence demonstrates that N-terminal proBNP(NT-proBNP)can provide a unique window into the diagnosis and risk stratification with HF.Herein,a simple yet robust aptasensor is developed for on-site recognizing the NT-proBNP by its targeting aptamer,thus achieving the accurate diagnosis of HF.This aptasensing system is prepared by absorbing the fluorophore-labeled aptamer strand onto the graphene oxide(GO),leading to efficient quenching without possible off-site signal leakage.The aptamer strand can specifically identify target NT-proBNP molecules via a versatile conformational transformation,resulting in the desorption of the aptamer-NTproBNP complexes from GO and re-generation fluorescence signal,thus allowing sensitive detection of NT-proBNP in 37 clinical blood samples.Taking advantage of the high specificity of aptamer-guaranteed recognitions of NT-proBNP,this aptasensor system readily achieves better diagnostic performance for HF than commercially adopted chemiluminescence immunoassay(Siemens,CLIA)in hospitals in terms of accuracy(89.2%vs 83.8%),specificity(89.5%vs 84.2%),and positive predictive value(88.9%vs 83.3%).This work provides a stable option for the diagnosis and treatment of elderly HF-related diseases inclinics.
文摘纳米酶的催化活性很大程度上依赖于纳米材料自身的晶体结构和理化性质.本研究可控合成了三种具有不同晶体结构的羟基氧化铁(α-FeOOH、β-FeOOH、γ-FeOOH)纳米晶,并系统研究了其类过氧化物酶活性的差异及其机制.结果表明,相比另外两种晶体结构,γ-FeOOH具有更高的类过氧化物酶活性,其催化常数分别是α-FeOOH和β-FeOOH的2.0和2.6倍,这归因于γ-FeOOH表面的Fe^(2+)/Fe^(3+)高于α-FeOOH和β-FeOOH.进一步基于γ-FeOOH的优异类过氧化物酶活性,以维生素B1为底物,本文建立了一种快速、高灵敏、高选择性的荧光新方法用于Hg^(2+)检测,其检测范围为10~100 nM,检出限为2 n M,并成功应用于日用化妆品中Hg^(2+)的含量测定.这项工作为通过调控晶体结构获得高效催化活性的酶模拟物提供了有效途径,并基于纳米酶催化原理开发了一种检测Hg^(2+)的新方法.
