A sensitive label-free fluorescent aptasensing strategy for the detection of adenosine triphosphate（ATP）has been developed with a metallocyclodextrin, tris（bipyridine）ruthenium（Ⅱ） complex containing six cyclode...A sensitive label-free fluorescent aptasensing strategy for the detection of adenosine triphosphate（ATP）has been developed with a metallocyclodextrin, tris（bipyridine）ruthenium（Ⅱ） complex containing six cyclodextrin units（6CD-Ru）, which exhibited much stronger emission signal compared to the parent compound Ru（bpy）_3Cl_2. Furthermore, the emission spectrum showed that the ATP-aptamer（ss DNA）could increase the fluorescence intensity of 6CD-Ru dramatically, attributed to the interaction between aptamer and cyclodextrin, which could provide protection to the ruthenium core from the quenching of emission by oxygen in the solution. With the addition of ATP, the interaction between aptamer and cyclodextrins on 6CD-Ru was diminished, since the ATP/aptamer complex had the priority to be formed,leading to the corresponding reduction of fluorescence intensity, which could be utilized to detect ATP quantitatively. A linear relationship was displayed between the fluorescence and the logarithm of ATP concentrations in the range from 1 nmol/L to 1μmmol/L with the detection limit of 0.5 nmol/L（S/N = 3）.The proposed fluorescent aptasensing strategy exhibited high sensitivity and specificity, without any labeling or amplification procedures, and it could also be applied for the detection of many other aptamer-specific targets.展开更多
The application of metal-organic frameworks(MOFs)nanozymes in biosensing has been extensively investigated,however,till now there is still no report on photoelectrochemical(PEC)sensing based on enzyme memetic properti...The application of metal-organic frameworks(MOFs)nanozymes in biosensing has been extensively investigated,however,till now there is still no report on photoelectrochemical(PEC)sensing based on enzyme memetic properties of MOFs.To further expand the utilization of MOFs nanozymes in biosensing,we developed a label-free homogenous PEC aptasensor for the detection of VEGF_(165),an important cancer biomarker,based on the DNA-regulated peroxidase-mimetic activity of Fe-MIL-88,a type of MOFs.In this strategy,the peroxidase-mimetic property of MOFs is integrated with the label-free homogeneous PEC sensing approach,and highly sensitive detection of VEGF_(165)is obtained with a detection limit down to 33 fg/m L,superior or comparable to the previously reported values.Moreover,this approach displays outstanding specificity,and has been successfully used to detect VEGF_(165)added in diluted serum samples.As far as we know,it is the first example to employ the peroxidase-like activity of MOFs in PEC biosensing,which may find potential application in bioanalysis and early disease diagnosis.展开更多
Recent advancements in nanotechnology have spotlighted the catalytic potential of nanozymes, particularly single-atom nanozymes(SANs), which are pivotal for innovations in biosensing and medical diagnostics. Among oth...Recent advancements in nanotechnology have spotlighted the catalytic potential of nanozymes, particularly single-atom nanozymes(SANs), which are pivotal for innovations in biosensing and medical diagnostics. Among others, DNA stands out as an ideal biological regulator. Its inherent programmability and interaction capabilities allow it to significantly modulate nanozyme activity. This study delves into the dynamic interplay between DNA and molybdenum-zinc single-atom nanozymes(Mo-Zn SANs). Using molecular dynamics simulations, we uncover how DNA influences the peroxidase-like activities of Mo-Zn SANs, providing a foundational understanding that broadens the application scope of SANs in biosensing.With these insights as a foundation, we developed and demonstrated a model aptasensor for point-ofcare testing(POCT), utilizing a label-free colorimetric approach that leverages DNA-nanozyme interactions to achieve high-sensitivity detection of lysozyme. Our work elucidates the nuanced control DNA exerts over nanozyme functionality and illustrates the application of this molecular mechanism through a smartphone-assisted biosensing platform. This study not only underscores the practical implications of DNA-regulated Mo-Zn SANs in enhancing biosensing platforms, but also highlights the potential of single-atom nanozyme technology to revolutionize diagnostic tools through its inherent versatility and sensitivity.展开更多
基金financially supported by the National Natural Science Foundation of China(Nos.21275054,21405049,31300819)
文摘A sensitive label-free fluorescent aptasensing strategy for the detection of adenosine triphosphate（ATP）has been developed with a metallocyclodextrin, tris（bipyridine）ruthenium（Ⅱ） complex containing six cyclodextrin units（6CD-Ru）, which exhibited much stronger emission signal compared to the parent compound Ru（bpy）_3Cl_2. Furthermore, the emission spectrum showed that the ATP-aptamer（ss DNA）could increase the fluorescence intensity of 6CD-Ru dramatically, attributed to the interaction between aptamer and cyclodextrin, which could provide protection to the ruthenium core from the quenching of emission by oxygen in the solution. With the addition of ATP, the interaction between aptamer and cyclodextrins on 6CD-Ru was diminished, since the ATP/aptamer complex had the priority to be formed,leading to the corresponding reduction of fluorescence intensity, which could be utilized to detect ATP quantitatively. A linear relationship was displayed between the fluorescence and the logarithm of ATP concentrations in the range from 1 nmol/L to 1μmmol/L with the detection limit of 0.5 nmol/L（S/N = 3）.The proposed fluorescent aptasensing strategy exhibited high sensitivity and specificity, without any labeling or amplification procedures, and it could also be applied for the detection of many other aptamer-specific targets.
基金funded by the National Natural Science Foundation of China(Nos.22174083 and 22076090)Shandong Provincial Natural Science Foundation(No.ZR2020ZD37)Shandong Province Higher Educational Program for Young Innovation Talents。
文摘The application of metal-organic frameworks(MOFs)nanozymes in biosensing has been extensively investigated,however,till now there is still no report on photoelectrochemical(PEC)sensing based on enzyme memetic properties of MOFs.To further expand the utilization of MOFs nanozymes in biosensing,we developed a label-free homogenous PEC aptasensor for the detection of VEGF_(165),an important cancer biomarker,based on the DNA-regulated peroxidase-mimetic activity of Fe-MIL-88,a type of MOFs.In this strategy,the peroxidase-mimetic property of MOFs is integrated with the label-free homogeneous PEC sensing approach,and highly sensitive detection of VEGF_(165)is obtained with a detection limit down to 33 fg/m L,superior or comparable to the previously reported values.Moreover,this approach displays outstanding specificity,and has been successfully used to detect VEGF_(165)added in diluted serum samples.As far as we know,it is the first example to employ the peroxidase-like activity of MOFs in PEC biosensing,which may find potential application in bioanalysis and early disease diagnosis.
基金supported by the Science and Technology Research Project from Education Department of Jilin Province (No. JJKH20231296KJ)the Natural Science Foundation of Science and Technology Department of Jilin Province (Joint Fund Project) (No. YDZJ202201ZYTS340)+9 种基金the Fundamental Research Funds for the Central Universities (No. 2412022ZD013)the Science and Technology Development Plan Project of Jilin Province (Nos. SKL202302030, SKL202402017, 20210204126YY, 20230204113YY, 20240602003RC, 20210402059GH)the National Natural Science Foundation of China (Nos. 22174137, 22322410, 92372102 and 22073094)the Cooperation Funding of Changchun with Chinese Academy of Sciences (No. 22SH13)the Capital Construction Fund Projects within the Budget of Jilin Province (No. 2023C042–5)the University Level Scientific Research Projects of Ordinary Universities in Xinjiang Uygur Autonomous Region (No. 2022YQSN002)the State Key Laboratory of Molecular Engineering of Polymers (Fudan University) (No. K2024–11)the Program for Young Scholars in Regional Development of CASthe essential support of the Network and Computing Center, CIAC, CASthe Computing Center of Jilin Province。
文摘Recent advancements in nanotechnology have spotlighted the catalytic potential of nanozymes, particularly single-atom nanozymes(SANs), which are pivotal for innovations in biosensing and medical diagnostics. Among others, DNA stands out as an ideal biological regulator. Its inherent programmability and interaction capabilities allow it to significantly modulate nanozyme activity. This study delves into the dynamic interplay between DNA and molybdenum-zinc single-atom nanozymes(Mo-Zn SANs). Using molecular dynamics simulations, we uncover how DNA influences the peroxidase-like activities of Mo-Zn SANs, providing a foundational understanding that broadens the application scope of SANs in biosensing.With these insights as a foundation, we developed and demonstrated a model aptasensor for point-ofcare testing(POCT), utilizing a label-free colorimetric approach that leverages DNA-nanozyme interactions to achieve high-sensitivity detection of lysozyme. Our work elucidates the nuanced control DNA exerts over nanozyme functionality and illustrates the application of this molecular mechanism through a smartphone-assisted biosensing platform. This study not only underscores the practical implications of DNA-regulated Mo-Zn SANs in enhancing biosensing platforms, but also highlights the potential of single-atom nanozyme technology to revolutionize diagnostic tools through its inherent versatility and sensitivity.
