| Research background and purpose:Mucin 1（MUC1）is a membrane-associated glycoprotein that is overexpressed in a variety of malignancies,including breast,ovarian,lung,and pancreatic cancers.The development of a highly sensitive and selective mucin 1 detection method is of great significance for the early screening of cancer.Aptamers have high affinity and specificity for a variety of targets from small organic molecules to proteins,as well as good stability,low cost,high reusability and easy modification.They are effective strategies for biosensor applications and disease diagnosis.In this study,electrochemical aptasensors were constructed in combination with novel MXene nanocomposites and nucleic acid signal amplification strategies to achieve rapid and sensitive detection of MUC1,providing a new idea for the detection of trace tumor markers in blood.Materials and methods:1.Study on MUC1 electrochemical aptasensor based on MXene/Mo S2/Pd Pt NPs and Zr-MOF nanomaterialsA novel MXene/Mo S2/Pd Pt NPs nanomaterial and hierarchical porous Zr-MOFs（HP-Ui O-66）were prepared by chemical synthesis.The high porosity of HP-UIO-66 is used to improve the loading of Methylene blue（MB）.On MXene/Mo S2/Pd Pt NPs modified glassy carbon electrode,single strand DNA（c DNA）was attached to the electrode by covalent bond and complementary hybridized with c DNA when MUC1aptamer was added.In the presence of MUC1,MUC1 can bind specifically to the aptamer and form a MUC1 aptamer complex to fall off the electrode.The signal probe MB@HP-Ui O-66-s DNA is then hybridized with c DNA to produce an electrochemical signal to detect MUC1.Scanning electron microscope（SEM）,X-ray diffraction（XRD）,Energy dispersive spectrometer（EDS）,to verify the preparation of MXene/Mo S2/Pd Pt NPs and HP-Ui O-66.Cyclic voltammetry（CV）and electrochemical impedance spectroscopy（EIS）were used to characterize the preparation process of the sensor,and the optimal conditions for analysis and detection were studied,and the detection performance of the sensor was evaluated.2.Study on MUC1 electrochemical aptasensor based on few layered MXene/Mo S2/Pd-Pt NPs nanomaterials combined with hybrid chain reactionFirstly,bimetallic functionalized Mo S2/MXene nanomaterials（MXene/Mo S2/Pd Pt NPs）were synthesized to construct sensitive interfaces and covalently immobilized single-stranded DNA（c DNA）to identify MUC1 aptamers.MUC1 competes to bind aptamers from the electrode.Initiator S,hairpin probes H1 and H2 bind to the remaining c DNA on the electrode,triggering a hybridization chain reaction（HCR）.The manganese porphyrin（Mn TMPy P）was embedded into the HCR product chain byπ-πstacking,which promoted the decomposition of H2O2 and synergically catalyzed the HQ oxidation to enhance the electric signal,thus realizing the ultra-sensitive detection of MUC1.The morphology and distribution of elements were characterized by SEM,XRD and EDS to verify the successful preparation of MXene/Mo S2/Pd Pt NPs.Electrochemical methods（CV,EIS）were used to characterize the preparation process of the sensor,and the optimal conditions for analysis and detection were studied,and the detection performance of the sensor was evaluated.Results:1.Based on MXene/Mo S2/Pd Pt NPs and Zr-MOF MUC1 electrochemical aptasensor,electrochemical method of linear range for 1 pg/m L-10 ng/m L,limit of detection（LOD）1 pg/m L（S/N=3）.The MUC1 aptasensor showed good selectivity,reproducibility（RSD=4.5%）,and stability（ΔI changed by 20.76%within 20 days）.The recoveries of MUC1 were 94.88%-110.88%and RSD were lower than 3.93%,which showed good anti-interference.2.Based on MXene/Mo S2/Pd Pt NPs combined hybrid nanomaterials chain reaction MUC1 electrochemical aptasensor,LOD for 1 pg/m L（S/N=3）,linear range for 1 pg/m L-10 ng/m L.The MUC1 aptasensor showed good selectivity,reproducibility（RSD=4.2%）,and stability（10.3%change inΔI within 7 days）.The recoveries were95.0%-110.0%and RSD were lower than 4.41%when the actual samples were simulated to detect MUC1.Conclusion:An electrochemical biosensor based on MXene/Mo S2/Pd Pt NPs and HP-Ui O-66labeling was constructed for MUC1 detection.The large specific surface area of MXene/Mo S2 can provide more active sites,and Pd Pt NPs has excellent conductivity on the electrode surface,which can effectively promote electron transfer and improve the sensitivity of the biosensor.The porous structure of HP-Ui O-66 can encapsulate a large amount of MB to enhance the aptasensor response signal.The sensor has the characteristics of high sensitivity,good selectivity,stability and high repeatability in the process of detecting MUC1,which can provide technical support for the detection of MUC1 content in blood.Based on the excellent electrochemical performance of MXene nanocomposites,an ultra-sensitive electrochemical MUC1 aptasensor based on MXene/Mo S2/Pd Pt NPs nanomaterials combined with hybrid chain reaction was constructed.Mo S2 and Pd Pt NPs can prevent the reaccumulation of MXene,and increase the specific surface area and conductivity of the electrode.Subsequently,a hybrid chain reaction was triggered and the mimicking enzyme Mn TMPy P molecule was embedded into the ds DNA scaffold.The synergistic catalytic ability of Mn TMPy P and Pd Pt NPs can produce significantly amplified signals,greatly enhance the electrochemical response and improve the performance of the sensor. |
PDF Full Text Request