Ultrasensitive detection of multiple diseases markers is of great importance in improving diagnostic accuracy,precision,and efficiency.A versatile Au nanozyme Raman probe strategy was employed to develop an ultrasensi...Ultrasensitive detection of multiple diseases markers is of great importance in improving diagnostic accuracy,precision,and efficiency.A versatile Au nanozyme Raman probe strategy was employed to develop an ultrasensitive multiplex surface-enhanced Raman scattering(SERS)immunosensor using encoded silica photonic crystal beads(SPCBs).The efficient Au nanozyme Raman probe strategy was constructed using a robust Au nanozyme with high dual enzyme-like activity and SERS activity.On the one hand,Au nanozyme tags with oxidase-like activity can catalyze the oxidation of Raman-inactive 3,3,5,5-tetramethylbenzidine(TMB)to Raman-active oxidized TMB(ox-TMB)in the presence of O_(2).On the other hand,Au nanozyme tags with peroxidase-like activity can catalyze Raman-inactive TMB to Ramanactive ox-TMB in the presence of H_(2)O_(2).This dual catalysis action results in many Raman-active reporter molecules(ox-TMB)enabling highly sensitive detection.Meanwhile,the Au nanozyme as an extraordinary SERS substrate further enhances the detection signals of these Raman reporter molecules.Using reflection peaks of different SPCBs to encode tumor markers,an ultrasensitive multiplex SERS immunosensor was developed for detection of carcinoembryonic antigen(CEA)and alpha-fetoprotein(AFP),which exhibited wide linear ranges of 0.001-100 ng/m L for CEA and 0.01-1000 ng/m L for AFP,accompanied by low detection limits of 0.66 pg/m L for CEA and 9.5 pg/m L for AFP,respectively.This work demonstrates a universal and promising nanozyme Raman probe strategy to develop ultrasensitive multiplex SERS immunosensors for precise clinical diagnosis of disease.展开更多
基金financially supported by National Natural Science Foundation of China(Nos.21475116,21575125 and 22474124)the National Natural Science Foundation of Jiangsu Province(Nos.BK20221370,BK20211362)+5 种基金Key University Natural Science Foundation of Jiangsu-Province(No.20KJA150004)the Project for Science and Technology of Yangzhou(No.YZ2022074)the Project for Yangzhou City and Yangzhou University corporation(No.YZ2023204)Cross cooperation project of Subei Peoples’Hospital of Jiangsu Province(No.SBJC220009)the Open Research Fund of State Key Laboratory of Analytical Chemistry for Life Science(No.SKLACLS2405)Postgraduate Research&Practice Innovation Program of Jiangsu Province(No.KYCX24_3728)。
文摘Ultrasensitive detection of multiple diseases markers is of great importance in improving diagnostic accuracy,precision,and efficiency.A versatile Au nanozyme Raman probe strategy was employed to develop an ultrasensitive multiplex surface-enhanced Raman scattering(SERS)immunosensor using encoded silica photonic crystal beads(SPCBs).The efficient Au nanozyme Raman probe strategy was constructed using a robust Au nanozyme with high dual enzyme-like activity and SERS activity.On the one hand,Au nanozyme tags with oxidase-like activity can catalyze the oxidation of Raman-inactive 3,3,5,5-tetramethylbenzidine(TMB)to Raman-active oxidized TMB(ox-TMB)in the presence of O_(2).On the other hand,Au nanozyme tags with peroxidase-like activity can catalyze Raman-inactive TMB to Ramanactive ox-TMB in the presence of H_(2)O_(2).This dual catalysis action results in many Raman-active reporter molecules(ox-TMB)enabling highly sensitive detection.Meanwhile,the Au nanozyme as an extraordinary SERS substrate further enhances the detection signals of these Raman reporter molecules.Using reflection peaks of different SPCBs to encode tumor markers,an ultrasensitive multiplex SERS immunosensor was developed for detection of carcinoembryonic antigen(CEA)and alpha-fetoprotein(AFP),which exhibited wide linear ranges of 0.001-100 ng/m L for CEA and 0.01-1000 ng/m L for AFP,accompanied by low detection limits of 0.66 pg/m L for CEA and 9.5 pg/m L for AFP,respectively.This work demonstrates a universal and promising nanozyme Raman probe strategy to develop ultrasensitive multiplex SERS immunosensors for precise clinical diagnosis of disease.