| With the highly rapid development of human society,the economy has been greatly improved,but the issues of environment,diseases,medicine and others related to people have become more and more impact on in human beings.Therefore,it is extremely important to develop the high sensitivity,high selectivity,accurate and fast detection methods to environmental pollutants,disease markers,food and drugs,and various types of sensors have emerged.In this paper,six chemiluminescence sensors were constructed based on aptamers with high specific recognition ability and different signal amplification strategies,which achieved high sensitivity,high selectivity,accurate and rapid detection of various targets.（1）A novel chemiluminescence（CL）sensor for insulin（INS）detection with high selectivity and high sensitivity was proposed based on aptamer recognition and oligonucleotide-gold nanoparticles functionalized nanosilica@graphene oxide aerogels.Firstly,nano-silica@graphene oxide aerogels（Si O2@GOAG）with abundant pore distribution,large specific surface area and good biocompatibility were prepared.The multifunctional composite material ss DNA-Au NPs/IGA3/Si O2@GOAG was obtained when the insulin aptamer IGA3 as the recognition element,and oligonucleotide chain-functionalized gold nanoparticles（ss DNA-Au NPs）as the CL signal amplifying material were functionalized on Si O2@GOAG,and the composite was used to construct a CL sensor for INS detection.INS will bind to IGA3when INS exists,and ss DNA-Au NPs will be released.Released ss DNA-Au NPs can catalyze the luminol-H2O2 CL reaction to generate strong luminescence intensity for quantitative detection of INS.The linear range of the sensor to detect INS was 7.5×10-12～5.0×10-9 mol/L,and the detection limit was 1.6×10-12 mol/L.The results showed that ss DNA-Au NPs/IGA3/Si O2@GOAG enabled the sensor have high selectivity and sensitivity,and was successfully used for insulin detection in recombinant human insulin injection.（2）A chemiluminescence sensor for streptomycin（STR）detection with high selectivity and sensitivity was constructed based on aptamer recognition and G-quadruplex-mimicking enzyme（G-DNAzyme）modified three-dimensional graphene composites.Firstly,β-cyclodextrin and ionic liquid functionalized graphene oxide aerogel（β-CD/IL@GOGA）was prepared,and graphene oxide aerogel（GOGA）with a large specific surface area was used as the framework material.Hydroxyl-richβ-cyclodextrin（β-CD）and ionic liquid（IL）containing a large number of stable ions enhance the biocompatibility and stability of the composite,respectively.Then streptomycin aptamer（S-Apt）and G-DNAzyme were continuously immobilized on the surface ofβ-CD/IL@GOGA.Finally,G-DNAzyme/S-Apt/β-CD/IL@GOGA was successfully used to construct a CL sensor for STR detection.S-Apt with specific recognition ability for the target and G-DNAzyme as the catalyst of luminol-H2O2 CL system improved the selectivity and sensitivity of the sensor,respectively.When STR exists,G-DNAzyme is released from the surface of S-Apt/β-CD/IL@GOGA to catalyze the CL reaction due to the specific recognition and binding ability between STR and S-Apt,so as to realize the highly sensitive and selective detection of STR.The sensor had a linear range of 1.4×10-12～2.8×10-9 mol/L and a detection limit of 9.2×10-14 mol/L,and showed excellent selectivity,reproducibility and stability.The sensor was successfully used for STR detection in cucumber and milk samples.（3）A target-triggered signal CL sensor was constructed for prostate-specific antigen（PSA）detection based on aptamer-encapsulated luminol hollow porous silica.Luminol was used as a chemiluminescence illuminant,and it was encapsulated in the cavity of hollow porous silica by aptamers to prepare Apt/Luminol/HPSi O2.Then,Apt/Luminol/HPSi O2 was used to construct a target-triggered CL sensor,which realized the high selectivity and sensitivity detection of PSA.When PSA exists,PSA and its aptamer（Apt）specifically recognize and bind together,and Apt falls off from the surface of the silicon material,so that luminol is released and triggers the luminol-H2O2 reaction,and at the same time horseradish peroxidase（HRP）is regarded as a catalyst,so a CL sensor with a target-triggered signal for PSA detection is successfully constructed.Under optimal conditions,the detection limit of the sensor was 0.27 pg/m L,and the linear range was 0.001 to 100 ng/m L.The sensor had good selectivity,reproducibility and stability,which provides a new method for the detection of PSA with high sensitivity,high selectivity and accuracy.（4）A novel CL sensor for detection of thrombin was constructed based on double aptamer recognition and encapsulation of hematin on mesoporous silica.Firstly,aptamer1-encapsulated hematin mesoporous silica（Apt1/hematin/M-Si O2）and aptamer 2-modified magnetic microspheres（Apt2/NH2-MS）were synthesized.The material was used to construct a CL sensor and realized the detection of thrombin（THR）.The thrombin samples were pretreated and separated by the specific recognition ability between the aptamer（Apt2）in Apt2/NH2-MS and the target molecule THR.Then,THR/Apt2/NH2-MS and Apt1 on Apt1/hematin/M-Si O2 are re-recognized to form Apt1/THR/Apt2/NH2-MS to realize dual aptamer recognition.The generation of Apt1/THR/Apt2/NH2-MS disengages Apt1 from the M-Si O2 surface,and release hematin.The novel catalytic system of luminol-H2O2-hematin exhibits strong CL strength in the presence of luminol and H2O2.Thus,a sandwich-type CL sensor with dual aptamer recognition and hematin catalysis was constructed for THR detection.The sensor had a linear range of 7.5×10-15～2.5×10-10 mol/L and a detection limit of 2.2×10-15 mol/L,and showed good selectivity,reproducibility and stability.The sensor was also successfully applied to the detection of THR in human serum samples.（5）An"turn on"CL sensor for alpha-fetoprotein（AFP）detection was constructed based on oligonucleotide strand-functionalized magnetic graphene oxide（MGO-c DNA/Apt-luminol）,copper-based organic framework composites co-modified by Au and Zn O nanoparticles（Zn ONPs-Au@Cu MOFs）,and aptamer as a recognition element.Magnetic graphene oxide（MGO）was functionalized by the complementary DNA of AFP aptamer（c DNA）,and then ligated with aptamer-modified luminol（Apt-luminol）by the complementary base pairing principle,so the functionalized magnetic graphene oxide（MGO-c DNA/Apt-luminol）with excellent selectivity as a magnetic separation material was prepared.The synergistic effect of Zn ONPs and Au@Cu MOFs significantly enhanced the catalytic performance of Zn ONPs-Au@Cu MOFs towards the luminol-H2O2 system.When AFP is present,AFP specifically recognizes Apt on MGO-c DNA/Apt-luminol,so that luminol is released and triggers the CL reaction.The released luminol is catalyzed by Zn ONPs-Au@Cu MOFs,and produces the strong CL intensity.Therefore,a highly selective and sensitive CL sensor is constructed for AFP detection.The linear range of the sensor was1.0×10-4～50 ng/m L,and the detection limit was 4.2×10-5 ng/m L.The sensor showed good selectivity,reproducibility and stability,and was finally successfully used in the detection of AFP in human serum samples.（6）A CL sensor for simultaneous detection of alpha-fetoprotein（AFP）and carcinoembryonic antigen（CEA）was constructed based on dual aptamers modified magnetic silicon composites.Firstly,Si O2@Fe3O4 was prepared,and polydiallyldimethylam-monium chloride（PDDA）was loaded on Si O2@Fe3O4.Then,Au NPs/PDDA-Si O2@Fe3O4 was synthesized through the electrostatic interaction between positively charged PDDA and negatively charged Au NPs.Then the complementary strand of CEA（c DNA）and the aptamer of AFP（Apt1）were linked to Au NPs/PDDA-Si O2@Fe3O4 through thiol groups.Then,the CEA aptamer（Apt2）and G-DNAzyme were sequentially connected to c DNA through the base complementary pairing principle to obtain final material Au NPs/PDDA-Si O2@Fe3O4-c DNA（Apt1）/Apt2/G-DNAzyme.The prepared composite was used to construct a CL sensor to simultaneously detect CEA and AFP.When AFP exists,it binds to Apt1 on the surface of the composite material,which hinders the catalytic ability of surface Au NPs to luminol-H2O2,and realizes the detection of AFP.When CEA exists,it specifically recognizes and binds to Apt2,and G-DNAzyme is released into solution.Released G-DNAzyme catalyzes the luminol-H2O2reaction,and the determination of CEA is realized.After the apply of dual-aptamer functionalized magnetic silicon,the simultaneous detection of AFP and CEA are achieved in the magnetic medium and supernatant,respectively,after simple magnetic separation by a magnet.The linear ranges of the sensor for the detection of AFP and CEA were 1.0×10-4～1.0 ng/m L and 0.0001～0.5 ng/m L,respectively,and the detection limits were 6.7×10-5ng/m L and 3.2×10-5ng/m L,respectively.Finally,the sensor was successfully used for the simultaneous detection of AFP and CEA in human serum samples,which provides an alternative new method for the simultaneous detection of multiple components in the early clinical diagnosis of liver cancer. |
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