Zhenyu Lin

Metal–organic framework (MOF): a novel sensing platform for biomolecules

The metal-organic framework (MOF) was first utilized as the sensing platform for assaying biomolecules. It has also been demonstrated that this novel strategy is effective and reliable for detection of HIV DNA and thrombin with high sensitivity and selectivity.

A highly sensitive and selective “signal-on” electrochemiluminescent biosensor for mercury

A highly sensitive and selective electrochemiluminescent biosensor was designed for mercury(ii) based on T-Hg(2+)-T complex by using Ru(bpy)(3)(2+)-doped silica nanoparticles (Ru-SNPs) to label the oligonucleotides in order to improve the sensitivity.

Surface-Enhanced Electrochemiluminescence of Ru@SiO2 for Ultrasensitive Detection of Carcinoembryonic Antigen

Carcinoembryonic antigen (CEA) is recognized as a disease biomarker to reflect the existence of various cancers and tumors in the human body. Sensitive detection of CEA in body fluid is valuable for clinical diagnosis and treatment assessment of cancers. Herein, we present a new approach for ultrasensitive determination of CEA in human serum based on localized surface plasmon resonance (LSPR) enhanced electrochemiluminescence (ECL) of Ru(bpy)3(2+). In this surface-enhanced ECL (SEECL) sensing scheme, Ru(bpy)3(2+)-doped SiO2 nanoparticles (Ru@SiO2) act as ECL luminophores, and AuNPs are used as LSPR source to enhance the ECL signal. Two different kinds of aptamers specific to CEA are modified on the surface of Ru@SiO2 and AuNPs, respectively. In the presence of CEA, a multilayer of Ru@SiO2-AuNPs nanoarchitectures would be formed. Our investigation reveals that the ECL signal of Ru@SiO2 can be effectively enhanced by AuNPs. One layer of Ru@SiO2-AuNPs nanoarchitectures would generate about 3-fold ECL enhancement compared with the ECL of the nanoarchitectures without the presence of AuNPs. As much as 30-fold ECL enhancement could be obtained by a multilayer of Ru@SiO2-AuNPs nanoarchitectures. Under the optimal conditions, a detection limit of 1.52 × 10(-6) ng/mL of CEA in human serum was achieved. To the best of our knowledge, CEA assays with such a low LOD have never been reported for an ECL sensor.

Highly Selective and Sensitive Electrochemiluminescence Biosensor for p53 DNA Sequence Based on Nicking Endonuclease Assisted Target Recycling and Hyperbranched Rolling Circle Amplification

An ultrasensitive and specific electrochemiluminescence (ECL) biosensor has been designed for the p53 DNA sequence, which is based on cascade signal amplification of nicking endonuclease assisted target recycling and hyperbranched rolling circle amplification (HRCA). First of all, biotin modified hairpin capture DNA (HP) probe was immobilized on the surface of streptavidin magnespheres paramagnetic particles (PMPs). Target DNA hybridized with the loop portion of the HP probe, therefore unfolding HP to form a double-stranded DNA (dsDNA) containing the specific nicking site of the nicking endonuclease. Then, the nicking endonuclease recognized the specific nicking site and cleaved the HP into two pieces, liberating target DNA and the complementary sequence piece for the padlock probe. The intact target DNA would initiate the next cycle of hybridization and cleavage, thereby releasing multiple complementary sequences for the padlock probes. The liberated complementary sequences hybridized with the padlock probes, subsequently inducing the HRCA reaction and generating numerous dsDNA segments. Herein, Ru(phen)3(2+) was embedded into dsDNA and worked as ECL signal reporter. The reaction products were eventually pretreated by dialysis tube with the cutoff membrane to remove the residual Ru(phen)3(2+) in the solution for the following ECL measurements. Using this cascade amplification strategy, an ultrasensitive p53 DNA sequence detection method was developed with a wide linear range from 0.05 to 100 fM and a low detection limit of 0.02 fM. Moreover, this cascade amplified ECL biosensor had specific recognition capacity for noncomplementary and single- and double-base mismatched DNA. The proposed ECL biosensor might have a great potential in biomedical research and clinic analysis.

Electrochemiluminescence biosensor for ultrasensitive determination of ochratoxin A in corn samples based on aptamer and hyperbranched rolling circle amplification

Determination of ochratoxin A (OTA) is highly important for food safety control. In this study, a signal-on electrochemiluminescence (ECL) biosensor which combined the characteristics of high efficiency of hyperbranched rolling circle amplification (HRCA) and high selectivity of aptamer was developed for OTA determination. The capture probe DNA (CDNA) was firstly immobilized on the gold electrode surface through Au-S interaction, then the OTA aptamer was modified on the electrode surface through hybridization with CDNA. Since OTA can competitively bind with the aptamer due to their high affinity, which would induce the releasing of aptamer from the electrode surface. Subsequently, the free CDNA on the electrode surface can hybridize with the padlock probe and induce HRCA reaction subsequently. Thus, the HRCA products which contained large amount of double-stranded DNA (dsDNA) fragments can be accumulated on the electrode surface. Since Ru(phen)3(2+) can intercalate into the groove of dsDNA and acts as ECL indicator, high ECL intensity can be detected from the electrode surface. The enhanced ECL intensity has a linear relationship with OTA in the range of 0.05-500 pg/mL with a correlation coefficient of 0.9957, and the limit of detection (LOD) was 0.02 pg/mL. The developed biosensor has been applied to determine OTA concentration in the corn samples with satisfied results.

Label-free aptamer-based electrochemical impedance biosensor for 17β-estradiol

A novel aptamer-based label-free electrochemical impedance spectroscopy biosensor for 17β-estradiol has been fabricated. The aptamers were firstly immobilized on the gold electrode through Au-S interaction; the aptamer probe was then bound with the addition of 17β-estradiol to form the estradiol/aptamer complex on the electrode surface. This leads to a significantly larger interfacial electron transfer resistance than that without the addition of 17β-estradiol. The change in the resistance had a linear relationship with 17β-estradiol concentration in the range of 1.0 × 10(-8) to 1.0 × 10(-11) mol L(-1), with a detection limit of 2.0 × 10(-12) mol L(-1). The biosensor showed high selectivity to 17β-estradiol and good stability. The designed biosensor has been applied to detect 17β-estradiol in human urine with satisfactory results.

An electrochemiluminescent biosensor for glucose based on the electrochemiluminescence of luminol on the nafion/glucose oxidase/poly(nickel(II)tetrasulfophthalocyanine)/multi-walled carbon nanotubes modified electrode

A poly(nickel(II) tetrasulfophthalocyanine)/multi-walled carbon nanotubes composite modified electrode (polyNiTSPc/MWNTs) was fabricated by electropolymerization of NiTSPc on MWNTs-modified glassy carbon electrode (GCE). The modified electrode was found to be able to greatly improve the emission of luminol electrochemiluminescence (ECL) in a solution containing hydrogen peroxide. Glucose oxidase (GOD) was immobilized on the surface of polyNiTSPc/MWNTs modified GC electrode by Nafion to establish an ECL glucose sensor. Under the optimum conditions, the linear response range of glucose was 1.0x10(-6) to 1.0x10(-4) mol L(-1) with a detection limit of 8.0x10(-8) mol L(-1) (defined as the concentration that could be detected at the signal-to-noise ratio of 3). The ECL sensor showed an outstanding well reproducibility and long-term stability. The established method has been applied to determine the glucose concentrations in real serum samples with satisfactory results.

Metal–organic frameworks-based biosensor for sequence-specific recognition of double-stranded DNA

A simple, cost-efficient, sensitive and selective fluorescence sensor is developed for sequence-specific recognition of duplex DNA (ds-DNA) in vitro using metal-organic framework (MOF) as the sensing platform. N,N-Bis(2-hydroxy-ethyl)dithiooxamidatocopper(II) (H(2)dtoaCu) was chosen as the example MOF, because it strongly chemisorbs the dye-labeled probe TFO (triplex-forming oligonucleotide), and quenches fluorescence from the dye. In the presence of target ds-DNA (the PPT of HIV RNA, a 16-bp ds-DNA sequence), the TFO could interact with the major groove in ds-DNA (via Hoogsteen hydrogen bonding) to form a rigid triplex structure, resulting in fluorescence recovery. The enhanced fluorescence signal has a relationship with the ds-DNA concentration, the detection limit is as low as 1.3 nmol L(-1) (S/N = 3) with good selectivity, which is lower than that based on a graphene oxide platform and electrochemical-DNA sensor.

Novel composites of multifunctional Fe3O4@Au nanofibers for highly efficient glycoprotein imprinting

A kind of surface glycoprotein imprinting over magnetic Fe3O4@Au multifunctional nanofibers (NFs) was developed and investigated. Magnetic Fe3O4@Au nanoparticles (NPs) as the core materials were modified consecutively with aniline, 3-aminophenylboronic acid (APBA) and acrylic acid to introduce boronic acids and polymerizable double bonds. With horseradish peroxidase (HRP) as a glycoprotein template, thin protein-imprinted films were fabricated via radical induced graft copolymerization of monomers on the surface of the multifunctional NFs. Experimental results show that the magnetic multifunctional Fe3O4@Au NFs can not only direct the selective occurrence of imprinting polymerization, but also drive glycoprotein templates into the polymer through reversible covalent complex formation. The results show that the imprinted NFs reached saturated adsorption at 0.3 mg mL-1 within 90 min and exhibited significant specific recognition towards the template protein. Moreover, the molecularly imprinted polymers (MIPs) were used to electrochemically detect HRP with good linearity in the range of low concentrations from 0.01 to 0.30 mg mL-1 through molecular recognition of K3[Fe(CN)6] current response. The detection limit of this method was found to be 0.005 mg mL-1 (S/N = 3). The synthetic strategy paves the way for preparation of functional nanomaterials by molecular imprinting technique and direct detection of proteins in a more convenient, simpler and cheaper way.

CEA fluorescence biosensor based on the FRET between polymer dots and Au nanoparticles.

Polymer dots were employed as luminophors to design a fluorescence biosensor for carcinoembryonic antigen (CEA) with high sensitivity and selectivity; the increased fluorescence intensity is proportional to CEA concentration in the range of 0.1-10 ng mL(-1).