Graphene-based chemiluminescence resonance energy transfer for homogeneous immunoassay.

We report on chemiluminescence resonance energy transfer (CRET) between graphene nanosheets and chemiluminescent donors. In contrast to fluorescence resonance energy transfer, CRET occurs via nonradiative dipole-dipole transfer of energy from a chemiluminescent donor to a suitable acceptor molecule without an external excitation source. We designed a graphene-based CRET platform for homogeneous immunoassay of C-reactive protein (CRP), a key marker for human inflammation and cardiovascular diseases, using a luminol/hydrogen peroxide chemiluminescence (CL) reaction catalyzed by horseradish peroxidase. According to our results, anti-CRP antibody conjugated to graphene nanosheets enabled the capture of CRP at the concentration above 1.6 ng mL(-1). In the CRET platform, graphene played a key role as an energy acceptor, which was more efficient than graphene oxide, while luminol served as a donor to graphene, triggering the CRET phenomenon between luminol and graphene. The graphene-based CRET platform was successfully applied to the detection of CRP in human serum samples in the range observed during acute inflammatory stress.

[1]  M. Pumera,et al.  Nucleic acid functionalized graphene for biosensing. , 2012, Chemistry.

[2]  Qian Xi,et al.  A graphene sheet as an efficient electron acceptor and conductor for photoinduced charge separation , 2011 .

[3]  R. Yu,et al.  Graphene oxide-peptide conjugate as an intracellular protease sensor for caspase-3 activation imaging in live cells. , 2011, Angewandte Chemie.

[4]  Zhihong Liu,et al.  Biosensing platform based on fluorescence resonance energy transfer from upconverting nanocrystals to graphene oxide. , 2011, Angewandte Chemie.

[5]  Renfu Li,et al.  Time-resolved FRET biosensor based on amine-functionalized lanthanide-doped NaYF4 nanocrystals. , 2011, Angewandte Chemie.

[6]  Xiang Cai,et al.  Synergistic antibacterial brilliant blue/reduced graphene oxide/quaternary phosphonium salt composite with excellent water solubility and specific targeting capability. , 2011, Langmuir : the ACS journal of surfaces and colloids.

[7]  Sook Hee Ku,et al.  Graphene–Biomineral Hybrid Materials , 2011, Advanced materials.

[8]  Yan Liu,et al.  Investigation on fluorescence quenching of dyes by graphite oxide and graphene , 2011 .

[9]  Jicun Ren,et al.  Gold nanoparticles based chemiluminescent resonance energy transfer for immunoassay of alpha fetoprotein cancer marker. , 2011, Analytica chimica acta.

[10]  Jing Li,et al.  Hemin-graphene hybrid nanosheets with intrinsic peroxidase-like activity for label-free colorimetric detection of single-nucleotide polymorphism. , 2011, ACS nano.

[11]  R. Ruoff,et al.  Toward practical gas sensing with highly reduced graphene oxide: a new signal processing method to circumvent run-to-run and device-to-device variations. , 2011, ACS nano.

[12]  Huimin Zhao,et al.  Distance-independent quenching of quantum dots by nanoscale-graphene in self-assembled sandwich immunoassay. , 2010, Chemical communications.

[13]  K. Loh,et al.  A graphene oxide-organic dye ionic complex with DNA-sensing and optical-limiting properties. , 2010, Angewandte Chemie.

[14]  Yunqi Liu,et al.  Controllable Synthesis of Graphene and Its Applications , 2010, Advanced materials.

[15]  H. Ju,et al.  Fluorescence resonance energy transfer between quantum dots and graphene oxide for sensing biomolecules. , 2010, Analytical chemistry.

[16]  Lifeng Yan,et al.  Preparation of graphene by the rapid and mild thermal reduction of graphene oxide induced by microwaves , 2010 .

[17]  C. Nuckolls,et al.  Energy transfer from individual semiconductor nanocrystals to graphene. , 2010, ACS nano.

[18]  Filip Braet,et al.  Carbon nanomaterials in biosensors: should you use nanotubes or graphene? , 2010, Angewandte Chemie.

[19]  K. L. Sebastian,et al.  Distance dependence of fluorescence resonance energy transfer , 2009 .

[20]  K. L. Sebastian,et al.  Long range resonance energy transfer from a dye molecule to graphene has (distance)(-4) dependence. , 2009, The Journal of chemical physics.

[21]  K. L. Sebastian,et al.  Resonance energy transfer from a dye molecule to graphene. , 2008, The Journal of chemical physics.

[22]  Francisco Ciruela,et al.  Fluorescence-based methods in the study of protein-protein interactions in living cells. , 2008, Current opinion in biotechnology.

[23]  Zhuang Liu,et al.  PEGylated nanographene oxide for delivery of water-insoluble cancer drugs. , 2008, Journal of the American Chemical Society.

[24]  G. Rao,et al.  A novel method for monitoring monoclonal antibody production during cell culture , 2008, Biotechnology and bioengineering.

[25]  E. Samulski,et al.  Synthesis of water soluble graphene. , 2008, Nano letters.

[26]  Huifeng Qian,et al.  A resonance energy transfer between chemiluminescent donors and luminescent quantum-dots as acceptors (CRET). , 2006, Angewandte Chemie.

[27]  Jing C. Zhou,et al.  Immunoassays for cortisol using antibody-doped sol–gel silica , 2004 .

[28]  Nader Rifai,et al.  Blood Pressure, C-Reactive Protein, and Risk of Future Cardiovascular Events , 2003, Circulation.

[29]  T. Zyung.  Synthesis, Properties, and Applications of Graphene , 2011 .

[30]  P. Ihalainen,et al.  Rapid electrochemiluminoimmunoassay of human C-reactive protein at planar disposable oxide-coated silicon electrodes. , 2006, Analytical chemistry.