荧光石墨烯量子点的制备及应用
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摘要
由于具有独特的量子限域和边界效应,石墨烯量子点(GQDs)碳基纳米材料表现出特殊的性质和诸多潜在应用.文中概括了近年来在GQDs制备方面的研究进展,包括"自上而下"方法利用水热、电化学和化学氧化等把大片石墨变为GQDs的方法,以及"自下而上方法"利用含碳有机小分子为前驱体,通过溶液化学、超声波和微波等方法实现碳原子重组制得GQDs的方法.同时,介绍了GQDs在成像技术、生物传感和电化学分析等领域的应用情况.最后指出,由于GQDs的发光机理还是一个开放性的课题,因此结合GQDs制备方法来研究其发光性质,将是未来该领域的研究重点.
Due to the unique quantum connement and edge effects,graphene quantum dots(GQDs) have exhibited extraordinary properties and potential applications. Herein,the advances on the preparation of GQDs in recent years are summarized,including the "top to down"routine from the graphite sheets through hydrothermal,electrochemical,and chemical oxidation methods,and the "down to up"routine from the carbon-contained organic molecules through solvochemical,sonochemical,and microwave methods. In addition,the applications of the GQDs in optical imaging,biosensor,and electrochemistry analytical fields are introduced. And based on the investigation status of the fluorescent mechanism of GQDs,it is pointed out that combining with the preparation of GQDs,the optical properties of GQDs should be especially studied in the future.
Due to the unique quantum connement and edge effects,graphene quantum dots(GQDs) have exhibited extraordinary properties and potential applications. Herein,the advances on the preparation of GQDs in recent years are summarized,including the "top to down"routine from the graphite sheets through hydrothermal,electrochemical,and chemical oxidation methods,and the "down to up"routine from the carbon-contained organic molecules through solvochemical,sonochemical,and microwave methods. In addition,the applications of the GQDs in optical imaging,biosensor,and electrochemistry analytical fields are introduced. And based on the investigation status of the fluorescent mechanism of GQDs,it is pointed out that combining with the preparation of GQDs,the optical properties of GQDs should be especially studied in the future.
引文
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[40]LI Y,ZHANG L,HUANG J,et al.Fluorescent graphene quantum dots with a boronic acid appended bipyridinium salt to sense monosaccharides in aqueous solution[J].Chemical Communications,2013,49(45):5180-5182.
[41]WANG Y,ZHANG L,LIANG R,et al.Using graphene quantum dots as photoluminescent probes for protein kinase sensing[J].Analytical Chemistry,2013,85(19):9148-9155.
[42]ZHU X,ZENG L,XU M,et al.A glassy carbon electrode modified with electrochemically reduced graphene for simultaneous determination of guanine and adenine[J].Analytical Methods,2012,4(9):2935-2939.
[43]ZHU X,LIANG Y,ZUO X,et al.Novel water-soluble multi-nanopore graphene modified glassy carbon electrode for simultaneous determination of dopamine and uric acid in the presence of ascorbic acid[J].Electrochimica Acta,2014,143:366-373.
[44]ZHU X,JIAO Q,ZHANG C,et al.Electropolymerization of graphene and 5-[o-(4-bromine amyloxy)phenyl]-10,15,20-triphenylporphrin(o-Br PETPP)composite film electrode for the electrocatalytic oxidation of indirubin[J].Journal of Electroanalytical Chemistry,2012,681:133-138.
[45]ZHU X,JIAO Q,ZUO X,et al.An electrochemical sensor based on carbon nano-fragments andβ-cyclodextrin composite-modified glassy carbon electrode for the determination of Rutin[J].Journal of the Electrochemical Society,2013,160(10):H699-H703.
[46]ZHU X,JIAO Q,ZHANG C,et al.Amperometric nonenzymatic determination of glucose based on a glassy carbon electrode modified with nickel(II)oxides and graphene[J].Microchimica Acta,2013,180(5/6):477-483.
[47]RAZMI H,MOHAMMADREZAEI R.Graphene quantum dots as a new substrate for immobilization and direct electrochemistry of glucose oxidase:application to sensitive glucose determination[J].Biosensors and Bioelectronics,2013,41:498-504.
[48]WANG X,CHEN L,SU X,et al.Electrochemical immunosensor with graphene quantum dots and apoferritin-encapsulated Cu nanoparticles double-assisted signal amplification for detection of avian leukosis virus subgroup J[J].Biosensors and Bioelectronics,2013,47:171-177.
[49]HOU J,BEI F,WANG M,et al.Electrochemical determination of malachite green at graphene quantum dots-gold nanoparticles multilayers-modified glassy carbon electrode[J].Journal of Applied Electrochemistry,2013,43(7):689-696.
[50]ZHAO J,CHEN G,ZHU L,et al.Graphene quantum dots-based platform for the fabrication of electrochemical biosensors[J].Electrochemistry Communications,2011,13(1):31-33.
[51]ZHANG Y,WU C,ZHOU X,et al.Graphene quantum dots/gold electrode and its application in living cell H2O2detection[J].Nanoscale,2013,5(5):1816-1819.
[52]LI L,JI J,FEI R,et al.A facile microwave avenue to electrochemiluminescent two-color Graphene quantum dots[J].Advanced Functional Materials,2012,22(14):2971-2979..
[53]LU J,YAN M,GE L,et al.Electrochemiluminescence of blue-luminescent graphene quantum dots and its application in ultrasensitive aptasensor for adenosine triphosphate detection[J].Biosensors and Bioelectronics,2013,47:271-277.
[54]ZHOU Y,QU Z,ZENG Y,et al.A novel composite of graphene quantum dots and molecularly imprinted polymer for fluorescent detection of paranitrophenol[J].Biosensors and Bioelectronics,2014,52:317-323.
[55]TIAN J,ZHAO H,QUAN X,et al.Fabrication of graphene quantum dots/silicon nanowires nanohybrids for photoelectrochemical detection of microcystin-LR[J].Sensors and Actuators B:Chemical,2014,196:532-538.
[2]LI L,WU G,YANG G,et al.Focusing on luminescent graphene quantum dots:current status and future perspectives[J].Nanoscale,2013,5(10):4015-4039.
[3]LIN L,RONG M,LUO F,et al.Luminescent graphene quantum dots as new fluorescent materials for environmental and biological applications[J].Trends in Analytical Chemistry,2014,54:83-102.
[4]王娇娇,冯苗,詹红兵.石墨烯量子点的制备[J].化学进展,2013,25(1):86-94.WANG J J,FENG M,ZHAN H B.Advances in preparation of graphene quantum dos[J].Progress in Chemistry,2013,25(1):86-94.
[5]CUI R,LIU C,SHEN J,et al.Gold nanoparticle-colloidal carbon nanosphere hybrid material:preparation,characterization,and application for an amplified electrochemical immunoassay[J].Advanced Functional Materials,2008,18(15):2197-2204.
[6]DONG X,MI X,ZHAO W,et al.Cd S nanoparticles functionalized colloidal carbon particles:preparation,characterization and application for electrochemical detection of thrombin[J].Biosensors and Bioelectronics,2011,26(8):3654-3659.
[7]ZHU X,ZHAO T,NIE Z,et al.Non-redox modulated fluorescence strategy for sensitive and selective ascorbic acid detection with highly photoluminescent nitrogen-doped carbon nanoparticles via solid-state synthesis[J].Analytical Chemistry,2015,87(16):8524-8530.
[8]ZHU X,ZHAO T,NIE Z,et al.Nitrogen-doped carbon nanoparticle modulated turn-on fluorescent probes for histidine detection and its imaging in living cells[J].Nanoscale,2016,8(4):2205-2211.
[9]PAN D,ZHANG J,LI Z,et al.Hydrothermal route for cutting graphene sheets into blue-luminescent graphene quantum dots[J].Advanced Materials,2010,22(6):734-738.
[10]PAN D,GUO L,ZHANG J,et al.Cutting sp2clusters in graphene sheets into colloidal graphene quantum dots with strong green fluorescence[J].Journal of Materials Chemistry,2012,22(8):3314-3318.
[11]ZHU X,XIAO X,ZUO X,et al.Hydrothermal preparation of photoluminescent graphene quantum dots characterized excitation-independent emission and its application as a bioimaging reagent[J].Particle&Particle Systems Characterization,2014,31(7):801-809.
[12]ZHU X,ZUO X,HU R,et al.Hydrothermal synthesis of two photoluminescent nitrogen-doped graphene quantum dots emitted green and khaki luminescence[J].Materials Chemistry and Physics,2014,147(3):963-967.
[13]KOSYNKIN D,HIGGINBOTHAM A,SINITSKII A,et al.Longitudinal unzipping of carbon nanotubes to form graphene nanoribbons[J].Nature,2009,458(7240):872-876.
[14]ZHU S,ZHANG J,QIAO C,et al.Strongly green-photoluminescent graphene quantum dots for bioimaging applications[J].Chemical Communications,2011,47(24):6858-6860.
[15]LIU Q,GUO B,RAO Z,et al.Strong two-photon-induced fluorescence from photostable,biocompatible nitrogendoped graphene quantum dots for cellular and deep-tissue imaging[J].Nano Letters,2013,13(6):2436-2441.
[16]BAO L,ZHANG Z,TIAN Z,et al.Electrochemical tuning of luminescent carbon nanodots:from preparation to luminescence mechanism[J].Advanced Materials,2011,23(48):5801-5806.
[17]LI Y,HU Y,ZHAO Y,et al.An electrochemical avenue to green-luminescent graphene quantum dots as potential electron-acceptors for photovoltaics[J].Advanced Materials,2011,23(6):776-780.
[18]LI Y,ZHAO Y,CHENG H,et al.Nitrogen-doped graphene quantum dots with oxygen-rich functional groups[J].Journal of the American Chemical Society,2011,134(1):15-18.
[19]SHINDE D,PILLAI V.Electrochemical preparation of luminescent graphene quantum dots from multiwalled carbon nanotubes[J].Chemistry-A European Journal,2012,18(39):12522-12528.
[20]ZHANG M,BAI L,SHANG W,et al.Facile synthesis of water-soluble,highly fluorescent graphene quantum dots as a robust biological label for stem cells[J].Journal of Materials Chemistry,2012,22(15):7461-7467.
[21]ANANTHANARAYANAN A,WANG X,ROUTH P,et al.Facile synthesis of graphene quantum dots from 3D graphene and their application for Fe3+sensing[J].Advanced Functional Materials,2014,24(20):3021-3026.
[22]PENG J,GAO W,GUPTA B K,et al.Graphene quantum dots derived from carbon fibers[J].Nano Letters,2012,12(2):844-849.
[23]DONG Y,CHEN C,ZHENG X,et al.One-step and high yield simultaneous preparation of single-and multi-layer graphene quantum dots from CX-72 carbon black[J].Journal of Materials Chemistry,2012,22(18):8764-8766.
[24]SUN Y,WANG S,LI C,et al.Large scale preparation of graphene quantum dots from graphite with tunable fluorescence properties[J].Physical Chemistry Chemical Physics,2013,15(24):9907-9913.
[25]SWAIN A,LI D,BAHADUR D.UV-assisted production of ferromagnetic graphitic quantum dots from graphite[J].Carbon,2013,57:346-356.
[26]LI L,YAN X.Colloidal graphene quantum dots[J].The Journal of Physical Chemistry Letters,2010,1(17):2572-2576.
[27]DONG Y,SHAO J,CHEN C,et al.Blue luminescent graphene quantum dots and graphene oxide prepared by tuning the carbonization degree of citric acid[J].Carbon,2012,50(12):4738-4743.
[28]TANG L,JI R,CAO X,et al.Deep ultraviolet photoluminescence of water-soluble self-passivated graphene quantum dots[J].ACS Nano,2012,6(6):5102-5110.
[29]GOKHALE R,SINGH P.Blue luminescent graphene quantum dots by photochemical stitching of small aromatic molecules:fluorescent nanoprobes in cellular imaging[J].Particle&Particle Systems Characterization,2014,31(4):433-438.
[30]DONG Y,LI G,ZHOU N,et al.Graphene quantum dot as a green and facile sensor for free chlorine in drinking water[J].Analytical Chemistry,2012,84(19):8378-8382.
[31]CHAKRABORTI H,SINHA S,GHOSH S,et al.Interfacing water soluble nanomaterials with fluorescence chemosensing:graphene quantum dot to detect Hg2+in 100%aqueous solution[J].Materials Letters,2013,97:78-80.
[32]JU J,CHEN W.Synthesis of highly fluorescent nitrogendoped graphene quantum dots for sensitive,label-free detection of Fe(III)in aqueous media[J].Biosensors and Bioelectronics,2014,58:219-225.
[33]VAN TAM T,TRUNG B,KIM H,et al.One-pot synthesis of N-doped graphene quantum dots as a fluorescent sensing platform for Fe3+ions detection[J].Sensors and Actuators B:Chemical,2014,202:568-573.
[34]HUANG H,LIAO L,XU X,et al.The electron-transfer based interaction between transition metal ions and photoluminescent graphene quantum dots(GQDs):a platform for metal ion sensing[J].Talanta,2013,117:152-157.
[35]WANG F,GU Z,LEI W,et al.Graphene quantum dots as a fluorescent sensing platform for highly efficient detection of copper(II)ions[J].Sensors and Actuators B:Chemical,2014,190:516-522.
[36]RAN X,SUN H,PU F,et al.Ag Nanoparticle-decorated graphene quantum dots for label-free,rapid and sensitive detection of Ag+and biothiols[J].Chemical Communications,2013,49(11):1079-1081.
[37]BAI J,ZHANG L,LIANG R,et al.Graphene quantum dots combined with europium ions as photoluminescent probes for phosphate sensing[J].Chemistry-A European Journal,2013,19(12):3822-3826.
[38]FAN L,HU Y,WANG X,et al.Fluorescence resonance energy transfer quenching at the surface of graphene quantum dots for ultrasensitive detection of TNT[J].Talanta,2012,101:192-197.
[39]LI Z,WANG Y,NI Y,et al.A sensor based on blue luminescent graphene quantum dots for analysis of a common explosive substance and an industrial intermediate,2,4,6-trinitrophenol[J].Spectrochimica Acta Part A:Molecular and Biomolecular Spectroscopy,2015,137:1213-1221.
[40]LI Y,ZHANG L,HUANG J,et al.Fluorescent graphene quantum dots with a boronic acid appended bipyridinium salt to sense monosaccharides in aqueous solution[J].Chemical Communications,2013,49(45):5180-5182.
[41]WANG Y,ZHANG L,LIANG R,et al.Using graphene quantum dots as photoluminescent probes for protein kinase sensing[J].Analytical Chemistry,2013,85(19):9148-9155.
[42]ZHU X,ZENG L,XU M,et al.A glassy carbon electrode modified with electrochemically reduced graphene for simultaneous determination of guanine and adenine[J].Analytical Methods,2012,4(9):2935-2939.
[43]ZHU X,LIANG Y,ZUO X,et al.Novel water-soluble multi-nanopore graphene modified glassy carbon electrode for simultaneous determination of dopamine and uric acid in the presence of ascorbic acid[J].Electrochimica Acta,2014,143:366-373.
[44]ZHU X,JIAO Q,ZHANG C,et al.Electropolymerization of graphene and 5-[o-(4-bromine amyloxy)phenyl]-10,15,20-triphenylporphrin(o-Br PETPP)composite film electrode for the electrocatalytic oxidation of indirubin[J].Journal of Electroanalytical Chemistry,2012,681:133-138.
[45]ZHU X,JIAO Q,ZUO X,et al.An electrochemical sensor based on carbon nano-fragments andβ-cyclodextrin composite-modified glassy carbon electrode for the determination of Rutin[J].Journal of the Electrochemical Society,2013,160(10):H699-H703.
[46]ZHU X,JIAO Q,ZHANG C,et al.Amperometric nonenzymatic determination of glucose based on a glassy carbon electrode modified with nickel(II)oxides and graphene[J].Microchimica Acta,2013,180(5/6):477-483.
[47]RAZMI H,MOHAMMADREZAEI R.Graphene quantum dots as a new substrate for immobilization and direct electrochemistry of glucose oxidase:application to sensitive glucose determination[J].Biosensors and Bioelectronics,2013,41:498-504.
[48]WANG X,CHEN L,SU X,et al.Electrochemical immunosensor with graphene quantum dots and apoferritin-encapsulated Cu nanoparticles double-assisted signal amplification for detection of avian leukosis virus subgroup J[J].Biosensors and Bioelectronics,2013,47:171-177.
[49]HOU J,BEI F,WANG M,et al.Electrochemical determination of malachite green at graphene quantum dots-gold nanoparticles multilayers-modified glassy carbon electrode[J].Journal of Applied Electrochemistry,2013,43(7):689-696.
[50]ZHAO J,CHEN G,ZHU L,et al.Graphene quantum dots-based platform for the fabrication of electrochemical biosensors[J].Electrochemistry Communications,2011,13(1):31-33.
[51]ZHANG Y,WU C,ZHOU X,et al.Graphene quantum dots/gold electrode and its application in living cell H2O2detection[J].Nanoscale,2013,5(5):1816-1819.
[52]LI L,JI J,FEI R,et al.A facile microwave avenue to electrochemiluminescent two-color Graphene quantum dots[J].Advanced Functional Materials,2012,22(14):2971-2979..
[53]LU J,YAN M,GE L,et al.Electrochemiluminescence of blue-luminescent graphene quantum dots and its application in ultrasensitive aptasensor for adenosine triphosphate detection[J].Biosensors and Bioelectronics,2013,47:271-277.
[54]ZHOU Y,QU Z,ZENG Y,et al.A novel composite of graphene quantum dots and molecularly imprinted polymer for fluorescent detection of paranitrophenol[J].Biosensors and Bioelectronics,2014,52:317-323.
[55]TIAN J,ZHAO H,QUAN X,et al.Fabrication of graphene quantum dots/silicon nanowires nanohybrids for photoelectrochemical detection of microcystin-LR[J].Sensors and Actuators B:Chemical,2014,196:532-538.