金属有机框架纳米功能界面的构筑及用于电化学同时检测嘌呤代谢物
|
摘要
同时检测DNA代谢产物黄嘌呤(XA)、次黄嘌呤(HX)和尿酸(UA)对代谢异常引起的相关疾病的早期诊断及预防具有十分重要的意义。本研究基于羟基功能化金属有机框架材料(OH-MIL-101(Fe),记为OH-MOFs)及电化学还原氧化石墨烯(ERGO)的协同催化作用,设计并构筑了OH-MOFs-ERGO纳米功能界面,实现了电化学法同时检测血清中尿酸、黄嘌呤和次黄嘌呤。通过超声混合法制备纳米复合功能材料,应用XRD、FT-IR和UV-vis等方法对材料进行了表征,通过滴涂法及电化学还原法在玻碳电极(GCE)表面构筑了OH-MOFs-ERGO/GCE。此修饰电极检测UA、XA和HX的线性范围分别为0.20～1150μmol/L、0.15～800μmol/L和0.40～600μmol/L,检出限分别为0.12、0.10和0.20μmol/L(S/N=3),实际血清样品中加标回收率在96.1%～106.6%之间。本方法为嘌呤代谢相关的生理病理研究提供了一种简单快速的检测方法。
The simultaneous and sensitive detection of metabolites of DNA(uric acid(UA), xanthine(XA) and hypoxanthine(HX)) is of great significance for the early diagnosis and prevention of related diseases caused by abnormal metabolism. In this study, hydroxyl functionalized metal-organic framework(OH-MOFs) and electrochemically reduced graphene oxide(ERGO) nano-functional interface was designed and constructed based on the synergic effect of FeⅢ terephthalate OH-MOFs(OH-MIL-101(Fe) and ERGO for simultaneous detection of UA, XA and HX in blood. Nano-composites were prepared by ultrasonic mixing method, and were characterized by X-ray diffraction(XRD), Fourier transform infrared(FT-IR) and UV-Vis spectroscopic methods. By casting the surface of glassy carbon electrode(GCE) with the composite and electrochemical reduction of the modified electrode, OH-MOFs-ERGO/GCE was obtained. Under the optimum conditions, the oxidation peak currents of UA, XA and HX were linearly correlated to their concentrations in the ranges of 0.20-1150 μmol/L, 0.15-800 μmol/L, and 0.40-600 μmol/L, respectively. The detection limits for UA, XA and HX were 0.12, 0.10 and 0.20 μmol/L(S/N=3), respectively. The recoveries of UA, XA and HX in real serum samples were between 99.5% and 105.8%. The proposed electrode was expected to provide a simple and easy detection method for the physiological and pathological study of purine metabolism.
The simultaneous and sensitive detection of metabolites of DNA(uric acid(UA), xanthine(XA) and hypoxanthine(HX)) is of great significance for the early diagnosis and prevention of related diseases caused by abnormal metabolism. In this study, hydroxyl functionalized metal-organic framework(OH-MOFs) and electrochemically reduced graphene oxide(ERGO) nano-functional interface was designed and constructed based on the synergic effect of FeⅢ terephthalate OH-MOFs(OH-MIL-101(Fe) and ERGO for simultaneous detection of UA, XA and HX in blood. Nano-composites were prepared by ultrasonic mixing method, and were characterized by X-ray diffraction(XRD), Fourier transform infrared(FT-IR) and UV-Vis spectroscopic methods. By casting the surface of glassy carbon electrode(GCE) with the composite and electrochemical reduction of the modified electrode, OH-MOFs-ERGO/GCE was obtained. Under the optimum conditions, the oxidation peak currents of UA, XA and HX were linearly correlated to their concentrations in the ranges of 0.20-1150 μmol/L, 0.15-800 μmol/L, and 0.40-600 μmol/L, respectively. The detection limits for UA, XA and HX were 0.12, 0.10 and 0.20 μmol/L(S/N=3), respectively. The recoveries of UA, XA and HX in real serum samples were between 99.5% and 105.8%. The proposed electrode was expected to provide a simple and easy detection method for the physiological and pathological study of purine metabolism.
引文
1 Lan D X,Zhang L.J.Electroanal.Chem.,2015,757:107-115
2 Liu G,Ma W,Luo Y,Sun D M,Shao S.J.Anal.Methods Chem.,2014:984314
3 Wang Y,Tong L L.Sens.Actuators B,2010,150(1):43-49
4 Wang Y.Colloids Surf.B,2011,88:614-621
5 Si Y,Park J W,Jung S,Hwang G,Goh E,Lee H.Biosens.Bioelectron.,2018,121:265-271
6 Rita F,Maria L P,Jose B.Clin.Biochem.,2013,46(7-8):665-669
7 Zhao S L,Wang J S,Ye F G,Liu Y M.Anal.Biochem.,2008,378(2):127-131
8 Arivazhagan M,Jeyavijayan S.Spectrochim.Acta,2011,79(1):161-168
9 Kalimuthu P,Leimkuhler S,Bernhardt P V.Anal.Chem.,2012,84:10359-10365
10 SUN Kai,SUN Deng-Ming.Chinese J.Anal.Chem.,2014,42(7):991-996孙凯,孙登明.分析化学,2014,42(7):991-996
11 Karthik P,Vinoth R,Zhang P,Choi W,Balaraman E.ACS Appl.Energy Mater.,2018,1(5):1913-1923
12 ZHANG Dan-Yang,CAI Yao,SHEN Yu,XU Wen-Ju.Chinese J.Anal.Chem.,2018,46(11):1794-1801张丹阳,蔡瑶,沈雨,许文菊.分析化学,2018,46(11):1794-1801
13 Zheng Y,Zheng S,Xue H,Pang H.Adv.Funct.Mater.,2018,28:1804950
14 Zhu Q,Xu Q.Chem.Soc.Rev.,2014,43:5468-5512
15 Jo G,Choe M,Cho C,Kim J H,Park W,Lee S,Hong W,Kim T,Park S,Hong B H,Kahng Y H,Lee T.Nanotechnology,2010,21:175-201
16 Marinho B,Ghislandi M,Tkalya E,Koning C E.Powder Technol.,2012,221:351-358
17 Balandin A,Ghosh S,Bao W,Calizo I,Teweldebrhan D,Miao F,Lau C N.Nano Lett.,2008,8(3):902-907
18 Wang X,Wang Q X,Wang Q H,Gao F,Gao F,Yang Y Z,Guo H X.ACS Appl.Mater.Interfaces,2014,6(14):11573-11580
19 Li Y Z,Huang F C,Du H J,Liu W B,Li Y W,Ye J S.J.Electroanal.Chem.,2013,709:65-69
20 Yin D D,Liu J,Bo X J,Li M,Guo L P.Electrochim.Acta,2017,247:41-49
21 Lebedev O I,Millange F,Serre C,van Tendeloo,Ferey G.Chem.Mater.,2005,17(26):6525-6527
22 Li S X,Sun SL,Wu H Z,Wei C H,Hu Y.Catal.Sci.Technol.,2018,8(6):1696-1703
23 Tang X Q,Zhang Y D,Jiang Z W,Wang D M,Huang C Z,Li Y F.Talanta,2018,179:43-50
24 Hummers J,William S,Richard E.J.Am.Chem.Soc.,1958,80(6):1339-1339
25 Akiyama G,Matsuda R,Sato H,Hori A,Takata M.Kitagawa S.Micropor.Mesopor.Mater.,2012,157:89-93
26 Karthik P,Vinoth R,Zhang P,Choi W Y,Balaraman E,Neppolian B.ACS Appl.Energy Mater.,2018,1(5):1913-1923
27 Sarauli D,Borowski A,Peters K,Schulz B,Fattakhova-Rohlfing D,Leimkühler S,Lisdat F.ACS Catal.,2016,6(10):7152-7159
28 Wang X,Xi M,Guo M,Sheng F,Xiao G,Wu S,Uchiyama S,Matsuura H.Analyst,2016,141:1077-1082
29 Kalimuthu P,Leimkuühler S,Bernhardt P V.J.Phys.Chem.B,2011,115(11):2655-2662
30 Ojani R,Alinezhad A,Abedi Z.Sens.Actuators B,2013,188:621-630
31 Luo A,Lian Q W,An Z Z,Li Z,Guo Y Y,Zhang D X,Xue Z H,Zhou X B,Lu X Q.J.Electroanal.Chem.,2015,756:22-29
2 Liu G,Ma W,Luo Y,Sun D M,Shao S.J.Anal.Methods Chem.,2014:984314
3 Wang Y,Tong L L.Sens.Actuators B,2010,150(1):43-49
4 Wang Y.Colloids Surf.B,2011,88:614-621
5 Si Y,Park J W,Jung S,Hwang G,Goh E,Lee H.Biosens.Bioelectron.,2018,121:265-271
6 Rita F,Maria L P,Jose B.Clin.Biochem.,2013,46(7-8):665-669
7 Zhao S L,Wang J S,Ye F G,Liu Y M.Anal.Biochem.,2008,378(2):127-131
8 Arivazhagan M,Jeyavijayan S.Spectrochim.Acta,2011,79(1):161-168
9 Kalimuthu P,Leimkuhler S,Bernhardt P V.Anal.Chem.,2012,84:10359-10365
10 SUN Kai,SUN Deng-Ming.Chinese J.Anal.Chem.,2014,42(7):991-996孙凯,孙登明.分析化学,2014,42(7):991-996
11 Karthik P,Vinoth R,Zhang P,Choi W,Balaraman E.ACS Appl.Energy Mater.,2018,1(5):1913-1923
12 ZHANG Dan-Yang,CAI Yao,SHEN Yu,XU Wen-Ju.Chinese J.Anal.Chem.,2018,46(11):1794-1801张丹阳,蔡瑶,沈雨,许文菊.分析化学,2018,46(11):1794-1801
13 Zheng Y,Zheng S,Xue H,Pang H.Adv.Funct.Mater.,2018,28:1804950
14 Zhu Q,Xu Q.Chem.Soc.Rev.,2014,43:5468-5512
15 Jo G,Choe M,Cho C,Kim J H,Park W,Lee S,Hong W,Kim T,Park S,Hong B H,Kahng Y H,Lee T.Nanotechnology,2010,21:175-201
16 Marinho B,Ghislandi M,Tkalya E,Koning C E.Powder Technol.,2012,221:351-358
17 Balandin A,Ghosh S,Bao W,Calizo I,Teweldebrhan D,Miao F,Lau C N.Nano Lett.,2008,8(3):902-907
18 Wang X,Wang Q X,Wang Q H,Gao F,Gao F,Yang Y Z,Guo H X.ACS Appl.Mater.Interfaces,2014,6(14):11573-11580
19 Li Y Z,Huang F C,Du H J,Liu W B,Li Y W,Ye J S.J.Electroanal.Chem.,2013,709:65-69
20 Yin D D,Liu J,Bo X J,Li M,Guo L P.Electrochim.Acta,2017,247:41-49
21 Lebedev O I,Millange F,Serre C,van Tendeloo,Ferey G.Chem.Mater.,2005,17(26):6525-6527
22 Li S X,Sun SL,Wu H Z,Wei C H,Hu Y.Catal.Sci.Technol.,2018,8(6):1696-1703
23 Tang X Q,Zhang Y D,Jiang Z W,Wang D M,Huang C Z,Li Y F.Talanta,2018,179:43-50
24 Hummers J,William S,Richard E.J.Am.Chem.Soc.,1958,80(6):1339-1339
25 Akiyama G,Matsuda R,Sato H,Hori A,Takata M.Kitagawa S.Micropor.Mesopor.Mater.,2012,157:89-93
26 Karthik P,Vinoth R,Zhang P,Choi W Y,Balaraman E,Neppolian B.ACS Appl.Energy Mater.,2018,1(5):1913-1923
27 Sarauli D,Borowski A,Peters K,Schulz B,Fattakhova-Rohlfing D,Leimkühler S,Lisdat F.ACS Catal.,2016,6(10):7152-7159
28 Wang X,Xi M,Guo M,Sheng F,Xiao G,Wu S,Uchiyama S,Matsuura H.Analyst,2016,141:1077-1082
29 Kalimuthu P,Leimkuühler S,Bernhardt P V.J.Phys.Chem.B,2011,115(11):2655-2662
30 Ojani R,Alinezhad A,Abedi Z.Sens.Actuators B,2013,188:621-630
31 Luo A,Lian Q W,An Z Z,Li Z,Guo Y Y,Zhang D X,Xue Z H,Zhou X B,Lu X Q.J.Electroanal.Chem.,2015,756:22-29