基于金屬石墨烯納米復(fù)合材料構(gòu)建電化學(xué)生物傳感器的研究及應(yīng)用
發(fā)布時(shí)間:2018-04-19 08:26
本文選題:電化學(xué)傳感器 + 納米復(fù)合材料 ; 參考:《濟(jì)南大學(xué)》2017年碩士論文
【摘要】:電化學(xué)免疫傳感器作為一種新型的檢測(cè)方法已被廣泛應(yīng)用于不同的領(lǐng)域中。本論文利用不同的方法制備了一系列具有催化性能以及生物相容性較好、導(dǎo)電能力強(qiáng)等優(yōu)點(diǎn)的納米復(fù)合材料,并將納米復(fù)合材料應(yīng)用于對(duì)電化學(xué)免疫傳感器的構(gòu)建中以實(shí)現(xiàn)對(duì)目標(biāo)生物分子的定量檢測(cè)。石墨烯作為一種具有二維結(jié)構(gòu)的納米材料具有較大的BET比表面積、良好的導(dǎo)電能力、生物相容性好等優(yōu)點(diǎn)而被廣泛應(yīng)用于電化學(xué)免疫傳感器中。金屬納米粒子生物相容性好并且具有較好的催化性能,其構(gòu)建的復(fù)合材料較好的保留了金屬粒子的相關(guān)特性。金屬石墨烯復(fù)合材料結(jié)合了兩者的優(yōu)點(diǎn)有效地改善了傳感器的相關(guān)性能。本論文主要包括以下五個(gè)部分:第一部分,首先對(duì)電化學(xué)傳感器、傳感器的類型、納米材料、生物分子的定義及其基本特性進(jìn)行了介紹,最后介紹了該論文的研究?jī)?nèi)容。第二部分,以氨基化石墨烯金(Au-NH_2-rGO)作為基底材料,具有三維結(jié)構(gòu)的石墨烯-碳納米管-鈀(rGO-MWCNT-Pd)作為二抗標(biāo)記物構(gòu)建了夾心型免疫傳感器實(shí)現(xiàn)了對(duì)前列腺特異抗原(PSA)的定量檢測(cè)。以三維結(jié)構(gòu)的rGO-MWCNT-Pd納米復(fù)合材料作為信號(hào)放大器,在降低傳感器的檢出限、拓寬檢測(cè)范圍方面發(fā)揮了重要作用。該傳感器對(duì)PSA的檢測(cè)范圍為0.5 pg/mL至15.0ng/mL,檢出限為0.17 pg/mL并將該傳感器成功用于對(duì)實(shí)際樣品的檢測(cè)中。第三部分,通過(guò)原位還原的方法將非貴金屬鎳與貴金屬鉑、金三種元素進(jìn)行摻雜制備了鎳鉑金-還原石墨烯(Ni AuPt-rGO)納米復(fù)合材料,由于三金屬之間的協(xié)同作用使得NiAuPt-rGO對(duì)雙氧水(H_2O_2)具有較強(qiáng)的催化能力。以水溶性好識(shí)別能力強(qiáng)的環(huán)糊精-石墨烯(β-CD@rGO)作為基底材料,NiAuPt-rGO作為二抗標(biāo)記物催化H_2O_2構(gòu)建了一種夾心型免疫傳感器,實(shí)現(xiàn)對(duì)癌胚抗原(CEA)的定量檢測(cè)。該傳感器對(duì)癌胚抗原的線性檢測(cè)范圍為0.001-100.0 ng/mL,檢出限為0.27 pg/mL并展現(xiàn)出良好的重現(xiàn)性、穩(wěn)定性以及較高的選擇性等性能。第四部分,利用原位還原的方法制備了石墨烯-四氧化三鐵@金鈷(rGO@Fe_3O_4@AuCo)磁性納米復(fù)合材料。具有較大直徑的Fe_3O_4納米粒子的加入防止了rGO的團(tuán)聚增大了復(fù)合材料的比表面積,為AuCo納米粒子的負(fù)載提供了較多的結(jié)合位點(diǎn);谝陨喜牧蠘(gòu)建了檢測(cè)AFP夾心型免疫傳感器,檢測(cè)范圍在0.5 pg/mL-50.0 ng/mL,檢出限為0.18 pg/mL,對(duì)AFP的臨床檢測(cè)具有重要的應(yīng)用價(jià)值。第五部分,利用1,8-二氨基萘氨基化石墨烯制備了1,8-二氨基萘-石墨烯-金(1,8-DN-rGO-Au)并將其作為傳感器的基底材料捕獲抗體,以具有三維結(jié)構(gòu)的三維刺狀四氧化三鐵@二氧化鈦@金銀@環(huán)糊精(Fe_3O_4@TiO_2@AuAg@β-CD)納米復(fù)合材料作為二抗標(biāo)記物構(gòu)建了夾心型免疫傳感器。該傳感器對(duì)PSA的檢測(cè)范圍為0.5 pg/mL-100.0 ng/mL,檢出限為0.2 pg/mL。并且具有良好的穩(wěn)定性、選擇性以及重現(xiàn)性等優(yōu)點(diǎn),該傳感器具有臨床檢測(cè)分析的應(yīng)用前景。
[Abstract]:Electrochemical immunosensor as a new detection method has been widely used in different fields.In this paper, a series of nanocomposites with good catalytic performance, good biocompatibility and strong conductivity were prepared by different methods.Nanocomposites were applied to the construction of electrochemical immunosensors for quantitative detection of target biomolecules.Graphene is widely used in electrochemical immunosensors because of its large BET specific surface area, good conductivity, good biocompatibility and so on.Metal nanoparticles have good biocompatibility and good catalytic performance.Metal graphene composites combine the advantages of the two to improve the performance of the sensor.This thesis mainly includes five parts as follows: in the first part, the electrochemical sensor, the type of sensor, the nanomaterials, the definition of biomolecules and their basic characteristics are introduced. Finally, the research content of this thesis is introduced.In the second part, a sandwich immunosensor was constructed using Au-NH2-rGOA as substrate material and graphene carbon nanotube palladium (PD) as a second antibody marker to realize the quantitative detection of prostate specific antigen (PSAs).Three-dimensional rGO-MWCNT-Pd nanocomposites as signal amplifiers play an important role in reducing the detection limit and widening the detection range of the sensor.The detection range of PSA is 0. 5 pg/mL to 15. 0 ng / mL, and the detection limit is 0. 17 pg/mL. The sensor has been successfully used in the detection of real samples.In the third part, Nickel-platinum / reduced graphene Ni AuPt-rGOA nanocomposites were prepared by doping non-precious metal nickel with precious metal platinum and gold by in-situ reduction.Due to the synergistic effect of trimetals, NiAuPt-rGO has a strong catalytic activity for H _ 2O _ 2 (H _ 2O _ 2).A sandwich immunosensor was constructed by using 尾 -CDDP-graphene (尾 -CDR) as the substrate material and NiAuPt-rGO as the second antibody marker to construct a sandwich immunosensor for the quantitative detection of carcinoembryonic antigen (CEA).The linear detection range of carcinoembryonic antigen was 0.001-100.0 ng / mL, and the detection limit was 0.27 pg/mL. The sensor showed good reproducibility, stability and high selectivity.In the fourth part, in situ reduction method was used to prepare the magnetic nanocomposites of graphene / Fe _ 2O _ 4 @ AuCo _ 2O _ 4 / Co _ (3) O _ (3) O _ (4) O _ (4) O _ (4) O _ (4) AuCoC.The addition of Fe_3O_4 nanoparticles with large diameters prevents the agglomeration of rGO from increasing the specific surface area of the composites and provides more binding sites for the loading of AuCo nanoparticles.Based on the above materials, a sandwich immunosensor for detection of AFP was constructed. The detection range was 0.5 pg/mL-50.0 ng / mL, and the detection limit was 0.18 PG / mL, which has important application value for clinical detection of AFP.In the fifth part, we prepared 1H8-diaminonaphthalene-graphene-Amino-au) and used it as the substrate material of the sensor to capture the antibody.A sandwich immunosensor was constructed using three-dimensional spinned-iron trioxide @ titanium dioxide @ gold and silver @ cyclodextrin / tio _ 3O _ 4tio _ 4tio _ 2d AuAg@ 尾 -CDCD nanocomposite as a second antibody marker.The detection range of PSA is 0.5 pg/mL-100.0 / mL and the detection limit is 0.2 PG / mL.The sensor has the advantages of good stability, selectivity and reproducibility.
【學(xué)位授予單位】:濟(jì)南大學(xué)
【學(xué)位級(jí)別】:碩士
【學(xué)位授予年份】:2017
【分類號(hào)】:O657.1;TP212
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