基于表面分子开关的生物传感器新方法研究
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摘要
科学和技术发展最重要的挑战之一就是进一步实现对微观的控制和研究，这就意味着要利用化学手段自下而上(bottom-up)来构建分子水平上器件和机器，即从原子或分子开始建造微观结构。“自下而上”是指以原子，分子为基本单元，根据人们的意愿进行设计和组装，从而构筑成具有特定功能的器件。同时，随着微电子技术和生物工程这两项高科技的互相渗透，分子开关实际上已为研制分子器件提供了可能。所谓分子开关泛指结构上组织化了的具有“开／关”功能的化学体系。它也是指具有双稳态的量子化体系，当外界光、电、热、磁、酸碱度等条件变化时，分子的形状、化学键的生成或断裂、振动以及旋转等性质会随之变化，通过这些几何和化学的变化，能实现信息传输的功能。
分子水平上的开关需要一个外部刺激来引起电子和原子核的重排，3种用来开启化学体系功能的最重要的刺激是光能(光子)，电能(电子或空穴)和化学能(以质子、金属离子或特殊分子形式)。最常见的光化学激发开关过程与光异构化和光诱导氧化还原反应是相关的。如果输入的是电化学激发，当然就是氧化还原反应的诱导反应，与化学激发相比，光化学和电化学激发的分子开关更容易发生且响应迅速。利用电化学能代替化学氧化还原作用，具有开、关简便快捷的优势。况且，电化学技术也是监测机器运行的有用方式，电极则是分子系统与宏观世界相连的最佳方式。电场控制的表面分子开关可以用于蛋白质的可控吸附和分离．再结合分子设计、有机合成和高分子化学，还可以给这种表面引入亲疏水功能团或抗原抗体识别对等，方便的实现亲疏水开关或者免疫开关表面。
本论文主要创新之处是基于自组装膜技术、电化学控制技术以及温敏聚合物材料构建具有表面分子开关功能的仿生界面，从而利用这些智能化表面对生物分子及其动态相互作用过程进行实时在线控制和检测。智能化表面(smart surface)通常是指具有可操控开关功能的生物应用表面。智能化表面性质的可逆操控，是在外界激励下发生的。它可以由聚合物、有序自组装膜、纳米材料(特别是金属氧化物)等组成，激励它发生性质可逆转化的因素包括温度、光照、电场、pH值、溶剂等等。在这些外界激励下，表面分子可以发生可逆的构象转化、构型转化、氧化态的转化等等，从而在宏观上，使整个表面呈现出亲疏水性、光学性质、带电性等性质的可逆转化，即可呈现出“开／关”的性质。本论文通过构建的低密度自组装膜，在表面上形成电化学可操控的具有生物识别能力的亲疏水开关，从而实现了对抗生物素一链霉亲和素功能蛋白间微观作用过程的快速、灵敏、可控检测和表征。进一步地，利用温敏高分子材料poly(N-isopropylacrylamide)PNIPAAm与抗BSA抗体合成生物复合物，构建了具有温度敏感开关功能的可再生免疫传感器。该方法可保持生物识别体系的活性和环境，再生的抗原／抗体表面均可重复识别相应目标物，检测灵敏度高、速度快，所构建的温敏开关免疫传感器可重复使用30次以上，解决了目前免疫传感器抗体表面仅能单次使用的弊端，同时为研究蛋白质-蛋白质动态相互作用过程提供了新手段。
本论文共五章内容，主要摘要如下：
第一章综述了表面分子开关的研究现状及其相关技术在生物传感器领域的应用进展。分子自组装和高分子聚合物是构建分子开关的两条重要途径。自组装单分子层是构膜分子与基底材料间发生物化作用而自发形成的一种热力学稳定、排列规则的单层分子膜。这种构膜方式，可以容易的为表面引入各种各样的功能团，这就为制备具有多种不同功能的智能化表面打下了很好的基础。温敏材料是指对温度可感知且可响应并具有功能发现能力的一类材料。具有“温度开关”特性的聚-N异丙基丙烯酰胺(PNIPAAm)是近年来引起研究兴趣的一类高分子材料。利用它对温度响应的敏感性，使其在药物缓释、免疫分析、生命科学等研究领域都有着广泛的潜力。
第二章介绍了基于人工自组装膜技术构建表面亲疏水开关发展生物传感器的新方法。本章利用环糊精作为巯酸分子间距有效的调控手段，以乙醇作为高效的洗脱溶剂，通过自组装方法在金电极表面构建了间距均一、性能稳定的巯基化合物低密度薄膜，由此构建了具有亲疏水可逆开关的智能化表面生物传感器。以高密度自组装膜表面的覆盖度为100％计算可知，α，β，γ三种环糊精分子构建的低密度自组装膜表面的覆盖度分别为61.2％，45.3％和29.2％。通过改变外加电压状况，使巯基化合物构型发生改变，从而实现表面的亲水／疏水性能的转换。通过质谱，核磁，交流阻抗，QCM，荧光等多种检测手段对膜表面可逆过程进行了实时监控。
第三章主要围绕此类亲疏水开关生物传感器进行抗生物素及链霉亲和素可控组装的应用研究。本章采用荧光标记抗生物素、链霉亲和素功能蛋白分子作为研究对象，通过改变外加电流正负情况使得低密度自组装膜表面具有亲疏水可逆转换性能。在pH值为7.4的缓冲溶液中，两种蛋白质由于等电点的差异而带上了两种不同的电荷，由于表面电荷作用及亲疏水性质的转换，两种蛋白质可以在外加电场作用下发生可控组装行为。主要利用EQCM实验和荧光光谱实验对两种蛋白质的可控组装进行了实时监测，对于Avidin蛋白在β-CD构建的低密度自组装膜上的组装过程，将其在负电压下组装30分钟后它的荧光强度是正电压条件下的4.9倍。对于Streptavidin蛋白来说，当外加正电压30分钟后，在β-CD构建的低密度自组装膜表面上蛋白组装量分别是负电压条件下同种组装膜的1.5倍。利用微电极中获得的良好分离分析效果，我们还初步尝试将之应用于微流控芯片体系，发展了一种利用“分子开关”原理构建的蛋白质芯片。
第四章是基于温敏聚合物的表面分子开关构建及抗原抗体可逆识别界面的研究。本章主要研究温敏高分子材料PNIPAAm与抗BSA抗体合成的生物复合物(bioconjugate)组装到金表面与对应抗原BSA识别时的可逆过程。由于这种温敏高分子材料的存在，这个结合过程与抗体-抗原直接结合的情况有很大变化，选择不同分子量的聚合物进行构建，该材料对抗原结合过程中造成的空间位阻有所不同，结合量可通过测定QCM，交流阻抗法，天然PAGE胶以及荧光标记抗原的光亮度加以定量。当抗原抗体结合完毕后，改变溶液的温度，由于温敏材料分子量的差异，高分子量时随着温度升高，抗体结合位点附近的高分子材料会团聚在已经结合的抗原周围，而且会产生较大的空间力以及疏水力，从而将已经结合的抗原从抗体结合部位顶开，使得所构建的温敏开关免疫传感器具有良好的再生功能。高温降至低温过程中，免疫识别体系抗原抗体结合常数差别可以达到两个数量级。高分子量聚合物构建的免疫开关传感器对于抗原抗体结合后表面的再生率最高可以达到89％以上，跟通常文献中大量报道的有机溶液再生表面法(再生率80％-92％)相差很小，而且这个方法基本没有破坏生物识别体系的活性和环境，抗原抗体均可重复利用，这种温敏开关免疫传感器可重复使用30次以上，抗疲劳性较好。综上所述，这种基于温敏聚合物的表面开关可以在免疫生物传感领域进行广泛的应用。
第五章工作围绕基于手性氨基酸抗体构建电容型手性免疫传感器进行相关研究。利用自制手性抗体构建高选择性的新型电容型免疫传感器，设计了逆向竞争法进行检测，得到了很好的响应，这一部分工作仍在进行中。构建的电容性手性免疫传感器从所有的图表中可以看出这种传感器对于小分子的手性氨基酸具有很强的识别和分析能力，检测限可以达到5pg／mL，对氨基酸混合物中痕量D型苯丙氨酸可以达到0.001％的检测灵敏度。竞争法测定灵敏快速，既可以测定D型、L型苯丙氨酸对电极表面半抗原与抗体免疫识别的抑制情况，还可以测定消旋体中单一构型(D型)氨基酸含量，此方法对于混合氨基酸体系中痕量的单一构型抗原检测限比标准的手性色谱分析方法还要低一个数量级，具有高灵敏度、高选择性的特点，为无标记法检测手性氨基酸提供了一种可行的检测方法。具有操作简便，重现性好，成本低廉等一系列优点，对于手性物质的快速在线分析对于临床检测及手性药物分析等具有较大的意义。
第六章是对本论文工作的总结及对下一步工作的展望。
总之，本论文围绕表面分子开关进行了多种生物传感新方法的成功尝试。利用自组装膜技术，温敏聚合物材料等结合外界不同触发条件构建了亲疏水表面开关、温度敏感表面开关生物传感器，形成了具有良好生物相容性的仿生界面，将其应用于蛋白质分子、抗原-抗体体系等进行人工可操控的生物过程的考察与研究均获得了良好的结果。
Controlled study of microscopic fields is one of the most important challenges to scientific and technological development. Scientists use chemical and biological methods to build complex molecular-level devices from the basic building blocks of atomic or molecular microstructure. This strategy, known as "bottom-up" design allows for devices with specific structure or function to be built. Of particular interest has been the development of molecular switches, which could serve as the precursor to the preparation of more complicated molecular devices. Molecular switches are molecules which are capable of changing their behavior in a controlled fashion based on external stimuli such as light, electricity, heat, magnetic fields, or pH. By taking advantage of such switching behavior it should be possible to realize the transmission of information.
Switching behavior requires an external stimuli to cause either an electronic transition or a structural rearrangement. The three most important stimuli are light (absorption of photons), electricity (addition or removal of electrons) and chemical energy (binding of protons, metal ions, or other special molecules). The most common photochemical switches are related to light-induced isomerization and light-induced oxidation and reduction reactions. Electrochemical methods can also be used to produce redox type switching behavior. Moreover, electrochemical techniques are a useful way to monitor the operation of molecular machinery, with the electrode serving as the connection to the macroscopic world. As an example, surface electric switches can be used to control protein adsorption and separation. By combining molecular design, organic synthesis, and polymer chemistry, it is possible to introduce hydrophilic or hydrophobic functional groups or antigen-antibody complexes to the surface resulting in a reversible switch.
This thesis is based on the use of a low-density self-assembled monolayer and temperature-sensitive polymer to build a biocompatible surface. By using these innovative methods, controlled in situ determination and monitoring for biological molecules could be carried on. The intelligent modification of surface properties allows for the detection of a wide range of biological species. The focus of this work has been the development of a sensitive and reversible switch for the detection of specific biomolecules. By using a low-density self-assembled monolayer (SAM) to establish a hydrophobic/hydrophilic switch it has been possible to achieve the rapid and controlled detection of avidin and streptavidin. Reversible control of the surface properties has been achieved with various methods, including: photoillumination, potential effects, and thermal driving. By using temperature-sensitive poly (N-isopropylacrylamide) (PNIPAAm) materials, an immune switch sensor for Anti-BSA antibody and FITC-BSA could be created. The switch is stable in biological environments, does not interfere with the antibody/antigen detection, and can be reused more than 30 times.
In the first chapter we review the research on surface molecular switches and related technical progress in the field of biosensors. Polymers and self-assembly are two important ways to build molecular surface switches. Using self-assembled monolayers could supply a thermodynamically stable and ordered membrane. The structure of SAMs can easily be varied by the introduction of a wide range of functional groups. Temperature-sensitive materials are also found to be good candidates and have the useful ability to respond to external temperature stimuli. In recent years PNIPAAm has attracted interest in the study of temperature-sensitive polymer materials because of its potential application in drug delivery, immunoassays, and life science research.
The second chapter describes using SAMs to constructsmart hydrophobic/hydrophilic reversible surfaces as a new method for biosensor development. The inclusion complex (IC) between 16-mercaptohexadecanoic acid (MHA) andα-,β- orγ-cyclodextrin acted as the space-filling group of the SAM. The unwrapping procedure, the removal of n-CD from the SAM, was accomplished by dissociating the bond n-CD—MHA with ethanol. The surface coverage for LD-SAM-n referring to high-density SAM shows an obvious decrease from 100% to 61.2%, 45.3% and 29.2%, respectively. The thus-prepared low density-SAM shows reversible conformational reorientation under negative and positive potential; this induces changes in wettability, which can be observed by means of contact angle measurements. The removal of n-CD was monitored by quartz crystal microbalance (QCM), nuclear magnetic resonance (NMR), impedance (IMP), and MALDI-TOF-MS.
The third chapter describes the application of our LD-SAM surface to the controlled assembly of two kinds of fluorescent-labeled avidin and streptavidin. Selective protein adsorption was demonstrated on the above-mentioned switchable surface. The assembly of the two proteins on MHA-SAM-n was performed in PBS buffer (pH 7.4) at an applied potential of 0.3 V and -0.3 V (vs.SCE), respectively. From either QCM or fluorescence spectra (FL) data, distinctly different assembly behaviors for the two proteins were observed at two controlled potentials. For example, the emission intensity for avidin-LD-SAM-1 assembled at negative potential for 30 min was about 4.9 times that for assembly at positive potential. The dissimilarity of the surface loading for these two proteins is believed to be mainly due to the charge status difference originating from their isoelectric points. We believe that it might lead to versatile applications, e.g. control of protein adsorption/release in a functionalized capillary or microfluidics channel, or design of intelligent protein chips. We have also attempted to apply this system to a homemade microfluidic chip.
The fourth chapter works on establishing the PNIPAAm-antibody surface that could supply the most effective dissociation of the antigen and regeneration of antibody into reuse of the immunosensors. As a model antibody-antigen system, bovine serum albumin (BSA) and the corresponding antibody (anti-BSA) were chosen. A reversible PNIPAAm-antibody (anti-BSA) conjugates surface was established by triggered control of external temperature. This took advantage of the thermally tunable conformational changes for the PNIPAAm-conjugated antibody surface, and could be used for switchable antigen association and dissociation. The temperature controlling strategy could realized the regeneration of the immunosensor on which immobilized anti-BSA antibodies retain the activity and specificity necessary to carry out more than 30 reproducible assays for BSA. The dissociation reaches 89%, which can compare with the general recovery methods. The controlled binding and unbinding were monitored by quartz crystal microbalance (QCM), confocal fluorescence, native electrophoresis, laser induced fluorescence, and electrochemical impedance.
The fifth chapter describes a highly enantioselective and sensitive immunosensor for the detection of chiral amino acids based on capacitive measurement. The sensor was prepared by first binding mercaptoacetic acid to the surface of a gold electrode, followed by modification with tyramine utilizing carbodiimide activation. Stereoselective binding of an anti-D-amino acid antibody to the hapten-modified sensor surface resulted in capacitance changes that were detected with high sensitivity by a potentiostatic step method. Using capacitance measurement, detection limits of 5 pg of antibody/mL were attained. The exquisite stereoselectivity of the antibody was also utilized in a competitive setup to quantitatively determine the concentration of D-phenylalanine in nonracemic samples. Trace impurities of D-phenylalanine as low as 0.001% could be detected. This method should be useful not only for the enantioselective detection of amino acids as described here but also for investigating other targets (e.g., drugs) using appropriate antibodies.
The sixth chapter is the summary of this thesis and the future prospects for related research.
This thesis reports on the development of several different surface molecular switches which can be used as biosensors. Using self-assembled monolayers, hydrophobic/hydrophilic surface switches capable of responding to external temperature and electrical stimuli were prepared. These switches could supply a smart and biocompatible interface to determine and analyze proteins and antigen-antibody immune systems, which may open a new paradigm for the design of functional biocomposite films.
分子水平上的开关需要一个外部刺激来引起电子和原子核的重排，3种用来开启化学体系功能的最重要的刺激是光能(光子)，电能(电子或空穴)和化学能(以质子、金属离子或特殊分子形式)。最常见的光化学激发开关过程与光异构化和光诱导氧化还原反应是相关的。如果输入的是电化学激发，当然就是氧化还原反应的诱导反应，与化学激发相比，光化学和电化学激发的分子开关更容易发生且响应迅速。利用电化学能代替化学氧化还原作用，具有开、关简便快捷的优势。况且，电化学技术也是监测机器运行的有用方式，电极则是分子系统与宏观世界相连的最佳方式。电场控制的表面分子开关可以用于蛋白质的可控吸附和分离．再结合分子设计、有机合成和高分子化学，还可以给这种表面引入亲疏水功能团或抗原抗体识别对等，方便的实现亲疏水开关或者免疫开关表面。
本论文主要创新之处是基于自组装膜技术、电化学控制技术以及温敏聚合物材料构建具有表面分子开关功能的仿生界面，从而利用这些智能化表面对生物分子及其动态相互作用过程进行实时在线控制和检测。智能化表面(smart surface)通常是指具有可操控开关功能的生物应用表面。智能化表面性质的可逆操控，是在外界激励下发生的。它可以由聚合物、有序自组装膜、纳米材料(特别是金属氧化物)等组成，激励它发生性质可逆转化的因素包括温度、光照、电场、pH值、溶剂等等。在这些外界激励下，表面分子可以发生可逆的构象转化、构型转化、氧化态的转化等等，从而在宏观上，使整个表面呈现出亲疏水性、光学性质、带电性等性质的可逆转化，即可呈现出“开／关”的性质。本论文通过构建的低密度自组装膜，在表面上形成电化学可操控的具有生物识别能力的亲疏水开关，从而实现了对抗生物素一链霉亲和素功能蛋白间微观作用过程的快速、灵敏、可控检测和表征。进一步地，利用温敏高分子材料poly(N-isopropylacrylamide)PNIPAAm与抗BSA抗体合成生物复合物，构建了具有温度敏感开关功能的可再生免疫传感器。该方法可保持生物识别体系的活性和环境，再生的抗原／抗体表面均可重复识别相应目标物，检测灵敏度高、速度快，所构建的温敏开关免疫传感器可重复使用30次以上，解决了目前免疫传感器抗体表面仅能单次使用的弊端，同时为研究蛋白质-蛋白质动态相互作用过程提供了新手段。
本论文共五章内容，主要摘要如下：
第一章综述了表面分子开关的研究现状及其相关技术在生物传感器领域的应用进展。分子自组装和高分子聚合物是构建分子开关的两条重要途径。自组装单分子层是构膜分子与基底材料间发生物化作用而自发形成的一种热力学稳定、排列规则的单层分子膜。这种构膜方式，可以容易的为表面引入各种各样的功能团，这就为制备具有多种不同功能的智能化表面打下了很好的基础。温敏材料是指对温度可感知且可响应并具有功能发现能力的一类材料。具有“温度开关”特性的聚-N异丙基丙烯酰胺(PNIPAAm)是近年来引起研究兴趣的一类高分子材料。利用它对温度响应的敏感性，使其在药物缓释、免疫分析、生命科学等研究领域都有着广泛的潜力。
第二章介绍了基于人工自组装膜技术构建表面亲疏水开关发展生物传感器的新方法。本章利用环糊精作为巯酸分子间距有效的调控手段，以乙醇作为高效的洗脱溶剂，通过自组装方法在金电极表面构建了间距均一、性能稳定的巯基化合物低密度薄膜，由此构建了具有亲疏水可逆开关的智能化表面生物传感器。以高密度自组装膜表面的覆盖度为100％计算可知，α，β，γ三种环糊精分子构建的低密度自组装膜表面的覆盖度分别为61.2％，45.3％和29.2％。通过改变外加电压状况，使巯基化合物构型发生改变，从而实现表面的亲水／疏水性能的转换。通过质谱，核磁，交流阻抗，QCM，荧光等多种检测手段对膜表面可逆过程进行了实时监控。
第三章主要围绕此类亲疏水开关生物传感器进行抗生物素及链霉亲和素可控组装的应用研究。本章采用荧光标记抗生物素、链霉亲和素功能蛋白分子作为研究对象，通过改变外加电流正负情况使得低密度自组装膜表面具有亲疏水可逆转换性能。在pH值为7.4的缓冲溶液中，两种蛋白质由于等电点的差异而带上了两种不同的电荷，由于表面电荷作用及亲疏水性质的转换，两种蛋白质可以在外加电场作用下发生可控组装行为。主要利用EQCM实验和荧光光谱实验对两种蛋白质的可控组装进行了实时监测，对于Avidin蛋白在β-CD构建的低密度自组装膜上的组装过程，将其在负电压下组装30分钟后它的荧光强度是正电压条件下的4.9倍。对于Streptavidin蛋白来说，当外加正电压30分钟后，在β-CD构建的低密度自组装膜表面上蛋白组装量分别是负电压条件下同种组装膜的1.5倍。利用微电极中获得的良好分离分析效果，我们还初步尝试将之应用于微流控芯片体系，发展了一种利用“分子开关”原理构建的蛋白质芯片。
第四章是基于温敏聚合物的表面分子开关构建及抗原抗体可逆识别界面的研究。本章主要研究温敏高分子材料PNIPAAm与抗BSA抗体合成的生物复合物(bioconjugate)组装到金表面与对应抗原BSA识别时的可逆过程。由于这种温敏高分子材料的存在，这个结合过程与抗体-抗原直接结合的情况有很大变化，选择不同分子量的聚合物进行构建，该材料对抗原结合过程中造成的空间位阻有所不同，结合量可通过测定QCM，交流阻抗法，天然PAGE胶以及荧光标记抗原的光亮度加以定量。当抗原抗体结合完毕后，改变溶液的温度，由于温敏材料分子量的差异，高分子量时随着温度升高，抗体结合位点附近的高分子材料会团聚在已经结合的抗原周围，而且会产生较大的空间力以及疏水力，从而将已经结合的抗原从抗体结合部位顶开，使得所构建的温敏开关免疫传感器具有良好的再生功能。高温降至低温过程中，免疫识别体系抗原抗体结合常数差别可以达到两个数量级。高分子量聚合物构建的免疫开关传感器对于抗原抗体结合后表面的再生率最高可以达到89％以上，跟通常文献中大量报道的有机溶液再生表面法(再生率80％-92％)相差很小，而且这个方法基本没有破坏生物识别体系的活性和环境，抗原抗体均可重复利用，这种温敏开关免疫传感器可重复使用30次以上，抗疲劳性较好。综上所述，这种基于温敏聚合物的表面开关可以在免疫生物传感领域进行广泛的应用。
第五章工作围绕基于手性氨基酸抗体构建电容型手性免疫传感器进行相关研究。利用自制手性抗体构建高选择性的新型电容型免疫传感器，设计了逆向竞争法进行检测，得到了很好的响应，这一部分工作仍在进行中。构建的电容性手性免疫传感器从所有的图表中可以看出这种传感器对于小分子的手性氨基酸具有很强的识别和分析能力，检测限可以达到5pg／mL，对氨基酸混合物中痕量D型苯丙氨酸可以达到0.001％的检测灵敏度。竞争法测定灵敏快速，既可以测定D型、L型苯丙氨酸对电极表面半抗原与抗体免疫识别的抑制情况，还可以测定消旋体中单一构型(D型)氨基酸含量，此方法对于混合氨基酸体系中痕量的单一构型抗原检测限比标准的手性色谱分析方法还要低一个数量级，具有高灵敏度、高选择性的特点，为无标记法检测手性氨基酸提供了一种可行的检测方法。具有操作简便，重现性好，成本低廉等一系列优点，对于手性物质的快速在线分析对于临床检测及手性药物分析等具有较大的意义。
第六章是对本论文工作的总结及对下一步工作的展望。
总之，本论文围绕表面分子开关进行了多种生物传感新方法的成功尝试。利用自组装膜技术，温敏聚合物材料等结合外界不同触发条件构建了亲疏水表面开关、温度敏感表面开关生物传感器，形成了具有良好生物相容性的仿生界面，将其应用于蛋白质分子、抗原-抗体体系等进行人工可操控的生物过程的考察与研究均获得了良好的结果。
Controlled study of microscopic fields is one of the most important challenges to scientific and technological development. Scientists use chemical and biological methods to build complex molecular-level devices from the basic building blocks of atomic or molecular microstructure. This strategy, known as "bottom-up" design allows for devices with specific structure or function to be built. Of particular interest has been the development of molecular switches, which could serve as the precursor to the preparation of more complicated molecular devices. Molecular switches are molecules which are capable of changing their behavior in a controlled fashion based on external stimuli such as light, electricity, heat, magnetic fields, or pH. By taking advantage of such switching behavior it should be possible to realize the transmission of information.
Switching behavior requires an external stimuli to cause either an electronic transition or a structural rearrangement. The three most important stimuli are light (absorption of photons), electricity (addition or removal of electrons) and chemical energy (binding of protons, metal ions, or other special molecules). The most common photochemical switches are related to light-induced isomerization and light-induced oxidation and reduction reactions. Electrochemical methods can also be used to produce redox type switching behavior. Moreover, electrochemical techniques are a useful way to monitor the operation of molecular machinery, with the electrode serving as the connection to the macroscopic world. As an example, surface electric switches can be used to control protein adsorption and separation. By combining molecular design, organic synthesis, and polymer chemistry, it is possible to introduce hydrophilic or hydrophobic functional groups or antigen-antibody complexes to the surface resulting in a reversible switch.
This thesis is based on the use of a low-density self-assembled monolayer and temperature-sensitive polymer to build a biocompatible surface. By using these innovative methods, controlled in situ determination and monitoring for biological molecules could be carried on. The intelligent modification of surface properties allows for the detection of a wide range of biological species. The focus of this work has been the development of a sensitive and reversible switch for the detection of specific biomolecules. By using a low-density self-assembled monolayer (SAM) to establish a hydrophobic/hydrophilic switch it has been possible to achieve the rapid and controlled detection of avidin and streptavidin. Reversible control of the surface properties has been achieved with various methods, including: photoillumination, potential effects, and thermal driving. By using temperature-sensitive poly (N-isopropylacrylamide) (PNIPAAm) materials, an immune switch sensor for Anti-BSA antibody and FITC-BSA could be created. The switch is stable in biological environments, does not interfere with the antibody/antigen detection, and can be reused more than 30 times.
In the first chapter we review the research on surface molecular switches and related technical progress in the field of biosensors. Polymers and self-assembly are two important ways to build molecular surface switches. Using self-assembled monolayers could supply a thermodynamically stable and ordered membrane. The structure of SAMs can easily be varied by the introduction of a wide range of functional groups. Temperature-sensitive materials are also found to be good candidates and have the useful ability to respond to external temperature stimuli. In recent years PNIPAAm has attracted interest in the study of temperature-sensitive polymer materials because of its potential application in drug delivery, immunoassays, and life science research.
The second chapter describes using SAMs to constructsmart hydrophobic/hydrophilic reversible surfaces as a new method for biosensor development. The inclusion complex (IC) between 16-mercaptohexadecanoic acid (MHA) andα-,β- orγ-cyclodextrin acted as the space-filling group of the SAM. The unwrapping procedure, the removal of n-CD from the SAM, was accomplished by dissociating the bond n-CD—MHA with ethanol. The surface coverage for LD-SAM-n referring to high-density SAM shows an obvious decrease from 100% to 61.2%, 45.3% and 29.2%, respectively. The thus-prepared low density-SAM shows reversible conformational reorientation under negative and positive potential; this induces changes in wettability, which can be observed by means of contact angle measurements. The removal of n-CD was monitored by quartz crystal microbalance (QCM), nuclear magnetic resonance (NMR), impedance (IMP), and MALDI-TOF-MS.
The third chapter describes the application of our LD-SAM surface to the controlled assembly of two kinds of fluorescent-labeled avidin and streptavidin. Selective protein adsorption was demonstrated on the above-mentioned switchable surface. The assembly of the two proteins on MHA-SAM-n was performed in PBS buffer (pH 7.4) at an applied potential of 0.3 V and -0.3 V (vs.SCE), respectively. From either QCM or fluorescence spectra (FL) data, distinctly different assembly behaviors for the two proteins were observed at two controlled potentials. For example, the emission intensity for avidin-LD-SAM-1 assembled at negative potential for 30 min was about 4.9 times that for assembly at positive potential. The dissimilarity of the surface loading for these two proteins is believed to be mainly due to the charge status difference originating from their isoelectric points. We believe that it might lead to versatile applications, e.g. control of protein adsorption/release in a functionalized capillary or microfluidics channel, or design of intelligent protein chips. We have also attempted to apply this system to a homemade microfluidic chip.
The fourth chapter works on establishing the PNIPAAm-antibody surface that could supply the most effective dissociation of the antigen and regeneration of antibody into reuse of the immunosensors. As a model antibody-antigen system, bovine serum albumin (BSA) and the corresponding antibody (anti-BSA) were chosen. A reversible PNIPAAm-antibody (anti-BSA) conjugates surface was established by triggered control of external temperature. This took advantage of the thermally tunable conformational changes for the PNIPAAm-conjugated antibody surface, and could be used for switchable antigen association and dissociation. The temperature controlling strategy could realized the regeneration of the immunosensor on which immobilized anti-BSA antibodies retain the activity and specificity necessary to carry out more than 30 reproducible assays for BSA. The dissociation reaches 89%, which can compare with the general recovery methods. The controlled binding and unbinding were monitored by quartz crystal microbalance (QCM), confocal fluorescence, native electrophoresis, laser induced fluorescence, and electrochemical impedance.
The fifth chapter describes a highly enantioselective and sensitive immunosensor for the detection of chiral amino acids based on capacitive measurement. The sensor was prepared by first binding mercaptoacetic acid to the surface of a gold electrode, followed by modification with tyramine utilizing carbodiimide activation. Stereoselective binding of an anti-D-amino acid antibody to the hapten-modified sensor surface resulted in capacitance changes that were detected with high sensitivity by a potentiostatic step method. Using capacitance measurement, detection limits of 5 pg of antibody/mL were attained. The exquisite stereoselectivity of the antibody was also utilized in a competitive setup to quantitatively determine the concentration of D-phenylalanine in nonracemic samples. Trace impurities of D-phenylalanine as low as 0.001% could be detected. This method should be useful not only for the enantioselective detection of amino acids as described here but also for investigating other targets (e.g., drugs) using appropriate antibodies.
The sixth chapter is the summary of this thesis and the future prospects for related research.
This thesis reports on the development of several different surface molecular switches which can be used as biosensors. Using self-assembled monolayers, hydrophobic/hydrophilic surface switches capable of responding to external temperature and electrical stimuli were prepared. These switches could supply a smart and biocompatible interface to determine and analyze proteins and antigen-antibody immune systems, which may open a new paradigm for the design of functional biocomposite films.
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