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金电极上短链硫醇和DNA自组装单层的基本电化学行为研究

中文摘要第10-14页
英文摘要第14-19页
本论文工作的主要创新之处第20-21页
Chapter One.Introduction第21-108页
    1.1 Progesses of studies on the electron transfer through DNA第21-32页
        1.1.1 Reasearches on the electron transfer through DNA第21-32页
            1. Electrochemical study第22-27页
            2. Photoelectrochemical study第27-28页
            3. Photochemical study第28-32页
        1.1.2 Future research directions for electron transfer through DNA第32页
    1.2 Researches on the fundamental behaviors of gold electrode第32-45页
        1.2.1 Factors influencing electrochemical behavior of gold electrode第33-36页
            1. Electrochemical polarization (altering substrate potential of gold)第33-35页
            2. pH,polarization time and temperature第35页
            3. Crystal surface of gold第35页
            4. Adsorption of anions第35-36页
        1.2.2 Adsorption abilities of water and anions on gold第36-41页
        1.2.3 Methods for calculating surface area of gold electrode第41-45页
            1. Randles-Sevcik equation第41-42页
            2. Oxygen adsorption第42-43页
            3. Iodine adsotption第43页
            4. Underpotential deposition第43-44页
            5. According to Gouy-Chapman theory第44-45页
    1.3 Factors influcing the self-assembly of thiols on gold第45-51页
        1.3.1 Surface pretreatment of gold第45-47页
        1.3.2 Potential control第47-48页
        1.3.3 Underpotential deposition第48-49页
        1.3.4 Running velocity of solvent第49页
        1.3.5 Methods for self-assembly第49-50页
        1.3.6 Other factors(solvent,temperature,chain length of thiols,assembly time and content of oxygen in assembly solvent)第50-51页
    1.4 Summarization on the important interfacial parameters of Au-SAMs第51-58页
    1.5 Summarization on the research progress on the tunneling process through self-assembled monolayers第58-77页
        1.5.1 Methods for calculating the parameters (k,α)in tunneling equation第58-70页
            1. Cyclic voltammetry(CV)第58-63页
            2. Electrochemical impedance spectroscopy (EIS)第63-65页
            3. Alternating current voltammetry (ACV)第65-66页
            4. Chronoamperometry (CA)第66页
            5. Open circuit potential (OCP)determination第66页
            6. Scanning electrochemical microscopy (SECM)第66-68页
            7. Indirect laser induced temperature jump technique(ILIT)第68-70页
        1.5.2 Methods and influencing factors for calulating tunneling constant β in tunneling equation第70-75页
            1. Methods for calculating β第70-72页
            2. Influencing factors for calculating β第72-75页
        1.5.3 Application of tunneling equation第75-77页
            1. Judging the existence of collapsed sites in Au-SAMs第75-76页
            2. Discussing the relationship of surafce coverage of collapsed sites with the thickness of Au-SAMs第76-77页
    1.6 The aim of the research in the thesis第77页
    1.7 参考文献第77-108页
Chapter Two. Direct Current Potential Control Characteristics of Short-chain Thiols ofThioctic Acid and Mercaptohexanol Self-assembled on Gold第108-155页
    2.1 Introduction第108-110页
    2.2 Experimental第110-114页
        2.2.1 Chemicals and apparatus第110页
        2.2.2 Pretreatment of gold electrodes第110-111页
        2.2.3 Preparation of SAMs第111-112页
        2.2.4 Electrochemical characterization第112-114页
    2.3 Results and Discussion第114-127页
        2.3.1 Self-assembly of TA and MCH on gold for a short time (30 min) under different E_(dc)第114页
        2.3.2 Self-assembly of TA and MCH on gold for a long time (24 h) under E_(dc) values第114-115页
        2.3.3 Self-assembly of TA and MCH on gold for different time (from 2 min to 72 h) under the optimal E_(dc)第115-121页
        2.3.4 Relationships of C~v,Φ_(1Hz)~C and Δj-logR_(ct) for TA-SAMs and MCH-SAMs第121-123页
        2.3.5 Discussion of the possible mechanism for the effect of E_(dc) on the self-assembly of short-chain thiols (TA and MCH) on gold第123-126页
        2.3.6 Exploration of the effect of chain length on the characteristics of SAMs from the literature第126-127页
    2.4 Conclusions第127-128页
    2.5 References第128-137页
    2.6 Supporting Information第137-146页
    References第146-155页
Chapter Three. Studies on the Effect of Solvents on Self-assembly of Thioctic Acid andMercaptohexanol on Gold第155-178页
    3.1 Introduction第155-157页
    3.2 Experimental第157-159页
        3.2.1 Chemicals and apparatus第157页
        3.2.2 Pretreatment of gold electrodes第157-158页
        3.2.3 Preparation of SAMs第158页
        3.2.4 Electrochemical characterization第158-159页
    3.3 Results and Discussion第159-167页
        3.3.1 Electrochemical characteristics of TA-SAMs and MCH-SAMs on gold assembled in different solvents第159-162页
        3.3.2 Relationships of C~v,Φ_(1Hz)~C and Δj~logR_(ct) for TA-SAMs and MCH-SAMs第162-165页
        3.3.3 Exploration of the effect of solvents on self-assembly of thiols with different terminal groups on gold第165-167页
    3.4 Conclusions第167-171页
    3.5 References第171-178页
Chapter Four. Electrochemical Studies on the Permeable Characteristics of Thiol-modifiedDouble-stranded DNA Self-assembled Monolayers on Gold第178-216页
    4.1 Introduction第178-179页
    4.2 Experimental第179-183页
        4.2.1 Reagents and apparatus第179-180页
        4.2.2 Preparation of ds-DNA-SAMs on gold第180页
        4.2.3 Electrochemical characterization第180-183页
    4.3 Results and Discussion第183-193页
        4.3.1 Electrochemically characterizing the permeability of ds-DNA-SAMs on gold assembled under different NaCl concentrations第183-186页
        4.3.2 Construction of a simple model for exploring the permeable characteristics of ds-DNA-SAMs on gold第186-189页
        4.3.3 Confirmation of the simple model and its application to explore the mechanism for ions permeability of ds-DNA-SAMs on gold第189-193页
    4.4 Conclusions第193-194页
    4.5 References第194-204页
    4.6 Supporting Information第204-210页
    4.7 Appendix第210-216页
Chapter Five. Electrochemical Exploration of the Specific Structural Characteristics ofThiol-modified Single-stranded DNA Self-assembled Monolayers on Gold第216-248页
    5.1 Introduction第216-217页
    5.2 Experimental第217-220页
        5.2.1 Reagents and apparatus第217-218页
        5.2.2 Preparation of ss-DNA-SAMs on gold第218页
        5.2.3 Electrochemical characterization第218-220页
    5.3 Results and Discussion第220-229页
        5.3.1 Electrochemical exploration of the specific structural characteristics of ss-DNA-SAMs on gold assembled under different NaCl concentrations第220-222页
        5.3.2 Construction of a simple model to describe the configuration of ss-DNA-SAMs on gold第222-226页
        5.3.3 Confirmation of the simple model by comparing with literature reports and our experimental results and exploration of its application in designing DNA sensor第226-229页
    5.4 Conclusions第229-230页
    5.5 References第230-237页
    5.6 Supporting Information第237-242页
    5.7 Appendix第242-248页
Chapter Six. Effect of Monovalent Cations (Li~+, Na~+, K~+, Cs~+) on the Self-assembly ofThiol-modified Double-stranded and Single-stranded DNA on Gold Electrode第248-274页
    6.1 Introduction第248-249页
    6.2 Experimental第249-253页
        6.2.1 Chemicals and apparatus第249-250页
        6.2.2 Preparation of DNA-SAMs第250页
        6.2.3 Electrochemical characterization第250-253页
    6.3 Results and Discussion第253-260页
        6.3.1 Electrochemically characterizing ds-DNA-SAMs on gold assembled in the solutions with different monovalent cations (0.1 M or 1 M LiCl,NaCl, KCl, CsCl)第253-255页
        6.3.2 Electrochemically characterizing ss-DNA-SAMs on gold assembled in the solutions with different monovalent cations (0.1 M or 1 M LiCl, NaCl, KCl, CsCl)第255-258页
        6.3.3 Comparing the different effects of monovalent cations on self-assembly of ds-DNA-SAMs and ss-DNA-SAMs on gold第258-260页
    6.4 Conclusions第260-262页
    6.5 References第262-268页
    6.6 Supporting Information第268-274页
附录 攻读博士学位期间发表和待发表的论文第274-276页
致谢第276-278页

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