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 |