硫醚-金配位相互作用的单分子力谱研究

doi:10.7503/cjcu20180496

摘要/Abstract

摘要：

利用基于原子力显微镜的单分子力谱技术, 定量研究了独立状态下自组装单层膜中的单个硫醚-金相互作用强度, 并从单分子水平探讨了外界因素对硫-金配位键强度的影响. 结果表明, 硫醚分子以配位键形式与金基底结合; 与还原金表面相比, 氧化金表面能够加强硫-金作用强度; 另外, 溶剂对其硫-金配位键强度也产生影响.

关键词: 单硫醚-金配位相互作用, 配位键, 单分子力谱, 溶剂效应, 自组装膜

Abstract:

We have employed atomic force microscopy(AFM)-based single molecule force spectroscopy(SMFS) to quantify the stability of the individual thioether-gold contact in isolated as well as in a self-assembled monolayer. The external factors that affect the sulfide-gold binding strength were investigated at the single-molecule level. The results show that the alkyl sulfide molecule formed coordinate bond on gold surface. Compared with reduced gold, the oxidized gold can enhance the sulfide-gold interactions in both isolated individual monosulfide-gold contacts and in self-assembled membranes(SAMs). Also, the solution condition can affect the stability of Au—S coordinate bonds.

Key words: Interaction between monosulfide and Au surface, Coordinate bond, Single-molecule force spectroscopy, Solvent effect, Self-assembled membrane

中图分类号:

O631

TrendMD:

李逊, 薛玉瑞, 宋宇, 张文科. 硫醚-金配位相互作用的单分子力谱研究. 高等学校化学学报, 2018, 39(12): 2774.

LI Xun,XUE Yurui,SONG Yu,ZHANG Wenke. Coordinate Interaction Between Monosulfide and Au Surfaces^†. Chem. J. Chinese Universities, 2018, 39(12): 2774.

图/表 10

Scheme 1 Schematic drawing of the rupturing of isolated single 2-(ethylthio)ethylamine-gold contacts from the gold surfaces

Fig.1 Histograms of the rupture forces of isolated single monosulfide from oxidized(red) and reduced(blue) gold surfaces, respectively(A) and representative force-extension curves obtained from SMFS experiments, for clarity those force curves were offset from trace to trace by 600 pN along the y-axis(B)

Scheme 2 Schematic drawing of the rupturing of isolated single ethyl-terminated AFM tip and gold contacts from the gold surfaces

Fig.2 Histograms of the unbinding force of ethyl-terminated AFM tips on oxidized(red) and reduced(blue) gold surfaces

Scheme 3 Schematic drawing of the rupturing of isolated single 2-(ethylthio)ethylamine-gold contacts from the oxidized gold surfaces(step Ⅰ) and same AFM tip employed in(step Ⅰ) brought into contact with the sulphydryl-terminated silicon surfaces(step Ⅱ)

Fig.3 Histograms of the rupture forces obtained in step Ⅰ(A) and step Ⅱ(B)

Fig.4 XPS spectra of bare gold and SAMs of 2-(ethylthio)ethylamine on oxidized(solid red trace) and reduced(dashed blue trace) gold surfaces(A) Au4f;(B) S2p.

Scheme 4 Schematic of the detection of monosulfide-gold interactions in amino-terminated SAMs

Fig.5 Histograms of the rupture forces of individual sulfide-gold contacts obtained from SAMs of 2-(ethylthio)ethylamine on oxidized(red) and reduced(blue) gold surfaces in 1,4-dioxane

Fig.6 Comparison of the unbinding forces of individual thioether molecule from SAMs of 2-(ethylthio)ethylamine on reduced gold surfaces in PBS(pH=8.0) and 1,4-dioxane conditions

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