Wang Hao, Griffiths Jon-Paul, Egdell Russell G, Moloney Mark G, Foord John S
Chemistry Research Laboratory, Department of Chemistry, University of Oxford, Mansfield Road, Oxford OX1 3TA, United Kingdom.
Langmuir. 2008 Feb 5;24(3):862-8. doi: 10.1021/la702701p. Epub 2008 Jan 5.
A rapid route to the chemical functionalization of hydrogen-terminated diamond surfaces deposited by chemical vapor deposition involving their reaction with substituted diaryl carbenes has been investigated. To avoid difficulties in the handling of highly reactive compounds, the carbene is generated in situ from the thermal decomposition at 400 K of a thin film of the corresponding diaryl diazomethane precursor deposited at the diamond interface. X-ray photoelectron spectroscopy (XPS) has been used to verify that surface functionalization using two starting compounds, bis(4-iodophenyl) diazomethane and bis(4-nitrophenyl) diazomethane, can be achieved using this approach in agreement with recent theoretical studies. The surface grafting density is measured to be around 10(14) cm(-2) in each case. The chemistry observed is found to be insensitive to the detailed properties of the diamond film and to the presence of oxygen contamination at the hydrogen-terminated diamond surface. We further demonstrate the utility of the approach, in the case of the bound nitrophenyl compound, by its reduction to the corresponding primary amine followed by reaction with fluorescein isothiocyanate to achieve fluorescent tagging of the diamond interface.
研究了一种通过化学气相沉积法制备的氢端基金刚石表面进行化学官能化的快速途径,该途径涉及它们与取代二芳基卡宾的反应。为避免处理高反应性化合物时遇到困难,卡宾通过在400K下热分解沉积在金刚石界面处的相应二芳基重氮甲烷前体薄膜原位生成。X射线光电子能谱(XPS)已被用于验证使用两种起始化合物双(4-碘苯基)重氮甲烷和双(4-硝基苯基)重氮甲烷进行表面官能化可以通过这种方法实现,这与最近的理论研究一致。在每种情况下,表面接枝密度测量值约为10(14) cm(-2)。发现观察到的化学现象对金刚石薄膜的详细性质以及氢端基金刚石表面的氧污染的存在不敏感。对于结合的硝基苯基化合物,我们通过将其还原为相应的伯胺,然后与异硫氰酸荧光素反应以实现金刚石界面的荧光标记,进一步证明了该方法的实用性。