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Organic Monolayers by B(C6F5)3-Catalyzed Siloxanation of Oxidized Silicon Surfaces

机译:B(C6F5)3-氧化硅表面的硅氧烷氧化有机单层

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摘要

Inspired by the homogeneous catalyst tris(pentafluorophenyl) borane [B(C6F5)3], which acts as a promotor of Si–H bond activation, we developed and studied a method of modifying silicon oxide surfaces using hydrosilanes with B(C6F5)3 as the catalyst. This dedihydrosiloxanation reaction yields complete surface coverage within 10 min at room temperature. Organic monolayers derived from hydrosilanes with varying carbon chain lengths (C8–C18) were prepared on oxidized Si(111) surfaces, and the thermal and hydrolytic stabilities of the obtained monolayers were investigated in acidic (pH 3) medium, basic (pH 11) medium, phosphate-buffered saline (PBS), and deionized water (neutral conditions) for up to 30 days. DFT calculations were carried out to gain insight into the mechanism, and the computational results support a mechanism involving silane activation with B(C6F5)3. This catalyzed reaction path proceeds through a low-barrier-height transition state compared to the noncatalyzed reaction path.
机译:受均相催化剂三(五氟苯基)硼烷[B(C6F5)3]的启发,该催化剂可促进Si–H键的活化,我们开发并研究了使用氢硅烷以B(C6F5)3作为改性硅氧化物表面的方法。催化剂。在室温下,该脱二氢硅氧烷化反应可在10分钟内完全覆盖表面。在氧化的Si(111)表面上制备了具有可变碳链长度(C8–C18)的氢硅烷衍生的有机单层,并在碱性(pH 11)的酸性(pH 3)介质中研究了所得单层的热稳定性和水解稳定性。培养基,磷酸盐缓冲盐水(PBS)和去离子水(中性条件)长达30天。进行了DFT计算以深入了解该机理,并且计算结果支持了一种涉及用B(C6F5)3进行硅烷活化的机理。与非催化反应路径相比,该催化反应路径通过低势垒高度的过渡态。

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