Vapor-Phase Molecular Doping in Covalent Organosiloxane Network Thin Films Via a Lewis Acid–Base Interaction for Enhanced Mechanical Properties,ACS Applied Materials & Interfaces

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Vapor-Phase Molecular Doping in Covalent Organosiloxane Network Thin Films Via a Lewis Acid–Base Interaction for Enhanced Mechanical Properties
ACS Applied Materials & Interfaces ( IF 8.3 ) Pub Date : 2021-10-15 , DOI: 10.1021/acsami.1c13257
Mingjun Qiu ₁ , Weiwei Du ₁ , Xinyu Luo ₁ , Siyuan Zhu _{2,

3} , Yingwu Luo ₁ , Junjie Zhao ₁

Affiliation

Incorporating inorganic components in organosiloxane polymer thin films for enhanced mechanical properties could enable better durability and longevity of functional coatings for a multitude of applications. However, molecularly dispersing the inorganic dopants while preserving the cyclosiloxane rings represents a challenge for cross-linked organosiloxane networks. Here, we report a molecular doping strategy using vapor-phase infiltration. On the basis of the proper Lewis acid–base interaction between diethyl zinc (DEZ) and cyclotrisiloxane rings, we achieved a complete infiltration of the organometallic precursors and well-distributed Zn–OH terminal groups formed in the initiated chemical vapor deposited poly(1,3,5-trimethyl-1,3,5-trivinylcyclotrisiloxane) (PV₃D₃) films. X-ray photoelectron spectroscopy and nanoscale infrared spectroscopy together with density functional theory simulation reveal that the formation of a Lewis acid–base adduct rather than a ring-opening process is possibly involved in anchoring DEZ in the cross-linked network of PV₃D₃. Because of the incorporation of Zn–OH components, the organic–inorganic hybrid films obtained via our vapor-phase molecular doping exhibit a 10.2% larger elastic modulus and 67.0% higher hardness than the pristine PV₃D₃. Unveiling the reaction mechanisms between organometallic precursors and cross-linked organic networks provides new insights for expanding the vapor-phase processing strategies for engineering hybrid materials at the nanoscale.

中文翻译：

通过路易斯酸碱相互作用在共价有机硅氧烷网络薄膜中进行气相分子掺杂以增强机械性能

在有机硅氧烷聚合物薄膜中加入无机成分以增强机械性能，可以使多种应用的功能涂层具有更好的耐用性和寿命。然而，在保留环硅氧烷环的同时以分子方式分散无机掺杂剂对交联有机硅氧烷网络来说是一个挑战。在这里，我们报告了一种使用气相渗透的分子掺杂策略。基于二乙基锌（DEZ）和环三硅氧烷环之间适当的路易斯酸碱相互作用，我们实现了有机金属前体的完全渗透和在引发的化学气相沉积聚（1， 3,5-三甲基-1,3,5-三乙烯基环三硅氧烷）（PV ₃ D ₃ ）薄膜。 X射线光电子能谱、纳米级红外光谱以及密度泛函理论模拟表明，DEZ在PV ₃ D ₃交联网络中的锚定可能涉及路易斯酸碱加合物的形成，而不是开环过程。。由于加入了 Zn-OH 成分，通过气相分子掺杂获得的有机-无机杂化薄膜的弹性模量比原始 PV ₃ D ₃高 10.2％，硬度高 67.0％。揭示有机金属前体和交联有机网络之间的反应机制，为扩展纳米级工程混合材料的气相加工策略提供了新的见解。

更新日期：2021-10-15

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