Synthesis of highly functional nanoparticles via a sol-gel process using X-ray scattering methods: from process development to process control

有机发光二极管或薄膜太阳能电池等复杂光电半导体系统中的功能纳米材料的制备和集成的替代工艺的开发，在能源转换和稀土半导体材料缺乏的背景下，具有非常高的科学价值。非水相溶胶-凝胶合成路线(NAR)提供了一种特别适合、成本效益高和可控性好的工艺路线，用于生产更广泛的高功能和晶态金属氧化物(MeO)，其具有可调节的颗粒特性(尺寸、形貌)，用于特定的产品特性(导电性、光学)的修饰，例如，对于铝掺杂的氧化锌(AZO)。为了控制NAR过程，需要应用各种测量技术来获得时间分辨的过程表征，从而为它们实时集成到一个自主的过程控制系统中提供良好的前提条件。颗粒过程的分析和控制通常依赖于合适的过程模型，这些模型一般由一维或多维偏积分-微分方程组成，即粒子数平衡，以及一个或多个常微分方程组来表示液体的质量和能量平衡。这些第一原理模型由本构方程、形核和生长动力学以及破裂和聚集关系来完成。本方案的最终目标是开发、实现和评估一种用于NAR法制备高结晶度MeO的新型自主式多用途工艺控制方案，并研究其扩展到对遵循Sol-Gel路线的一般颗粒工艺的工艺和性能的联合控制。该提案的实验部分由卡尔斯鲁厄理工学院机械过程工程研究所(Hermann Nirschl教授)负责，控制方面将由基尔大学自动化与控制教席(Thomas Meurer教授)开发。

The development of alternative processes for fabrication and integration of functional nano-materials in complex optoelectronic semiconductor systems, such as organic light-emitting diodes or thin-film solar cells, has a very high scientific value in the context of the energy transition and the lack of semiconductors made of rare earth materials. The non-aqueous sol-gel synthesis route (NAR) in the liquid phase delivers a particularly suitable, cost-effective and well controllable process route for the production of a broader variety of highly functional and crystalline metal oxides (MeO) having adjustable particle properties (sizes, morphologies) for the specific modification of the product properties (conductivity, optics), e.g., for aluminum-doped zinc oxide (AZO). To control the NAR process the application of diverse measurement technologies with access to time-resolved process characterization is required and thus provides excellent preconditions for their real time integration into an autonomous process control system. Analysis and control of particle processes typically relies on suitable process models that in general consist of one- or multi-dimensional partial integro-differential equation, i.e., the population balance, and one or multiple ordinary differential equations to represent mass and energy balances of the liquid phase. These first principle models are completed by constitutive equations, nucleation and growth kinetics as well as breakage and aggregation relationships. The final goal of the present proposal is the development, realization and evaluation of a novel autonomous multi-purpose process control scheme for the fabrication process of highly crystalline MeO via NAR and to investigate its extension to combined process and property control for general particle processes following the sol-gel route. The experimental part of the proposal is handled by the Institute of Mechanical Process Engineering at the Karlsruhe Institute of Technology (Prof. Hermann Nirschl) and the control aspects will be developed by the Chair of Automation and Control at the Kiel University (Prof. Thomas Meurer).