同步辐射X射线散射和吸收谱联用原位研究PEDOT纳米杂化材料的控制合成机制

本项目利用同步辐射光源先进结构表征技术研究导电聚合物纳米杂化材料的合成机制，原位追踪杂化材料的合成过程及复杂外场环境中的表界面结构及其动态演变路径，揭示“分子设计-材料结构-器件性能”的关联，对开发新型纳米杂化材料、改善器件性能具有重要理论指导意义。本项目计划将带正电胶体纳米粒子和氧化聚合工艺联用，制备形状、尺寸及化学组成精确控制的聚乙撑二氧噻吩-聚(苯乙烯磺酸盐)（PEDOT:PSS）纳米杂化材料。以此为研究对象并结合液体流控实验装置，按照“空间换时间”的思路，搭建一套基于同步辐射X射线散射和UV-Vis吸收谱联用的原位实验方法，揭示杂化材料的五级结构并原位研究其在合成过程或复杂外场环境下的结构演变行为。利用同步辐射原位结构表征和电池充放电装置联用，原位、在线研究材料结构和器件性能关联的本质。为聚合物基新型多功能性杂化材料的设计、制备及应用提供一套新范式。

Synchrotron-based advanced structural characterization protocols contribute to study in situ the material synthesis process, to decipher surface/interface structure and their evolution as a function of the external stimuli, to illuminate the principles lying among “molecular design-material structure-device performance”, all that help us to develop new hybrid materials with controlled structure and better performance. In this project, the positively charged silica colloidal nanoparticle (SiNP) is introduced to the synthesis of the conjugate polymer that acts as a structure template to prepare poly(3,4-ethylenedioxythiophene) polystyrene sulfonate (PEDOT:PSS) hybrid with controlled shape, size and clear chemical composition. The synthesis and the following colloidal stability behavior of the PEDOT:PSS@SiNP hybrid will be studied in situ by combining the characterization of X-ray scattering of synchrotron light and ultraviolet–visible (UV-Vis) spectroscopy with the flow cells. To achieve the goal, two sets of flow cells, i.e., the continuous-flow and stopped-flow ones, will be designed by following the principle that the process occurs in the short reaction time and complex background can be deciphered by scanning along the flow direction of the liquid with X-ray and the complementary UV-Vis light. All these designs will illuminate the formation of the complex quinary structure of the PEDOT:PSS@SiNP hybrid during synthesis and decipher the colloidal stability behavior of the PEDOT:PSS@SiNP hybrid under complex environment. To disclose the structure-property relationship, the PEDOT:PSS@SiNP hybrid will be fabricated into electrodes of a symmetric supercapacitor, which will be installed in a home-made sample holder adapted for the synchrotron beamline environment. Under the help of the battery charging device, we can collect the structure information of the electrodes with synchrotron-based X-ray scattering measurements during the charging/discharging of the supercapacitor. The detailed information will shed light on the relationship of molecular design-controlled synthesis-materials structure-device performance and thus guide the development of new hybrid material with multifunction.