有机电子给/受体共插层LDHs复合体系的设计，构筑及其光电催化性能研究

Light excitation can realize the electron transfer between organic electron donor and accepter at microscopic contact, and results in the separation of photo-generated electron/holes to form the reductant /oxidant. However, the photo/thermostability and photocatalytic properties of organic electron donor/accepter remain to be investigated and impoved. This project aimed to, employing the intercalation capability of one type of inorganic layered double hydroxides(LDHs) and theoretical calculation of structural design, make the organic electron donor/accepter with matched energy level involved into the interlayers of LDHs by co-intercalation process, which realized the 2D photo-electron transfer and obtained the photo-generated electron/hole with certain energy for photoelectrochemical water splitting, photocatalytic oxidation and reduction reactions. The optical absorption, photo-generated electron/hole separation, transportation and reaction of this co-intercalation composites can be adjusted by multiple co-intercalating, doped mixing and being thin film for the LDHs with adjustable elements, charges and interlayered configurations. The structure-activity relationship will be revealed, and the chemical preparation method for this composite will be established, in order to obtain a novel LDHs based organic electron donor/accepter co-intercalated composite photocatalysis with stable performance and well-defined structure. This project will be significant academically for the development of inorganic materials chemistry and inorganic solid state chemistry, and is also vital in application research for enriching the photocatalysis materials, developing novel opto-electric functional composite materials.

光激发能实现微观接触的有机电子给体和受体间电子转移，导致光生电子和空穴的分离而成为还原剂和氧化剂，但有机给受体的光热稳定性和光生电子-空穴的光催化性能有待研究和提高。本课题旨在利用一类无机层状复合氢氧化物（LDHs）的可插层性，结合理论计算进行结构设计，使能级匹配的有机电子给/受体共插层于LDHs层间以实现二维光致电子转移，获得具有特定能量的光生电子与空穴，进而用于光电化学分解水，光催化氧化与还原等反应。利用LDHs元素、电荷、层间结构可调等特点，采用多元共插层、掺杂复合、薄膜制备等手段对光吸收，电子/空穴分离，传输和反应进行调控，研究其构-效关系，建立针对此类复合体系的化学制备方法，从而得到性能稳定，结构明确的新型LDHs基有机电子给受体共插层复合光催化剂。本课题对于发展无机材料化学和无机固体化学有重要的学术价值，对于丰富光催化材料的研究领域，拓展新型复合光电功能材料有重要的应用研究价值

光激发能实现微观接触的能级匹配的有机电子给体和受体间电子转移，导致光生电子和空穴的分离而分别成为还原剂和氧化剂，但有机给受体的光热稳定性和光生电子-空穴的光催化性能有待研究和提高。本课题利用一类无机层状复合氢氧化物(LDHs)的可插层性与剥层组装特性，结合理论计算进行结构设计，使能级匹配的有机电子给/受体共插层于LDHs层间以实现二维光致电子转移，获得具有特定能量的光生电子与空穴，进而用于光催化和光电探测等领域。利用LDHs的元素、电荷、层间结构可调等特点，采用多元共插层、掺杂复合、薄膜制备等手段对光吸收，电子/空穴分离，传输和反应进行调控，研究其构-效关系，建立针对此类复合体系的化学制备方法，从而得到性能稳定，结构明确的新型LDHs基有机电子给受体共插层复合光功能材料。. 本课题成功的实现了有机电子给受体在LDHs层间的共插层和共组装，实现了建立了成熟的有机电子给受体共插层或共组装的化学方法，实现了二维层间的电子转移和能量转移，用于光解水产氢，光催化还原CO2、荧光检测和光电探测等领域，总结其中的构-效关系，发表了研究论文，申请了发明专利。有机电子给受体、量子点或有机染料进入层间后，发光强度，发光寿命等性能得到不同程度的提高和强化，如：BP4分子共插层后，其发光量子产率，寿命和强度分别增加了近14，4和45倍，并且其辐射跃迁速率常数增加近3倍。CdTe量子点进入层间后，发光强度增强了10倍。. 本课题对于发展插层化学和无机-有机复合材料化学有重要的学术价值，对于丰富光催化材料的研究领域，拓展新型复合光电功能材料有重要的应用研究价值。