新型叠层光解水分子器件的组装和性能优化

Utilization of solar energy to replace traditional fossil fuels is a tendency to develop a sustainable society in the future. Conversion of solar energy into chemical fuels, such as hydrogen, by visible light driven water splitting using dye-sensitized photoelectrochemical cells (DS-PECs) is regarded as a particularly attractive approach. During the past years, DS-PECs attracted worldwide attention and experienced rapid development. However, these approaches suffer from inherent drawbacks, for instance decreased total light absorption by photosensitizer (PS); serious light damage and desorption of PS and catalyst from photoanode; low stabilities or poor photoactivities of molecular devices, and so on. Therefore, based on our experience, in this project, we devote ourselves to develop series of new efficient multi-layer photoanodes to improve the photoactive and stability of the whole DS-PECs. To meet those shortages, we’ll try to improve the fastness of dye used in molecular devices through increasing the number of adsorption group; Broaden the light absorption band and improve the utilization efficiency of light through selection and development of some structural stability, wide light absorption and high energy level organic dye molecules as auxiliary energy photosensitive dye or isolation layer; Decrease the light damage and the desorption through functional modification with the auxiliary isolate layer; Reduce invalid electron transfer in the system through functional modification photoanodes with application of some suitable organic polymer materials as auxiliary layer.

利用太阳光分解水制取氢气是人们解决未来能源需求的一条可行性路径，而染料敏化光解水分子器件被认为是实现分子水平太阳能转换，高效利用太阳光分解水制取氢气的理想方法之一。本项目基于已有的工作基础，针对目前光解水分子器件中光利用率不高、光破坏和脱吸附严重、无效电子传递严重、稳定性不高等问题，致力于通过选用和优化染料敏化光解水分子器件中用到的光敏染料，通过增加染料上的吸附基团数量来提高吸附牢度；同时选用和开发一些结构稳定、光吸收范围较宽，能量较高的有机分子染料作为辅助光敏染料或隔离层；结合目前已经开发的具有较好稳定性和催化性能的金属有机分子作为水氧化或质子还原催化剂，组装新型高效的叠层光解水分子器件，用以拓宽光吸收谱带、提高光利用率和隔绝光解水产生的活性氧对光敏染料的破坏，减少体系中的无效电子传递，构建高活性和高稳定性的染料敏化光解水分子器件，提高整个光电化学池的光解水性能和工作寿命。

利用太阳能分解水制氢是一种经济、清洁的制氢方法，这方面的研究直接关系到能源开发与环境保护，是近年来生物无机化学和可再生能源领域中重要的前沿课题之一。利用太阳光分解水制取氢气是人们解决未来能源需求的一条可行性路径，而染料敏化光解水分子器件被认为是实现分子水平太阳能转换，高效利用太阳光分解水制取氢气的理想方法。目前，人们正逐渐将光解水制氢的研究的主要方向转向功能化和器件化，设计并合成具有光学活性的高效均相水氧化催化剂，构建由纳米半导体材料与光活性催化水氧化金属配合物组成的分子器件等，并由此构建光解水制氢分子器件，成功实现光解水同时制取氢气和氧气。.本项目主要从分子催化剂的开发，光催化分子器件的构建和优化、电催化器件的构建和性能等方面进行基础研究和探索。针对分子器件光解水效率低，稳定性差等关键科学问题，运用分子工程手段，通过巧妙设计和组装新型高效的光阳极，调控和优化分子催化剂/半导体界面电荷传输性能，构建更加高效的光解水分子器件。.1.运用分子工程构建光解水分子器件； .2.通过微纳米结构控制改性基底表面纳米结构，构建高效电解水催化剂器件；.3.通过微纳米结构控制开发异质原子掺杂Cu2Se-Cu2O复合材料，构建高效电解水催化剂器件；.4.运用纳米工程开发高效超薄二维薄膜光敏材料和高效钙钛矿结构的CoSn(OH)6催化剂