钙钛矿光伏驱动高效电解水的整体式光电化学池研究

In the process of industrialization, integrated PECs for water splitting driven by PSCs are currently facing with several key issues i.e. efficiency, stability and cost. To this end, this project will construct a novel integrated PEC, in which decomposition voltage for electrolysis of water is offered by solar-driven PSC module, electrode material used is highly active transition metal chalcogenides, and wireless PEC is explored. Specifically, PSCs will be prepared via solution-processed method, and consequently high-performance PSCs with stable output voltage will be further achieved by means of implementing and optimizing interface engineering, with emphasis on introducing inorganic interface materials with stable, highly conductive and energy bandgap-controlled characteristics into the photoactive perovskite layers. These interface layers can extract electrons and holes at the nearby electrodes, leading to the effective separation of photogenerated carriers. Based on this, tandem PSC module will be fabricated, and then applied to electrolytic tank containing chalcogenide-based electrodes. During the photoelectrocatalytic hydrogen production, water reduction dynamics, STH efficiency, and stability of integrated PECs will be examined step-by-step. Also, effect of PSC structure and electrode materials on STH efficiency and stable hydrogen production will be studied on mechanism. Synergic reaction mechanism coupling PSC and electrolytic tank for hydrogen evolution will be verified. This study will provide new materials and technical routes for the development of high-efficiency and low-cost hydrogen fuel devices.

针对光伏驱动电解水的整体式PEC在产业化过程中所面临的效率、稳定性以及成本等关键问题，本项目拟构筑一类全新的整体式PEC，其中电解水的分解电压由全太阳光驱动的PSC组件提供，电解水的电极材料采用催化活性高的过渡金属硫族化合物，光伏组件和电解池之间采用一体式的无线模式。实验采用溶液法构建PSC，通过实施和优化界面工程，在钙钛矿层间引入稳定、高导电、能带可控的无机界面材料，使其在电极附近分别抽取电子和空穴，促进载流子的有效分离，获得高效、有稳定输出电压的PSC器件。基此，构建PSC串联组件，并使之应用于硫族电极构成的电解池。检测整体式PEC在光电产氢过程中的水还原动力学特征、STH效率和产氢稳定性等性能评价参量，并从机理上探究PSC结构、电极材料对PEC的STH效率、产氢稳定性的影响规律，揭示PSC与电解池偶联产氢的协同反应机制，为发展高效低成本的氢燃料装置提供新的材料体系和技术路线。

项目针对光伏驱动电解水的整体式光电催化化学池（PEC）在产业化过程中所面临的效率、稳定性以及成本等关键问题，构筑钙钛矿太阳能电池（PSC）与电解池为一体式PEC。通过优化材料、界面及系统集成工艺，制备出廉价、高效稳定的PSC以及高效的PEC催化体系，具体研究结果包括：.1.廉价高效稳定的PSC器件：通过阳离子与卤素掺杂、晶相工程、界面工程、光谱调控与电池结构优化等策略，从纳米尺度上调控钙钛矿吸光薄膜的结晶性、钝化钙钛矿的缺陷、改善各功能层的能级匹配，深入探究了器件各界面的光生载流子的分离、输运、收集过程与作用机制，制备出高效稳定、低迟滞的平面PSC，光电转化效率超过20%；采用维度调控、离子掺杂以及疏水性导电材料界面修饰提高钙钛矿材料结构稳定性、薄膜和器件的抗湿性和光/热稳定性；通过器件结构调整以及空气环境中器件集成工艺的优化，获得低成本、高效稳定的碳基PSC器件（SnO2/钙钛矿/碳三明治结构），光电转化效率超过16%。.2.高活性催化剂：采用溶液法制备MoS2、MoSe2、BiVO4、g-C3N4等单相/掺杂/复合无机半导体催化材料，通过相态工程、缺陷工程、异原子掺杂等策略调控催化剂的相态、缺陷数量、电子结构、形貌、活性位点等，提升材料的催化活性和稳定性。.3.一体式PEC：将优化好的光阳极、稳定的碳基PSC和辅助电极Pt对电极串联，集成太阳光驱动的PEC池。研究一体式装置的产氢动力学特征、稳定性、电流密度、STH效率等，优化系统的集成制作工艺，最终获得稳定性好的、STH效率高的整体式PEC装置。并从机理上探究PSC结构、电极材料对PEC的STH效率、产氢稳定性的影响规律，揭示PSC与电解池偶联产氢的协同反应机制，为发展高效低成本的氢燃料装置提供新的材料体系和技术路线。. 本项目研究成果目前已发表SCI论文16篇，授权3项。参加国际会议3次，国内会议2次。培养博士生7名（毕业4名），硕士生18名（毕业12名）。