Tandem Perovskite-Molecular Catalyst Based Artificial Leaf for Solar Fuel Synthesis

太阳能转化为化学能是一种很有前途的可持续经济方式。光电化学将二氧化碳转化为各种燃料是一项关键技术，其中太阳能储存在产品的化学键中。由于钙钛矿是最先进的光收集材料，使用高效钙钛矿光伏装置产生二氧化碳转换所需的偏压目前正引起人们的兴趣。此外，还需要一种催化剂来加速二氧化碳的催化作用，并将选择性引向所需的产物。然而，PV在水介质中的稳定性、器件效率、催化剂降解、产物选择性等方面存在局限性。该项目旨在解决这些挑战，并雄心勃勃地开发用于可持续燃料和化学合成的真实太阳能技术。根据中期项目，光电阴极将使用串联钙钛矿装置和分子催化剂组装。优化后的串联光电阴极将与无线人工叶片结构中的光电阳极相结合，用于无偏置二氧化碳转换（图1d）。此外，其他协同生物催化剂将与分子催化剂一起使用，以产生除合成气以外的产品。例如，使用产醋细菌和酶作为共生物催化剂，可以开辟通往高价值化学品和燃料（如乙酸和醇）的不同诱人途径。

Solar energy conversion into chemical energy is a promising approach toward a sustainable economy. Photoelectrochemical conversion of CO2 into various fuels is a key technology, where solar energy is stored in the chemical bonds of the products. Using a high efficiency perovskite photovoltaic device to generate the required bias for CO2 conversion is currently gaining interest as perovskites are state-of-the-art light harvesting materials. In addition, a catalyst is required to accelerate CO2 catalysis and guide the selectivity toward a desired product. However, there are limitations regarding the PV stability in aqueous medium, device efficiency, catalyst degradation, product selectivity, etc. This project aims to address these challenges with the ambition to develop real-world solar technology for sustainable fuel and chemical synthesis. Following on from the midi-project, a photocathode will be assembled using a tandem perovskite device and a molecular catalyst. The optimised tandem photocathode will be combined with a photoanode in a wireless artificial leaf configuration for bias free CO2 conversion (Figure 1d). Additionally, other co-biocatalysts will be used concomitantly with the molecular catalysts to generate products beyond syngas. For example, the use of acetogenic bacteria and enzymes as co-biocatalysts can open different attractive pathways towards higher-value chemicals and fuels such as acetic acid and alcohols.