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

将太阳能转化为化学能是实现可持续经济的一种有前途的方法。将CO2光电化学转化为各种燃料是一项关键技术，其中太阳能储存在产物的化学键中。使用高效钙钛矿光伏器件来产生用于CO2转化所需的偏压目前正受到关注，因为钙钛矿是最先进的光捕获材料。此外，需要催化剂来加速CO2催化并引导朝向所需产物的选择性。然而，在水介质中的光伏稳定性，器件效率，催化剂降解，产品选择性等方面存在局限性，该项目旨在解决这些挑战，并致力于开发可持续燃料和化学合成的真实太阳能技术。在midi项目之后，将使用串联钙钛矿设备和分子催化剂组装光电阴极。优化的串联光电阴极将与无线人工叶片配置中的光电阳极相结合，以实现无偏压CO2转换（图1d）。此外，其他辅助生物催化剂将与分子催化剂一起使用，以产生合成气以外的产品。例如，使用产乙酸细菌和酶作为辅助生物催化剂可以打开不同的有吸引力的途径，以获得更高价值的化学品和燃料，如乙酸和醇。

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.