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很有前途的方法。光电化学将二氧化碳转化为各种燃料是一项关键技术，太阳能储存在产品的化学键中。由于钙钛矿是最先进的捕光材料，使用高效率的钙钛矿光伏器件来产生二氧化碳转化所需的偏压目前正受到越来越多的关注。此外，需要一种催化剂来加速二氧化碳催化，并引导选择性接近所需的产品。然而，光伏在水介质中的稳定性、设备效率、催化剂降解、产品选择性等方面都存在限制。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世界太阳能技术。在MIDI项目的基础上，将使用串联钙钛矿装置和分子催化剂组装光电阴极。优化的串联光电阴极将与光阳极结合在无线人造叶子配置中，实现无偏置二氧化碳转化(图1D)。此外，其他共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，使用产乙酸菌和酶作为共生物催化剂，可以开辟不同的诱人途径，获得价值更高的化学品和燃料，如醋酸和酒精。

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.