Molecular hybrid photocatalysts for selective solar H2 and material generation from real life wastes

太阳能废物光转化是一种利用充足的阳光从废弃废物和水中产生有价值的H2燃料和化学物质的过程，为废物管理、清洁燃料发电和材料生产等许多全球性挑战提供了解决方案。尽管具有潜力，但目前最先进的光重整工艺存在主要缺陷，包括使用高度碱性介质和非选择性产品生成，这妨碍了它们的大规模实施。“Waste2Fuel”计划试图通过使用混合光催化剂来解决这些缺陷，将分子氧化催化剂固定在光催化剂表面，在良性条件下进行选择性的废物光转化。这种方法的灵感来自于最近使用类似混合策略的选择性CO2光还原的成功。在不同的目标中，首先将分子催化剂通过共价键固定在阳极上，并优化条件，通过表面结合催化剂在水条件下获得选择性电化学废物氧化。然后将分子催化剂接枝到光催化剂上，得到混合光阳极，随后将用于选择性太阳能废物光转化。我们推测，在光重整过程中，将发生从光催化剂到锚定分子催化剂的初始空穴转移，后者依次氧化废底物，从而获得与分子配合物通常观察到的高效率和产物选择性。我们的最终目标是开发一个可扩展的10.10 cm2的面板，表面沉积混合催化剂用于大规模的太阳能光重整，证明其适用性。这项研究的成功完成将使废物光转化过程商业化，有助于燃料和材料的可持续生产，同时回收我们社会产生的废物。

Solar waste photoreforming is a process that generates valuable H2 fuel and chemicals from discarded waste and water using abundant sunlight, providing solutions to many global challenges including waste management, clean fuel generation, and material production. Despite the potential, current state-of-the-art photoreforming processes suffer from major deficiencies including the use of highly basic medium and nonselective product generation that preclude their large-scale implementation. The "Waste2Fuel" proposal seeks to address these deficiencies by employing hybrid photocatalysts, with molecular oxidation catalysts anchored onto photocatalyst surfaces, to carry out selective waste photoreforming under benign conditions. Inspiration to such an approach comes from the recent success in selective CO2 photoreduction with similar hybrid strategy. Among different objectives, molecular catalysts will be first immobilized onto anodes by covalent bond, and conditions will be optimized to obtain selective electrochemical waste oxidation under aqueous conditions by surface-bound catalysts. The molecular catalysts will then be grafted onto photocatalysts to get hybrid photoanodes, which will be subsequently employed for selective solar waste photoreforming. We surmise that during photoreforming, initial hole transfer from photocatalyst to the anchored molecular catalyst will take place, with the latter oxidizing waste substrates in turn, giving high efficiency and product selectivity as is generally observed with molecular complexes. Our final objective is to develop a scalable 10.10 cm2 panel with surface deposited hybrid catalyst for large-scale solar photoreforming, demonstrating its applicability. Successful completion of the research would enable commercialization of the waste photoreforming process, contributing towards the sustainable production of fuel and materials, while at the same time, recycling the generating wastes of our society.