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

太阳能废物光重整是一种利用充足的阳光从废物和水中产生有价值的氢气燃料和化学品的过程，为包括废物管理、清洁燃料产生和材料生产在内的许多全球挑战提供了解决方案。尽管有潜力，但目前最先进的光重整过程存在着重大缺陷，包括使用高度基本的介质和非选择性的产品生成，这阻碍了它们的大规模实施。“Wast2Fuel”建议旨在解决这些不足之处，采用混合型光催化剂，将分子氧化催化剂固定在光催化剂表面，在良好的条件下进行选择性废物光转化。这种方法的灵感来自最近在选择性二氧化碳光还原方面的成功，以及类似的混合策略。在不同的目标中，分子催化剂将首先以共价键的方式固定在阳极上，并将优化条件，以获得表面结合催化剂在水相条件下选择性地氧化废水。然后将分子催化剂嫁接到光催化剂上，得到复合光阳极，随后将其用于选择性太阳能废物的光重整。我们推测，在光重整过程中，初始空穴将从光催化剂转移到锚定的分子催化剂，而锚定的分子催化剂依次氧化废底物，从而获得高效率和高选择性，就像通常观察到的分子络合物一样。我们的最终目标是开发一种可扩展的10.10平方厘米的面板，表面沉积混合催化剂，用于大规模的太阳能光重整，展示其适用性。这项研究的成功完成将使废物光重整过程商业化，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.