EAGER: Exploring unique properties of sub-nm metal nanoparticles for photocatalysis

利用太阳光和催化剂从水中生产氢气是太阳能储存和转换的一个关键的可取策略。这个过程是人工光合作用的一种形式。尽管在这一领域投入了大量的科学努力，但水分解反应的量子效率仍然很低，这表明需要新的方法来解决这一具有挑战性的问题。纽约州立大学石溪分校的调查员亚历山大·奥尔洛夫曾考虑并在该地区工作，调查了一系列半导体材料，取得了一些成功。总结观察表明，尽管La/KTaO_3和硫化锌催化剂具有相当高的量子效率，但这些材料只在紫外光下活跃，仅占到达地球表面的太阳能的5%。因此，挑战仍然是利用可见光来启动水分解反应。可见光催化的最佳QE仅为6.5%，大大低于使该技术在商业上可行所需的10%QE。为了在这一领域取得科学突破，重要的是开发新的光催化剂方法来解决这一具有挑战性的问题。最近，PI开发了一种新的方法来合成含有少于11个原子的亚1 nm金属纳米团簇。在初步实验中，与最活跃的商用催化剂相比，这些纳米颗粒在各种氧化反应中表现出了非凡的活性。这个项目现在将尝试探索这种颗粒对水分解反应的反应性。拟议的项目在开发可持续能源生产的新催化剂方面具有巨大潜力。此外，它还将产生重大的教育影响，因为它将用于在材料科学和工程系启动一个新的环境研究培训领域，重点是环境催化和可持续能源研究。

ABSTRACTProducing hydrogen from water using sunlight and catalysts is a key desirable strategy for solar energy storage and conversion. The process is a form of artificial photosynthesis. Despite significant scientific efforts invested in this field, the quantum efficiency of the water splitting reaction remains low, indicating that new approaches are needed to address this challenging problem. Investigator Alexander Orlov of SUNY at Stony Brook, NY has considered and worked in the area, investigating a series of semiconductor materials, with some success. Summary observations indicate that despite a respectable quantum efficiency of La/KTaO3 and ZnS based catalysts, these materials are only active under UV radiation, which represents only 5% of the solar energy reaching the earths surface. Therefore, the challenge remains to utilize visible light to initiate the water splitting reaction. The best QE for visible light photocatalysis is only 6.5%, which is significantly below the 10% QE necessary to make this technology commercially viable. In order to achieve a scientific breakthrough in this area, it is important to develop new photocatalyst approaches to address this challenging problem. Recently the PI has developed a new procedure for synthesis of sub-1 nm metal nanoclusters containing less than 11 atoms. In preliminary experiments these nanoparticles have exhibited an extraordinary activity in various oxidation reactions as compared to the most active commercially available catalysts. This project will now attempt to explore the reactivity of such particles for the water splitting reaction. The proposed project has a significant potential to develop new catalysts for sustainable energy generation. In addition, it will also have a substantial educational impact, as it will be used to start a new area of environmental research training at the Materials Science and Engineering Department, which will be focused on environmental catalysis and sustainable energy research.