Collaborative Research: SusChEM: The Design and Study of Systems for Making Solar Hydrogen

该项目由美国国家科学基金会化学催化项目资助，由罗切斯特大学的David McCamant和Richard Eisenberg教授以及布法罗大学的Michael Detty和David Watson教授四人合作完成。这项研究的目标是对利用太阳能将水分子分解成氢（H2）和氧（O2）气体产生氢的化学系统有一个新的基本认识。对于太阳能的捕获和储存，水分解是理想的反应。H2和O2复合制取水是一种方便、清洁的能源。这个研究项目包括在艾森伯格实验室制造新的分子来促进水分解反应，在迪蒂实验室制造新的染料分子来吸收来自太阳的可见光，在麦卡曼特实验室研究这些分子吸收光后发生的快速光化学反应，在沃森实验室制造新的纳米粒子半导体系统作为太阳能制氢的支架。每位研究人员都为合作研究带来了不同的观点和技能，从而对太阳能转换中一个根本性的挑战性问题有了重要的新认识。在外联工作中，获得这笔资助的科学家正在与纽约州罗切斯特市和布法罗市的当地小学合作，开发与能源有关的科学模块，以激励下一代科学家。本研究由美国国家科学基金会化学催化项目资助，包括设计和研究水相质子光驱动生成H2的系统，以及相关的光化学和光物理研究，以充分了解这种转化。该反应对应于水分解的还原侧2H+ + 2e- - H2，是人工光合作用和光转化为储存的化学势能的关键反应。虽然看起来很简单，但光驱动生成H2的详细机制是复杂的，特别是在一个集成系统中。在本项目中，研究人员将重点关注三个具体的研究目标：新发色团的合成和表征；含有常见金属离子的新型催化剂的设计和开发，这些催化剂在光化学系统中对水介质中的光驱动质子还原有效；构建基于SrTiO3等半导体材料作为结构支架和CuAlO2等光电阴极材料的新型集成质子还原体系，消除质子还原对化学电子源的需求。这些领域中的每一个都在探索尖端的飞秒时间分辨光谱，能够探测涉及初始光驱动事件的动力学，更长的持续时间瞬态吸收方法，以跟踪后来的电子转移，以及可以建立催化机制，分子和界面结构以及长期系统稳定性的稳态方法。获得这笔资助的科学家还与纽约州罗切斯特市和布法罗市的当地小学合作，开发与能源相关的科学模块，以激励下一代科学家。

This project is supported by the Chemical Catalysis Program of the National Science Foundation and involves a four-way collaboration between Professors David McCamant and Richard Eisenberg of the University of Rochester, and Michael Detty and David Watson of the University at Buffalo. The goal of the research is to develop a new fundamental understanding of chemical systems that can produce hydrogen by splitting water molecules into hydrogen (H2) and oxygen (O2) gases using solar energy. For the capture and storage of solar energy, water splitting is the ideal reaction. The recombination of H2 and O2 to produce water is a convenient and clean source of energy upon demand. This research project involves making new molecules to facilitate the water splitting reaction in the Eisenberg lab, making new dye molecules to absorb visible light from the sun in the Detty lab, studying the fast photochemical reactions that occur after those molecules absorb light in the McCamant lab, and making new nanoparticle semiconductor systems as scaffolds for solar hydrogen production in the Watson lab. Each of the investigators brings to the collaborative research different perspectives and skills that are leading to a significant new understanding of a fundamentally challenging problem in solar energy conversion. In outreach efforts, the scientists supported by this grant are working with local elementary schools in Rochester and Buffalo, New York, to develop energy-related science modules that can inspire the next generation of scientists. This research, funded by the Chemical Catalysis Program of the NSF, consists of the design and study of systems for the light-driven generation of H2 from aqueous protons, and associated photochemical and photophysical investigations to fully understand this transformation. The reaction corresponds to the reductive side of water splitting, 2H+ + 2e- - H2, which is the key reaction in artificial photosynthesis and the conversion of light into stored chemical potential energy. While seemingly simple, the detailed mechanism of the light-driven generation of H2 is complex, particularly in an integrated system. In this project, the researchers focus on three specific research goals: the synthesis and characterization of new chromophores; the design and development of new catalysts containing common metal ions that are effective in photochemical systems for light-driven proton reduction in aqueous media; and the construction of new integrated proton reduction systems based on semiconductor materials such as SrTiO3, as structural scaffolds and on photocathode materials such as CuAlO2, to eliminate the need for chemical sources of electrons for proton reduction. Each of these areas are being explored with cutting-edge femtosecond time-resolved spectroscopy capable of probing dynamics involving initial light-driven events, longer duration transient absorption methods to follow later electron transfers and steady-state methods that can establish mechanisms of catalysis, molecular and interfacial structures, and long-term system stability. The scientists supported by this grant are also working with local elementary schools in Rochester and Buffalo, New York, to develop energy related science modules that can inspire the next generation of scientists.