Orchestrating Electron and Proton Transfer for Solar Energy Conversion

协调电子和质子转移以实现太阳能转换

• 批准号: 1055547
• 负责人: Stefan Bernhard
• 金额: $ 41.5万
• 依托单位: Carnegie-Mellon University
• 依托单位国家: 美国
• 项目类别: Continuing Grant
• 财政年份: 2011
• 资助国家: 美国
• 起止时间: 2011-09-15 至 2014-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1055547&HistoricalAwards=false
• 关键词: Orchestrating; Electron; Proton; Transfer; Solar

In this project funded by the Chemical Catalysis Program of the Chemistry Division, Stefan Bernhard of Carnegie Mellon University will design, synthesize and study novel light-absorbing metal complexes combined with reduction catalysts able to generate hydrogen from water and sunlight. Coordination complexes of biologically innocuous and inexpensive first-row transition metal ions will be investigated for use as catalysts and chromophores. Strongly chelating hemi-cage and wrap-around ligand topologies that stabilize these normally labile structures will be explored. Advanced spectroscopic and electrochemical techniques will be used to understand the structure and function of these complexes and their application to water-splitting systems, and parallel photoreactors will be employed to study large numbers of candidate complexes and reaction conditions. Through a combination of these spectroscopic and synthetic methods, quantitative structure-activity relationships of photocatalytic systems will be determined. These insights will be used to further improve the robustness and reaction rate of hydrogen evolution. The solution-based chemistry of these water reduction catalysts will then be modified into scalable photoelectrochemical systems immobilized on transparent electrodes suitable for use in full water-splitting systems. The broader impacts involve training undergraduate and graduate students, hosting visiting high school teachers for summer research opportunities, teaching a course on the chemistry of chocolate, and the potential societal impact of renewable energy technology. This work will provide fundamental and applied knowledge about catalysts that generate hydrogen fuel from water and sunlight, and potentially could show how earth abundant metals can be used for such technologies. Results from this research would be important to the energy industry and to industries that manufacture commercial consumer products that require fuels sources, such as the automotive and aerospace sectors.

在这个由化学部化学催化计划资助的项目中，卡内基梅隆大学的Stefan Bernhard将设计，合成和研究新型吸光金属络合物与还原催化剂的结合，能够从水和阳光中产生氢气。生物无害和廉价的第一行过渡金属离子的配位络合物将被用作催化剂和发色团。 强螯合半笼和环绕配体拓扑结构，稳定这些通常不稳定的结构将被探讨。 先进的光谱和电化学技术将用于了解这些配合物的结构和功能及其在水裂解系统中的应用，并将采用并行光反应器来研究大量的候选配合物和反应条件。 通过这些光谱和合成方法的结合，将确定光催化体系的定量结构-活性关系。这些见解将用于进一步提高析氢的鲁棒性和反应速率。然后，这些水还原催化剂的基于溶液的化学将被改性成固定在透明电极上的可扩展的光电化学系统，适用于完全的水裂解系统。 更广泛的影响包括培训本科生和研究生，为暑期研究机会接待来访的高中教师，教授巧克力化学课程，以及可再生能源技术的潜在社会影响。这项工作将提供有关从水和阳光中产生氢燃料的催化剂的基础知识和应用知识，并可能展示如何将地球上丰富的金属用于此类技术。 这项研究的结果对能源行业和制造需要燃料来源的商业消费品的行业（如汽车和航空航天行业）非常重要。