Interfacing earth-abundant electrocatalysts with mesostructured oxide photoanodes for solar photoelectrocatalysis.

获得美国国家科学基金会化学部化学催化项目的奖金后，西雅图华盛顿大学的Daniel Gamelin教授将开展以化学燃料形式进行太阳能转换和储存领域的研究。具体来说，该项目旨在解决将非晶态水氧化电催化剂与晶体半导体光电极相连接以实现光电化学（PEC）太阳能转换的挑战。该研究将结合制备和分析技术，对一组复合催化剂/半导体光阳极的界面有更深入的了解。首席研究员（PI）将应用最先进的光电化学和光谱技术来分析这些光电极，并推进对表面形态、功能化和氧化还原催化之间微观关系的理解。PI和他的团队将寻求发展基本的结构/功能关系，以解决催化剂-半导体耦合，电子-空穴复合动力学，以及这些催化剂对光阳极电子结构的影响。本研究将解决这类水氧化催化剂的电催化和光电催化反应的机理差异，以及性能差异。这项工作将提高这些复合光阳极在PEC电池结构中的太阳能水分解效率，特别是在低过电位下，复合损失最严重，对能量转换效率有害。这项研究的重点是将非晶态电催化剂与介结构氧化物光阳极连接起来，用于能够分解水的太阳能光电化学装置，从而产生作为化学燃料的氢。该研究将促进人们对这种用于光电化学太阳能转换的复合光电极的普遍认识。这项研究将产生新的复杂材料和新的基础知识，对未来的替代能源技术产生广泛的影响。该项目还将提供无机化学、物理化学、电子化学和材料化学领域的高级跨学科培训，为参与的本科生、研究生和博士后研究人员未来在科学、工程和教育领域的职业做好准备。特别强调早期职业水平（本科，高中）的研究和教育的整合，通过本科生积极参与，将本研究的实验和概念纳入华盛顿大学本科课程，与本科院校的教师和学生合作，以及在西雅图地区的高中和社区学院开展成熟的推广活动。

With this award from the Chemical Catalysis Program of the Chemistry Division of the National Science Foundation, Professor Daniel Gamelin at the University of Washington, Seattle, will carry out studies in the area of solar energy conversion and storage in the form of chemical fuels. Specifically, this project seeks to address the challenge of interfacing non-crystalline water-oxidation electrocatalysts with crystalline semiconductor photoelectrodes for photolectrochemical (PEC) solar energy conversion. The research will use a combination of preparative and analytical techniques to develop a deeper understanding of interfaces in a set of composite catalyst/semiconductor photoanodes. The principal investigator (PI) will apply state-of-the-art photoelectrochemical and spectroscopic techniques to assay these photoelectrodes and to advance understanding of microscopic relationships between surface morphology, functionalization, and redox catalysis. The PI and his team will seek to develop fundamental structure/function relationships that address catalyst-semiconductor coupling, electron-hole recombination dynamics, and the impact such catalysts have on the photoanode electronic structure. The research will address mechanistic differences between electrocatalytic and photoelectrocatalytic responses of this family of water-oxidation catalysts, as well as performance differences. This work will improve the solar water splitting efficiencies of these composite photoanodes in PEC cell configurations, particularly at low overpotentials where recombination losses are most severe and detrimental to energy conversion efficiencies.This research will focus on interfacing non-crystalline Earth-abundant electrocatalysts with mesostructured oxide photoanodes for use in solar photoelectrochemical devices capable of splitting water that will generate hydrogen as a chemical fuel. This research will advance the general understanding of such composite photoelectrodes for photoelectrochemical solar energy conversion. The research will yield new complex materials and new fundamental knowledge that could broadly impact future alternative-energy technologies. This project will also provide advanced interdisciplinary training in the areas of inorganic, physical, electro-, and materials chemistries, in order to prepare participating undergraduates, graduate students, and postdoctoral researchers for future careers in science, engineering, and education. There is a special emphasis on integration of research and education at the early career levels (undergraduate, high school) through aggressive involvement of undergraduates, incorporation of experiments and concepts from this research into the University of Washington undergraduate curriculum, collaboration with faculty and students from undergraduate institutions, and mature outreach activities at Seattle-area high schools and community colleges.