Molecular Strategies for Converting and Storing Solar Energy

Berlinguette项目的首要目标是开发方法，提高阳光转化为电能的效率，进而转化为化学燃料。该提案的一个主要组成部分是设计和合成用于染料敏化太阳能电池（DSSC）的金属发色团和电解质。Berlinguette团队在DSSC应用的环金属化钌发色团的开发中发挥了主导作用，该提案将继续开发这类染料。本提案还将描述在基本水平上更好地理解DSSC内特定过程的策略，并更好地理解这些钌配合物的激发态动力学。Berlinguette团队还将通过精心设计和研究溶液中的分子水氧化催化剂以及附着在表面上的水氧化催化剂，探索有效地从水中提取氢的方法。这方面的建议将询问单位点均相（光）催化剂的反应性，特别强调研究质子耦合电子转移化学。本提案中概述的研究将为本科生和研究生提供无机合成，物理和计算方法（例如，核磁共振光谱，x射线衍射技术，电化学，紫外-可见和荧光光谱，随时间变化的密度泛函理论）方面的广泛培训。参与太阳能电池项目的学生还将学习如何制造和表征（例如，IV图，阻抗谱）先进的太阳能电池。

The overarching goal of the Berlinguette program is to develop methods to improve the conversion efficiency of sunlight into electricity and, in turn, into chemical fuels. A major component of this proposal is the design and synthesis of metal chromophores and electrolytes for applications in the dye-sensitized solar cell (DSSC). The Berlinguette group has played a leading role in the development of cyclometalated ruthenium chromophores for DSSC applications, and this proposal will continue the development of this class of dyestuff. This proposal will also describe strategies to better understand specific processes within the DSSC at a fundamental level, and to better understand the excited-state dynamics of these ruthenium complexes. The Berlinguette group will also explore methods to efficiently extract hydrogen from water through the careful design and study of molecular water oxidation catalysts in solution and tethered to surfaces. This aspect of the proposal will interrogate the reactivities of single-site homogeneous (photo)catalysts, with a particular emphasis on studying proton-coupled electron transfer chemistry. The studies outlined in this proposal will give undergraduate and graduate students extensive training in inorganic synthesis, and physical and computational methods (e.g, NMR spectroscopy, X-ray diffraction techniques, electrochemistry, UV-vis and fluorescence spectroscopy, time-dependent density functional theory). Students involved in the solar cell project will also learn how to fabricate and characterize (e.g., IV plots, impedance spectroscopy) advanced solar cells.