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Coupled Experimental and Computational Investigation of Interfaces in Multicomponent Photoelectrodes for Solar Water Splitting

用于太阳能水分解的多组分光电极界面的耦合实验和计算研究

基本信息

批准号：
1764399
负责人：
Kyoung-Shin Choi
金额：
$ 54.09万
依托单位：
University of Wisconsin-Madison
依托单位国家：
美国
项目类别：
Standard Grant
财政年份：
2018
资助国家：
美国
起止时间：
2018-09-15 至 2021-08-31
项目状态：
已结题

来源：
https://www.nsf.gov/awardsearch/showAward?AWD_ID=1764399&HistoricalAwards=false
关键词：
Coupled Experimental Computational Investigation Interfaces

项目摘要

Solar water splitting provides a sustainable and environmentally benign route for the production of hydrogen gas for use as a clean fuel source. This is why low cost and efficient solar water splitting is one of the grand scientific challenges. One way to split water with sunlight is with a photoelectrochemical cell (PEC), but these devices are not yet efficient enough for practical use. This project examines methods of optimizing parts of the PEC: the catalyst and protection layers that are key components for efficient and sustainable solar water splitting. It also examines the semiconductor electrodes that harvest solar energy, then generate and transport the electrical charge used for hydrogen generation. The overall performance of a PEC is affected not only by the bulk properties of these individual parts, but also by the interfaces formed between them. However, the difficulty of studying the interfaces relevant to water splitting have stood in the way of their study. In this project, Dr. Kyoung-Shin Choi of the University of Wisconsin - Madison and Dr. Giulia Galli of the University of Chicago combine experimental and computational studies to understand and control interfacial properties of a representative PEC system - bismuth vanadate-based photoanodes and their interfaces with other metal oxides. This project makes it possible to devise general strategies to construct optimal interfaces between the different parts of a PEC to enhance solar water splitting. Dr. Choi and Dr. Galli are also setting up combined experimental-computational tutorials to teach researchers in the field how to best compare computational and experimental results. Finally, they are creating and maintaining a website that contains useful data on PECs that can be accessed and used by researchers worldwide.In a photoelectrochemical cell (PEC), in addition to semiconductor electrodes that harvest solar energy and generate/transport charge carriers, catalyst and protection layers are key components for efficient and sustainable solar water splitting. The overall performance of multicomponent photoelectrodes is affected not only by the bulk properties of the individual constituents but also by the interfaces formed between them. The characteristics of these interfaces can considerably affect the charge transport properties and recombination loss, thus determining the number of charge carriers reaching the electrode surface to participate in water splitting reactions. To date, systematic studies of the atomic and electronic structures of interfaces relevant to water splitting have been extremely rare, due to numerous experimental and computational challenges. In this project, Dr. Choi and Dr. Galli are establishing a general and fundamental understanding of the effect of interfacial atomic and electronic structures on photoelectrochemical properties by combining experimental and computational studies. In order to elucidate interface-photoelectrochemical property relationships, BiVO4-based photoanodes are used as a representative multicomponent photoelectrode system, and a series of semiconductor/oxygen evolution catalyst (OEC), semiconductor/protection layer, and protection layer/OEC interfaces are constructed and examined by using single crystal and polycrystal BiVO4 electrodes with systematically varied surface terminations. An atomic level understanding of interface-photoelectrochemical property relationships makes it possible to devise general strategies to construct optimal interfaces among photon absorbers, protective materials, and catalysts to enhance solar water splitting. The proposed work also provides the community with validated coupled experimental-computational strategies for studying complex, heterogeneous interfaces.This award reflects NSF's statutory mission and has been deemed worthy of support through evaluation using the Foundation's intellectual merit and broader impacts review criteria.

太阳能水分解为氢气的生产提供了一种可持续和环保的途径，作为一种清洁燃料来源。这就是为什么低成本和高效的太阳能水分解是一个重大的科学挑战。一种利用阳光分解水的方法是使用光电化学电池（PEC），但这些设备的效率还不足以实际应用。该项目研究了优化PEC部分的方法：催化剂和保护层，它们是高效和可持续的太阳能水分解的关键部件。它还研究了半导体电极，这种电极可以收集太阳能，然后产生并传输用于制氢的电荷。PEC的整体性能不仅受到这些单独部件的整体性能的影响，还受到它们之间形成的界面的影响。然而，研究与水分裂有关的界面的困难一直阻碍着他们的研究。在这个项目中，威斯康星大学麦迪逊分校的kyyoung - shin Choi博士和芝加哥大学的Giulia Galli博士结合实验和计算研究来理解和控制典型PEC系统的界面特性——钒酸铋基光阳极及其与其他金属氧化物的界面。这个项目使得设计一般策略来构建PEC不同部分之间的最佳接口以增强太阳能水分解成为可能。Choi博士和Galli博士还建立了实验-计算结合教程，教该领域的研究人员如何最好地比较计算和实验结果。最后，他们正在创建和维护一个网站，其中包含有关PECs的有用数据，可供全世界的研究人员访问和使用。在光电化学电池（PEC）中，除了半导体电极收集太阳能并产生/传输电荷载流子外，催化剂和保护层是高效和可持续的太阳能水分解的关键部件。多组分光电极的整体性能不仅受到单个组分的体积特性的影响，还受到它们之间形成的界面的影响。这些界面的特性可以显著影响电荷输运性质和复合损失，从而决定到达电极表面参与水分解反应的载流子数量。迄今为止，由于许多实验和计算方面的挑战，对与水分裂相关的界面的原子和电子结构的系统研究非常罕见。在这个项目中，Choi博士和Galli博士通过结合实验和计算研究，对界面原子和电子结构对光电化学性质的影响建立了一般和基本的理解。为了阐明界面-光电化学性质之间的关系，以BiVO4基光阳极为代表的多组分光电极体系，采用具有系统变化表面末端的单晶和多晶BiVO4电极，构建并检测了一系列半导体/析氧催化剂（OEC）、半导体/保护层和保护层/OEC界面。在原子水平上理解界面-光电化学性质关系，可以设计出在光子吸收剂、保护材料和催化剂之间构建最佳界面的一般策略，以增强太阳能水分解。所提出的工作还为研究复杂的异构界面提供了有效的耦合实验-计算策略。该奖项反映了美国国家科学基金会的法定使命，并通过使用基金会的知识价值和更广泛的影响审查标准进行评估，被认为值得支持。