DMREF: Collaborative Research: A Blueprint for Photocatalytic Water Splitting: Mapping Multidimensional Compositional Space to Simultaneously Optimize Thermodynamics and Kinetics

DMREF：协作研究：光催化水分解的蓝图：映射多维组成空间以同时优化热力学和动力学

• 批准号: 1627583
• 负责人: Louis Piper
• 金额: $ 25.51万
• 依托单位: SUNY at Binghamton
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2016
• 资助国家: 美国
• 起止时间: 2016-10-01 至 2021-09-30
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1627583&HistoricalAwards=false
• 关键词: DMREF; Collaborative; Research; Blueprint; Photocatalytic

NON-TECHNICAL DESCRIPTION: Sunlight is a vast source of renewable energy but its intermittent nature means that its utilization requires a means of storing this energy. One attractive approach for solar energy storage is to harness the energy of sunlight to split water into hydrogen and oxygen i.e. solar generated fuels. The solar generated fuels can be combusted to release energy efficiently with water as the only by-product. As a result, this approach avoids the deleterious consequences of greenhouse emissions that accompany the combustion of conventional fossil fuels. The complex cascade of reactions required to harvest sunlight and split water into hydrogen and oxygen present a formidable scientific challenge. The project seeks to develop hybrid materials as the catalyst for water splitting, such that individual components are assembled and function synergistically. The project further works towards employing components that are highly tunable in terms of their energy levels, thereby providing a versatile platform that can be optimized for converting sunlight and water into fuel. Employing a judicious mix of calculations from supercomputers and selective experiments accelerates the rationally design of materials for efficient solar energy storage within chemical bonds. The project team mentors young scientists from underrepresented groups and engages K-12 students and teachers in activities that emphasize the opportunities made available by big data and solar energy.TECHNICAL DESCRIPTION: The project explores the design of programmable heterostructured platforms for photocatalytic water splitting based on interfacing ternary vanadium oxide bronzes with semiconductor quantum dots. In the former compounds, metal cations are intercalated within a variety of open vanadium oxide frameworks, enabling a multitude of compositional possibilities and considerable energy level tuning. Moreover, the energy levels of quantum dots can also be tuned as a function of composition as well as size and the presence of cores. Photocatalytic water splitting requires not just the appropriate alignment of energy levels but also precise control of charge transfer dynamics. Interfacing two versatile and tunable components yields a rich multidimensional space for identification of effective photocatalytic architectures for water oxidation that yield holes at potentials only minimally positive to the water oxidation potential, thereby allowing for efficient conversion of sunlight to solar fuels. The multidimensional parameter space is mapped through a closely integrated and iterative combination of first-principles structure prediction, electronic structure calculations, diversified materials synthesis, detailed spectroscopy, high-throughput screening, and big data analytics. The activity involves development of an open-source platform for statistical analysis and mining of spectroscopic data. A summer research activity engages undergraduates from diverse backgrounds.

非技术描述：阳光是可再生能源的广泛来源，但其间歇性的性质意味着其利用需要一种存储这种能量的方法。太阳能存储的一种有吸引力的方法是利用阳光的能量将水分成氢和氧气，即太阳能产生的燃料。可以将太阳能产生的燃料燃烧以用水为唯一的副产品有效释放能量。结果，这种方法避免了伴随常规化石燃料燃烧的温室排放的有害后果。收获阳光并将水分成氢和氧所需的复杂反应级联反应带来了巨大的科学挑战。该项目旨在开发混合材料作为水分割的催化剂，以使各个组件组装并协同起作用。该项目进一步致力于采用高度可调的能源水平的组件，从而提供了一个多功能平台，可以优化，以将阳光和水转换为燃料。 采用超级计算机和选择性实验的精确计算组合，加速了材料的理性设计，以在化学键内有效的太阳能存储。项目团队指导来自代表性不足的小组的年轻科学家，并与K-12学生和老师参与活动，这些活动强调了大数据和太阳能提供的机会。技术描述：该项目探索了基于光催化水的可编程异质结构平台的设计与半导体量子点的氧化三元式氧化钒的接口。在前一种化合物中，金属阳离子在各种开放的氧化钒框架中被插入，从而实现了多种组成的可能性和相当大的能级调整。此外，量子点的能级也可以根据组成以及大小和核心的存在来调整。光催化水分不仅需要适当的能量水平对齐，而且还需要对电荷转移动态的精确控制。连接两个多功能和可调的组件产生了丰富的多维空间，用于识别有效的光催化体系结构，用于水氧化，这些空间仅在电势处产生的孔仅对水氧化潜力，从而使阳光有效地转化太阳能燃料。多维参数空间通过第一原理结构预测，电子结构计算，多样化的材料合成，详细光谱，高通量筛选和大数据分析的紧密整合且迭代的组合映射。该活动涉及开发开源平台，用于统计分析和挖掘光谱数据。一项夏季研究活动吸引了不同背景的本科生。

项目成果

Structural water and disordered structure promote aqueous sodium-ion energy storage in sodium-birnessite

• DOI: 10.1038/s41467-019-12939-3
• 发表时间: 2019-10
• 期刊: Nature Communications
• 影响因子: 16.6
• 作者: Xiaoqian Shan;Fenghua Guo;Daniel S. Charles;Zachary W. Lebens-Higgins;Sara Abdel Razek;Jinpeng Wu;Wenqian Xu;Wanli Yang;K. Page;J. Neuefeind;M. Feygenson;L. Piper;Xiaowei Teng

Designing catalysts for water splitting based on electronic structure considerations

• DOI: 10.1088/2516-1075/ab7d86
• 发表时间: 2020-06-01
• 期刊: ELECTRONIC STRUCTURE
• 影响因子: 2.6
• 作者: Razek, Sara Abdel;Popeil, Melissa R.;Piper, Louis F. J.
• 通讯作者: Piper, Louis F. J.