SusChEM: Insights into the Surface Chemistry of Water Oxidation on Pure and Modified Hematite Surfaces

SusChEM：深入了解纯赤铁矿和改性赤铁矿表面水氧化的表面化学

• 批准号: 1465082
• 负责人: Bruce Koel
• 金额: $ 49.82万
• 依托单位: Princeton University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2015
• 资助国家: 美国
• 起止时间: 2015-06-01 至 2018-05-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=1465082&HistoricalAwards=false
• 关键词: SusChEM; Insights; into; Surface; Chemistry

SusChEM: Insights into the Surface Chemistry of Water Oxidation on Pure and Modified Hematite SurfacesSolutions for supplying sustainable energy, in particular our demand for fuels, will likely require developments in photoelectrocatalysis that enable us to go beyond only electricity generation. Hematite (iron oxide)-based materials are promising for water oxidation using sunlight, a reaction that currently limits performance in photoelectrocatalytic devices for generating hydrogen from water splitting or hydrocarbon fuel from carbon dioxide reduction. Iron oxide is an attractive photoelectrode material because it absorbs 40% of the solar spectrum, and is cheap, abundant, nontoxic, and stable against corrosion. Iron oxide is also very inefficient for energy conversion. This can be addressed by modifying the surface with other materials to improve performance. This project aims to develop a fundamental understanding of the surface chemistry of water oxidation on pure and modified hematite surfaces, which aid the development of new materials and future solar-driven photocatalytic devices. The work involves graduate and undergraduate students and postdoctoral research associates learning and collaborating on cutting-edge approaches in chemistry, surface science, and nanotechnology for discovering new catalysts and advancing sustainable energy production. The research results are integrated into undergraduate and graduate courses and undergraduate and K-12 educational outreach programs. With this award, the Chemical Catalysis Program of the Chemistry Division funds Dr. Bruce Koel of Princeton University to study the fundamental surface chemistry and processes associated with water oxidation on hematite (alpha-Fe2O3)-based photoanodes. The efficiency of this reaction must be increased to enable several transformative solar fuel production technologies to be utilized for future sustainable energy production. Iron oxide is attractive because of its solar absorption spectrum and abundance, but it is very inefficient. One strategy is to improve reaction kinetics and overpotentials by surface modifications with co-catalysts or by doping. Dr. Koel and his group establish composition-activity relationships on well-defined pure and modified single crystal alpha-Fe2O3 electrodes, with heteroatoms localized at the surface and subsurface. They also experimentally identify and characterize surface-bound species in order to investigate key aspects of the water oxidation mechanism. Measurements include using in operando techniques in which the electrode surface is probed during oxidation rate measurements. Insights provided by this work benefit the rational design of nanostructured catalysts and their applications in energy conversion. This is a Sustainable Chemistry, Engineering & Materials (SusChEM) proposal.

SusChEM：对纯赤铁矿和改性赤铁矿表面上水氧化的表面化学的见解供应可持续能源的解决方案，特别是我们对燃料的需求，可能需要光电催化的发展，使我们能够超越发电。基于赤铁矿（氧化铁）的材料有希望用于使用阳光的水氧化，该反应目前限制了光电催化装置的性能，该光电催化装置用于从水分解产生氢气或从二氧化碳还原产生烃燃料。氧化铁是一种有吸引力的光电极材料，因为它吸收40%的太阳光谱，并且便宜，丰富，无毒，耐腐蚀。 氧化铁对于能量转换也非常低效。这可以通过用其他材料改性表面来解决，以提高性能。该项目旨在对纯净和改性赤铁矿表面的水氧化表面化学进行基本了解，这有助于开发新材料和未来太阳能驱动的光催化设备。这项工作涉及研究生和本科生以及博士后研究人员，他们在化学、表面科学和纳米技术领域的前沿方法上进行学习和合作，以发现新的催化剂并推进可持续能源生产。研究成果被整合到本科和研究生课程以及本科和K-12教育推广计划中。有了这个奖项，化学部的化学催化计划资助普林斯顿大学的布鲁斯科尔博士研究基本的表面化学和与赤铁矿（α-Fe 2 O3）为基础的光阳极水氧化过程。必须提高这一反应的效率，以使几种变革性的太阳能燃料生产技术能够用于未来的可持续能源生产。氧化铁由于其太阳能吸收光谱和丰度而具有吸引力，但它的效率非常低。一种策略是通过用助催化剂进行表面改性或通过掺杂来改善反应动力学和过电位。Koel博士和他的团队在定义明确的纯和改性单晶α-Fe 2 O3电极上建立了成分-活性关系，杂原子位于表面和次表面。 他们还通过实验识别和表征表面结合的物种，以研究水氧化机制的关键方面。测量包括在操作中使用技术，其中在氧化速率测量期间探测电极表面。本研究为纳米结构催化剂的合理设计及其在能源转化中的应用提供了有益的启示。 这是一个可持续化学，工程材料（SusChEM）的建议。