Collaborative Research: New Anodic Catalysts for Water Oxygen Evolution Using Hybrid Solid-State Materials

大规模开发非化石能源可以说是科学和工程最重要的目标。拟议中的项目将解决大规模利用阳光的一个关键过程，即水的电催化氧化。电催化剂是一种材料，它可以使电驱动的化学反应进行得更快，更有效，和/或更少的电力输入。该项目将涉及发现新的催化材料，用于有效的电化学氧化水以产生氢（H2）和氧（O2）。所产生的二氢可以直接用作氢燃料电池发电的燃料，也可以作为将低品位含碳化合物升级为高价值燃料和化学品的反应物。该项目将处理将太阳能转化为化学能的可持续进程中的一个关键步骤，从而减轻对矿物资源的依赖。这项工作的一个关键方面是阐明催化剂性能的细节和理解，如果没有实验和计算的协同使用，这是不可能的。大规模使用电催化过程以利用绿色能源从水中生产氢的主要挑战是开发强大的阳极材料，催化快速和长寿命的水氧化。该研究的重点是开发新的碳支撑材料，以获得对电催化水氧化的基本理解，特别是关注将明确定义的分子催化剂结构整合到导电固体材料中的能力。通过分子催化（Gunnoe, Machan），纳米材料（Zhang），理论和计算建模（Goddard），碳材料和催化剂表征（Heumann），基准和机制研究（Spanos），包括原位EPR光谱（Schnegg），开发和优化具有配体功能的分子催化剂以增强电催化水氧化的策略的合作努力，将这些分子单元整合到导电碳基材料中，并对其效能和机理进行研究。为实现这些目标，将追求三个目标：增加了对盖环芳烃配体设计的理解，以优化杂化电催化剂的性能，包括多核过渡金属分子前体，用于Co或Fe金属的水氧化。目标2。开发吡啶烷氧配体的设计原则，以优化杂化电催化剂的性能，重点是为基于Cu和Co的OER生成多核过渡金属分子前体。了解碳载体对催化剂活性位点活性和稳定性的影响。此外，该项目还将涉及向主要本科院校（PUIs）进行教育推广，以增加来自不同背景的学生对科学家和工程师职业的兴趣。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。

The development of large-scale non-fossil sources of energy is arguably science and engineering's most important goal. The proposed project will address a key process for scaled use of sunlight, the electrocatalytic oxidation of water. Electrocatalysts are materials that make electrically-driven chemical reactions proceed faster, more efficiently, and/or with less input of electricity. This project will involve discovery of new catalytic materials for efficient electrochemical oxidation of water to produce hydrogen (H2) and oxygen (O2). The produced dihydrogen can be used directly as a fuel to produce electricity in hydrogen fuel cells or as a reactant to upgrade low-grade carbon-containing compounds to high-value fuels and chemicals. The project will address a critical step in a sustainable process for converting solar energy to chemical energy, thus alleviating dependence on fossil resources. A key aspect of this effort is to elucidate details and understanding of catalyst performance that would not be possible without the synergistic use of both experimental and computational interrogation.A major challenge for the scaled use of electrocatalytic processes for the use of green energy to produce hydrogen from water is the development of robust anodic materials that catalyze rapid and long-lived water oxidation. The proposed research is focused on the development of new carbon-supported materials to gain fundamental understanding of electrocatalytic water oxidation, especially with a focus on the ability to integrate well-defined molecular catalyst structures into conducting solid materials. Through a collaborative effort that involves groups in molecular catalysis (Gunnoe, Machan), nanomaterials (Zhang), theory and computational modeling (Goddard), carbon materials and catalyst characterization (Heumann), and benchmarking and mechanistic studies (Spanos) including in situ EPR spectroscopy (Schnegg), a strategy to develop and optimize molecular catalysts with ligand functionality to enhance electrocatalytic water oxidation, incorporate these molecular units into conducting carbon-based materials, and to study their efficacy and mechanism will be implemented. To achieve these goals, three objectives will be pursued: Objective 1. Increased understanding of the design of capping arene ligands to optimize performance of hybrid electrocatalysts, including multi-nuclear transition metal molecular precursors, for water oxidation based on Co or Fe metals. Objective 2. Develop design principles for pyridine-alkoxide ligands to optimize performance of hybrid electrocatalysts, with a focus on generating multi-nuclear transition metal molecular precursors, for the OER based on Cu and Co. Objective 3. Understand the impact of the carbon support on the activity and stability of the catalyst active site. Also, the project will also involve educational outreach to primarily undergraduate institutions (PUIs) to increase interest among students from diverse backgrounds in careers as scientists and engineers.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.