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

可以说，大规模非化石能源的开发是科学和工程学最重要的目标。拟议的项目将解决规模化利用太阳光的一个关键过程，即水的电催化氧化。电催化剂是一种使电驱动的化学反应进行得更快、更高效和/或用电量更少的材料。该项目将涉及发现新的催化材料，以有效地将水电化学氧化生成氢(H2)和氧(O2)。产生的二氢可直接用作燃料，在氢燃料电池中发电，或用作反应物，将低级含碳化合物升级为高价值燃料和化学品。该项目将解决将太阳能转换为化学能的可持续进程中的关键一步，从而减轻对化石资源的依赖。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询问的协同使用，这些细节和理解是不可能的。电催化过程用于利用绿色能源从水中生产氢气的规模化使用的主要挑战是开发能够催化快速和长寿命水氧化的坚固的阳极材料。拟议的研究重点是开发新的碳载体材料，以获得对电催化水氧化的基本了解，特别是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。通过涉及分子催化(Gunnoe，Machan)、纳米材料(Zhang)、理论和计算模拟(Goddard)、碳材料和催化剂表征(Heumann)以及标杆和机理研究(SPAN)包括原位EPR波谱(Schneg)的小组的协作努力，将实施一项战略，以开发和优化具有配体功能的分子催化剂，以加强电催化水氧化，将这些分子单元引入导电碳基材料，并研究其有效性和机理。为了实现这些目标，将追求三个目标：目标1.提高对覆盖芳烃配体的设计的理解，以优化用于基于钴或铁金属的水氧化的混合电催化剂的性能，包括多核过渡金属分子前体。目的2.发展吡啶-醇盐配体的设计原则，以优化复合电催化剂的性能，重点是生成多核过渡金属分子前驱体，用于铜和钴的OER。目的3.了解碳载体对催化剂活性中心活性和稳定性的影响。此外，该项目还将涉及主要面向本科生机构(PUI)的教育推广，以提高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NSF的法定使命，并通过使用基金会的智力优势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.