Controlling oxygen electrocatalysis on model oxide surfaces using electrolyte design

析氧反应（OER）是自然界和技术中最基本的储能过程之一。OER的高过电位是氧电催化面临的重大挑战之一，并且显著改进是未来氢经济中可再生能源载体可持续生产的关键。几乎所有以前的活性和机理研究都集中在催化电极的组成和结构上，而本项目则集中在电解质的影响上，以确定结构-活性关系。预计氢键可以降低中间体和产物的相对形成能，这将导致反应的高过电位的降低。离子液体中氢键的强度可以系统地调节，从而使它们成为理想的模型电解质，以获得活性和产物产率的新描述符。将通过微分电化学质谱法（DEMS）检测具有限定量的水的模型电解质中的氧析出，同时使用通道电极测量过氧化物物质。所提出的方法是推广到其他不充分理解的多步反应的电催化表面，这提供了新的途径来了解电催化的机制和活性位点，以优化其活性。

The oxygen evolution reaction (OER) is one of the most fundamental processes for energy storage both in nature and technology. The high overpotential of the OER is one of the grand challenges faced in oxygen electrocatalysis and significant improvement is key for sustainable production of renewable energy carriers in a future hydrogen economy. Virtually all previous studies of activity and mechanism focused on the composition and structure of the catalytic electrode, while this project focuses on the influence of the electrolyte to identify structure-activity relationships. It is expected that hydrogen bonding can lower the relative formation energies of intermediates and products, which will lead to a reduction of the high overpotential of the reaction. The strength of hydrogen bonding in ionic liquids can be tuned systematically, thereby making them ideal model electrolytes to derive novel descriptors of activity and product yield. Oxygen evolution in model electrolytes with defined amounts of water will be detected by differential electrochemical mass spectroscopy (DEMS), while peroxide species will be simultaneously measured using a channel electrode. The proposed approach is generalizable to other insufficiently understood multi-step reactions on electrocatalytic surfaces, which offers new avenues to understand mechanisms and active sites of electrocatalysis for optimizing their activity.