Advancing cation-disordered electrode materials for high performing and sustainable batteries

拟议的研究计划旨在加快发现用于高性价比和高能电池的储能材料，用于先进应用，包括电动汽车和大规模绿色储能。我们通过对所谓的阳离子无序电极材料的实验和理论研究来探讨这一点，这种材料在先进的锂/钠电池应用中受到了极大的关注，因为它们可以由廉价的元素组成，并且可以提供比传统正极材料高50%的单位重量能量。由3名博士生、2名硕士生、4名本科生和1名博士后组成的小组将进行三项建设性的相关研究：(I)第一个重点是通过对组成空间、原位材料表征和密度泛函理论(DFT)计算的系统探索，发现具有新的氧化还原机理的超高能阳离子无序材料。特别是，我们专注于发现锰/铁基化合物，因为锰和铁是高度丰富的过渡金属；因此，我们的材料可以解决当前锂离子技术利用昂贵/稀有的钴(Co)来储存能量的资源限制问题。(2)第二个重点是开发能够扩大阳离子无序材料生产的新的合成加工方法。虽然这种阳离子无序材料为先进电池带来了希望，但它们的合成加工方法一直不适合规模化生产，而且涉及到在化合物中引入缺陷的粉化过程。我们的目标是开发新的方法来解决这些问题，同时促进阳离子无序电池材料的商业使用。(3)通过实验(如电化学、X射线、电子显微镜)和密度泛函(DFT)模拟，分析阳离子无序材料的结构稳定性及其与功能电解液的相容性，以开发具有长循环寿命的先进锂电池(如锂金属/固态)。我们预计，我们的由极其廉价的金属(锰、铁)组成的新材料将通过将阴极侧的存储成本(美元/千瓦时)降低至少两倍来加速高性能和成本效益电池的发展。此外，对我们的新型材料的结构-加工-性能关系的研究将突出材料科学对储能材料发展的重要性，正如我们之前的成就(例如，发表在《自然》、《科学》上的文章)所表明的那样。因此，我们的项目将解决可持续和高性能电池开发中的关键问题，并将为培养学生/博士后提供肥沃的土壤。此外，将寻求国际合作，以最大限度地发挥该计划的成果，从而促进加拿大在绿色能源储存技术方面的领先地位。

The proposed research program aims to accelerate the discovery of energy-storage materials for cost-effective and high-energy batteries to be used in advanced applications, including electric vehicles and large-scale green energy storage. We approached this via experimental and theoretical studies of so-called cation-disordered electrode materials, which are receiving significant attention in advanced Li/Na-battery applications as they can be made of inexpensive elements and can deliver ~50% high energy per weight than traditional cathode materials. A group of 3 Ph.D. students, 2 Masters' students, 4 undergraduate trainees, and 1 postdoctoral fellow will conduct three constructively correlated pieces of research: (i) The first thrust focuses on the discovery of new ultrahigh-energy cation-disordered materials with novel redox mechanism through a systematic exploration of the compositional space, in situ material characterization, and density functional theory (DFT) calculations. In particular, we focus on discovering Mn/Fe-based compounds because Mn and Fe are highly abundant transition metals; thus, our materials can resolve the resource-constraint issue of current Li-ion technology utilizing expensive/rare cobalt (Co) to store energy. (ii) The second thrust focuses on developing new synthesis-processing methods amenable to scale-up production of the cation-disordered materials. While the cation-disordered materials hold promises for advanced batteries, their synthesis-processing methods have not been suitable for scaled-up production and involve a pulverization process which introduces defects in the compounds. We aim to develop novel methods that can address these issues while facilitating the commercial use of cation-disordered battery materials simultaneously. (iii) Finally, we will analyze the structural stability of the cation-disordered materials and their compatibility with functional electrolytes by using experiments (e.g., electrochemistry, X-ray tools, electron-microscopy) and DFT modeling, to develop advanced Li-batteries (e.g., Li-metal/solid-state) with long cycle life. We expect that our new materials consisting of dirt-cheap metals (Mn, Fe) will accelerate the development of high performing and cost-effective batteries by decreasing the cost-to-store energy ($/kWh) at the cathode side at least by a factor of two. Also, the investigation of the structure-processing-properties relationship of our novel materials will highlight the importance of materials science to the development of energy-storage materials, as our previous achievements (e.g., publications in Nature, Science) demonstrate. As such, our program will address critical issues in the development of sustainable and high performing batteries and will provide a fertile ground for training students/postdocs. Moreover, international collaboration will be sought to maximize the outcomes of this program, hence advancing Canada's leadership in green energy storage technology.