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

拟议的研究计划旨在加速发现用于先进应用的高性价比和高能量电池的储能材料，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，这些材料在先进的Li/Na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制成，并且可以比传统的阴极材料提供约50%的高能量。一组3位博士本项目将由三名硕士生、四名本科生和一名博士后共同完成三项建设性的相关研究：（i）第一项研究重点是通过系统的组分空间探索、原位材料表征和密度泛函理论（DFT）计算，发现具有新型氧化还原机制的新型超高能阳离子无序材料。特别是，我们专注于发现Mn/Fe基化合物，因为Mn和Fe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/稀有钴（Co）储存能量的资源限制问题。(ii)第二个重点是开发新的合成加工方法，适合大规模生产的阳离子无序材料。虽然阳离子无序材料有望用于先进的电池，但它们的合成加工方法不适合大规模生产，并且涉及在化合物中引入缺陷的粉碎过程。我们的目标是开发新的方法，可以解决这些问题，同时促进阳离子无序电池材料的商业使用。(iii)最后，我们将通过实验分析阳离子无序材料的结构稳定性及其与功能电解质的相容性（例如，电化学，X射线工具，电子显微镜）和DFT建模，以开发先进的锂电池（例如，锂金属/固态），循环寿命长。我们预计，我们由非常便宜的金属（Mn，Fe）组成的新材料将通过将阴极侧的储能成本（$/kWh）降低至少两倍来加速高性能和成本效益电池的开发。此外，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，因为我们以前的成就（例如，发表在《自然》、《科学》上）。因此，我们的计划将解决可持续和高性能电池发展中的关键问题，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，以最大限度地提高该计划的成果，从而推动加拿大在绿色能源储存技术方面的领导地位。

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.