Engineering principles for sustainable organic electrode materials

可持续有机电极材料的工程原理

• 批准号: 2124604
• 负责人: Shiyu Zhang
• 金额: $ 43.73万
• 依托单位: Ohio State University
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2021
• 资助国家: 美国
• 起止时间: 2021-09-01 至 2024-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2124604&HistoricalAwards=false
• 关键词: Engineering; principles; sustainable; organic; electrode

Lithium-ion batteries have become one of the leading electrochemical energy storage systems driving the progress of modern electronic technologies. However, the production of conventional lithium-ion batteries relies on finite and unsustainably sourced transition metals, such as lithium and cobalt, which will inevitably restrict their application in the long term. In this research project, the investigators seek to develop new organic electrode materials as alternative energy storage media in batteries. These new battery materials are made of abundant elements, such as carbon, nitrogen, oxygen, and sulfur, and can provide a more economical and sustainable route to renewable energy storage. These research activities are integrated with the training of graduate and undergraduate students in addressing scientific challenges at the interface of electrochemistry, synthetic chemistry, and machine learning. The educational aims include developing a laboratory exercise for an undergraduate general chemistry course that will introduce students to connections between electrochemistry and environmental water quality testing and a mentoring program for these students which connects them with peer tutors. Organic electrode materials (OEM) are promising alternatives to unsustainably sourced transition metals as energy storage media in lithium-ion batteries. Current OEMs (primarily redox organic polymers), however, suffer from (a) poor conductivity (30% carbon loading required), (b) poor cycling stability (ca. 100 cycles), and (c) sloping/multiple-stage voltage profiles. The overall goal of the research project is to discover, elucidate, and apply engineering principles to improve the rechargeability of OEMs. First, a wide array of novel small-molecule OEMs featuring strong intermolecular interactions are prepared. In-situ and ex-situ spectroscopic studies are performed to understand how the intermolecular interactions between charge storage units change as a function of state-of-charge. These tasks will explore the hypotheses that complementary hydrogen bonding and pi-pi stacking improve the stability of quinone-fused aza-phenazine OEM materials. It is predicted that additional intermolecular disulfide bonds between sulfur-rich thiazyl charge storage units can improve conductivity and facilitate high-rate cycling of OEMs. These results and new fundamental understanding will be used to develop new design principles for optimizing the conductivity, stability, voltage profile of OEMs through modification of molecular structure. In the second part of the proposal, the research project seeks to develop machine learning-based models that can (a) predict the long-term cycling life of OEMs using data collected from short-term high-throughput tests and (b) recommend new highly stable OEMs based on physical organic descriptors. This systematic study will ultimately reveal unintuitive design principles that enable more focused research efforts in place of extensive trial-and-error screening.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.

锂离子电池已成为推动现代电子技术进步的主要电化学储能系统之一。然而，传统锂离子电池的生产依赖于有限且不可持续的过渡金属，如锂和钴，这将不可避免地限制其长期应用。在这项研究项目中，研究人员试图开发新的有机电极材料作为电池的替代储能介质。这些新的电池材料含有丰富的元素，如碳、氮、氧和硫，可以提供一种更经济、更可持续的可再生能源储存途径。这些研究活动与研究生和本科生在解决电化学、合成化学和机器学习之间的科学挑战的培训相结合。教育目标包括为本科普通化学课程开发一个实验室练习，向学生介绍电化学和环境水质测试之间的联系，以及为这些学生制定一个指导计划，将他们与同行导师联系起来。有机电极材料(OEM)是锂离子电池中替代不可持续来源的过渡金属作为储能介质的很有前途的材料。然而，目前的原始设备制造商(主要是氧化还原有机聚合物)存在以下问题：(A)导电性差(需要30%的碳负载)，(B)循环稳定性差(约100次)，以及(C)倾斜/多级电压分布。该研究项目的总体目标是发现、阐明并应用工程原理来提高原始设备制造商的充值能力。首先，制备了一系列具有强分子间相互作用的新型小分子OEM。进行了原位和非原位光谱研究，以了解电荷存储单元之间的分子间相互作用是如何随着电荷状态的变化而变化的。这些任务将探索互补氢键和pi-pi堆积提高苯二酚-氮杂吩嗪OEM材料稳定性的假设。据预测，富硫的噻唑基电荷存储单元之间额外的分子间二硫键可以提高OEM的导电性，促进OEM的高速循环。这些结果和新的基本认识将被用来开发新的设计原则，通过改变分子结构来优化OEM的导电性、稳定性和电压分布。在提案的第二部分，研究项目寻求开发基于机器学习的模型，该模型可以(A)使用从短期高通量测试收集的数据来预测原始设备制造商的长期循环寿命，以及(B)基于物理有机描述符推荐新的高度稳定的原始设备制造商。这项系统的研究最终将揭示不直观的设计原则，使研究工作更有针对性，而不是广泛的试错筛选。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。

项目成果

Gaseous Nitrogen Oxides Catholyte for Rechargeable Redox Flow Batteries

用于可充电氧化还原液流电池的气态氮氧化物阴极电解液

• DOI: 10.1002/anie.202216889
• 发表时间: 2023
• 期刊: Angewandte Chemie International Edition
• 作者: Zhang, Weiyao;Yang, Xin;Zhang, Shiyu
• 通讯作者: Zhang, Shiyu