Defining Critical Heterogeneity in Cathode Architectures for Li-ion Batteries with High Energy Density

定义高能量密度锂离子电池阴极结构的关键异质性

• 批准号: 2022723
• 负责人: Jordi Cabana
• 金额: $ 33.06万
• 依托单位: University of Illinois at Chicago
• 依托单位国家: 美国
• 项目类别: Standard Grant
• 财政年份: 2020
• 资助国家: 美国
• 起止时间: 2020-09-01 至 2024-08-31
• 项目状态: 已结题
• 来源: https://www.nsf.gov/awardsearch/showAward?AWD_ID=2022723&HistoricalAwards=false
• 关键词: Defining; Critical; Heterogeneity; Cathode; Architectures

Lithium-ion batteries are the premier choice for clean and efficient energy storage for portable devices and electric vehicles. However, their performance still falls short of the metrics required to drive a meaningful shift away from transportation based on fossil fuels. Specifically, the energy stored per unit of volume, or energy density, is too low. Challenges in increasing energy density stem from the concurrent increase in the rate of failure and loss of power. This trade-off is driven by limitations at the cathode, but its microscopic chemical structure and mechanisms must be precisely defined for effective solutions to arise. Through a suite of existing and emerging techniques based on X-ray mapping, researchers at the University of Illinois at Chicago seek to reveal how chemical variations, called heterogeneity, at the nano and microscale determine the ability of modern lithium-ion cathodes to achieve long lifetimes in batteries with high energy density. This research will advance electrochemical engineering and battery manufacturing by establishing novel engineering principles informed by spatially precise chemical knowledge, which will subsequently guide new breakthroughs. To maximize and expedite impact in current technology, this research focuses on fundamental questions, yet applied to cathode materials of interest to industry. The activities are intertwined with the training of future generations of scientists through internships for undergraduate and high school students, promotion of science in local elementary schools and a Summer workshop on electrochemistry. These activities will have a special focus on members of Chicago's Hispanic communities, which are traditionally underrepresented in STEM.Limitations in the energy density of Li-ion batteries stem from the cathode, mainly because layered oxides, the leading family of candidates, do not currently perform at their theoretical limit. This limitation is fundamentally underpinned by the underlying electrochemical reactions that generate flow of electrical charge, which are hindered by incomplete reversibility and competing processes that degrade activity. The objective of this research is to correlate macroscopic battery performance to local chemical composition and progress of the storage reactions in the complex architectures pursued today. Conventionally, these correlations are established at the ensemble averages of the bulk electrode and at the level of very few isolated particles. But these scales are mismatched to the current push to design multifunctional heterostructures to enhance cathode performance, where it is critical to ascertain the nanoscale distribution of different elements and its consistency both within and between many particles. They are also mismatched to pinpoint the microscopic origin of the failure of competitive cathodes at extreme rates and extensive cycling, which critically depends on the specific microscale activity relative to the complete architecture. This research will quantify critical heterogeneity at relevant length scales with a suite of techniques of X-ray imaging and mapping, including in 3D and during battery operation. Novel analytical methods of broad applicability in battery research will be part of the legacy of this project. The novel insight will provide actionable engineering inputs to overcome enduring cathode roadblocks toward transformational energy density in next-generation Li-ion batteries.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.

锂离子电池是便携式设备和电动汽车清洁高效储能的首选。然而，它们的表现仍然福尔斯达不到推动从基于化石燃料的交通运输进行有意义的转变所需的指标。具体地说，每单位体积储存的能量或能量密度太低。提高能量密度的挑战来自于故障率和功率损失率的同时增加。这种权衡是由阴极的限制所驱动的，但其微观化学结构和机制必须精确定义才能产生有效的解决方案。通过一套基于X射线成像的现有和新兴技术，伊利诺伊大学芝加哥分校的研究人员试图揭示纳米和微米尺度的化学变化（称为异质性）如何决定现代锂离子阴极在高能量密度电池中实现长寿命的能力。这项研究将通过建立由空间精确的化学知识提供信息的新工程原理来推进电化学工程和电池制造，随后将指导新的突破。为了最大限度地提高和加快当前技术的影响，这项研究侧重于基本问题，但适用于工业感兴趣的阴极材料。这些活动与通过本科生和高中生实习培训未来几代科学家、在当地小学促进科学和电化学夏季讲习班交织在一起。这些活动将特别关注芝加哥的西班牙裔社区的成员，这些社区在STEM中传统上代表性不足。锂离子电池能量密度的限制来自阴极，主要是因为层状氧化物，候选人的主要家族，目前没有达到理论极限。这种限制从根本上得到了产生电荷流动的潜在电化学反应的支持，而电荷流动受到不完全可逆性和降低活性的竞争过程的阻碍。这项研究的目的是将宏观电池性能与当今追求的复杂架构中的局部化学成分和存储反应的进展相关联。传统上，这些相关性建立在整体平均的散装电极和在非常少的孤立粒子的水平。但这些尺度与当前设计多功能异质结构以增强阴极性能的推动力不匹配，其中确定不同元素的纳米级分布及其在许多颗粒内和颗粒之间的一致性至关重要。它们也不匹配，以查明竞争性阴极在极端速率和广泛循环下失败的微观起源，这严重依赖于相对于完整架构的特定微观活动。这项研究将量化关键异质性在相关的长度尺度与一套技术的X射线成像和映射，包括在3D和电池运行期间。在电池研究中具有广泛适用性的新型分析方法将成为该项目遗产的一部分。这一新颖的见解将提供可操作的工程投入，以克服下一代锂离子电池能量密度转型的持久阴极障碍。该奖项反映了NSF的法定使命，并通过使用基金会的知识价值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

3D Quantification of Elemental Gradients within Heterostructured Particles of Battery Cathodes

• DOI: 10.1021/acsenergylett.2c02619
• 发表时间: 2023-02
• 期刊: ACS Energy Letters
• 影响因子: 22
• 作者: E. Allen;Young-Seop Shin;William Judge;M. Wolfman;V. De Andrade;S. Cologna;J. Cabana

Spatial Quantification of Microstructural Degradation during Fast Charge in 18650 Lithium-Ion Batteries through Operando X-ray Microtomography and Euclidean Distance Mapping

通过操作 X 射线显微断层扫描和欧几里德距离测绘对 18650 锂离子电池快速充电期间微观结构退化进行空间量化

• DOI: 10.1021/acsaem.2c02397
• 发表时间: 2022
• 期刊: ACS Applied Energy Materials
• 影响因子: 6.4
• 作者: Allen, Eva;Lim, Linda Y.;Xiao, Xianghui;Liu, Albert;Toney, Michael F.;Cabana, Jordi;Nelson Weker, Johanna
• 通讯作者: Nelson Weker, Johanna

sxdm—A python framework for analysis of Scanning X-Ray Diffraction Microscopy data

sxdm——用于分析扫描 X 射线衍射显微镜数据的 Python 框架

• DOI: 10.1016/j.simpa.2021.100172
• 发表时间: 2021
• 期刊: Software Impacts
• 作者: Judge, William;Plews, Michael;May, Brian;Holt, Martin V.;Cabana, Jordi
• 通讯作者: Cabana, Jordi