NSF-BSF: Physical-Chemical Stabilization of Electrodeposition through Fundamental Interfacial Studies

电化学存储系统(电池)无处不在，从商业电子产品到电动汽车无所不在。在电池中，物理化学过程在界面上驱动复杂的耦合现象，如电沉积。电沉积是指在电场作用下，金属离子(溶解在电解液中)沉积到导电表面(电极)上的过程。不稳定(即不均匀)电沉积在电池的电极上会导致性能下降和失效。这是限制下一代电池的主要挑战之一，下一代电池具有更远距离电动汽车和电网规模可再生能源储存的潜力。在这个项目中，研究人员将使用一种综合的计算-实验方法来研究电沉积过程中界面区域物理-化学过程的复杂耦合，从而导致不稳定的沉积。然后，研究小组将利用这些知识来确定电沉积的物理化学稳定(或不稳定)区域。这项研究将为设计出寿命更长、容量更高的更稳定的电池奠定基础。该项目是美国和以色列研究人员之间的合作，将为学生提供机会，不仅学习最先进的研究，而且还可以互动和了解不同的文化。该项目将在美国波士顿大学和以色列耶路撒冷希伯来大学培训研究生，并将通过在这两个国家的外联活动吸引K-12学生。不稳定的电沉积是由不均匀传输、反应性、压力等异质性造成的，并导致性能损失和失败。虽然理想情况下开发同质材料/界面/系统可以解决这些问题，但不可能制造出完美的系统。在这个项目中，研究人员将使用一种综合的计算-实验方法来研究电沉积过程中界面区域物理-化学过程的复杂耦合，从而导致不稳定的沉积。然后，研究小组将利用这些知识来确定电沉积的物理化学稳定(或不稳定)区域。利用计算和实验模型系统，我们将研究物理和化学性质对几种金属体系(如银、铜、锌等)电沉积的影响。目的是全面了解稳定电沉积的驱动力，这将导致绘制电沉积稳定和不稳定制度的地图。这个项目将检验这样一个假设，即电极表面的电沉积位置和速度可以通过调节材料系统的物理化学性质来控制。为了实现研究目标，界面区域的介观计算模型将与电沉积的受控实验研究相结合。电极界面的受控实验研究将为模型的参数化和验证提供数据；而计算模型将指导实验研究，并进一步深入了解导致观察到的实验行为的基本物理现象。通过将实验和计算研究相结合，该项目将对驱动不稳定或稳定电沉积的物理化学过程有一个基本的了解，包括界面传输、表面特征，如工程表面粗糙度，通过掺杂剂改变表面反应性，以及结构化界面。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。

Electrochemical storage systems (batteries) are ubiquitous, found in everything from commercial electronics to electric vehicles. In batteries, physical-chemical processes drive complex, coupled phenomena at the interfaces, such as electrodeposition. Electrodeposition is the deposition of metallic ions (dissolved in an electrolyte) onto an electrically conductive surface (the electrode) in the presence of an electric field. Unstable (i.e. non-uniform) electrodeposition on the electrodes of batteries leads to performance degradation and failure. This is one of the main challenges limiting next generation batteries, which hold potential for longer range electric vehicle and grid scale energy storage for renewable energy. In this project, the investigators will use an integrated computational-experimental approach to study the complex coupling of physical-chemical processes in the interface region during electrodeposition that lead to unstable deposition. The team will then use that knowledge to define regions of physical-chemical stabilization (or destabilization) of electrodeposition. This research will lay the foundation for engineering more stable batteries with longer lifetimes and higher capacities. This project is a collaboration between researchers in the United States and Israel and will provide opportunities for students to not only learn about state-of-the-art research but also to interact with and learn about different cultures. The project will train graduate students in both the United States at Boston University and in Israel at The Hebrew University of Jerusalem, and will engage k-12 students through outreach activities in both countries.Unstable electrodeposition is caused by heterogeneities, including non-uniform transport, reactivity, stresses, etc., and leads to performance loss and failure. While ideally development of homogeneous materials/interfaces/systems would solve these issues, it is impossible to fabricate perfect systems. In this project, the investigators will use an integrated computational-experimental approach to study the complex coupling of physical-chemical processes in the interface region during electrodeposition that lead to unstable deposition. The team will then use that knowledge to define regions of physical-chemical stabilization (or destabilization) of electrodeposition. Using computational and experimental model systems we will investigate the effects of both physical and chemical properties on electrodeposition for several metal systems (i.e. silver, copper, zinc, etc.) with the goal of developing a holistic understanding of the driving forces for stable electrodeposition that will lead to the mapping of electrodeposition stabilization and destabilization regimes. This project will test the hypothesis that the location and rate of electrodeposition on the electrode surface can be controlled by tuning the physical-chemical properties of the material system. To accomplish the research objectives a meso-scale computational model of the interfacial region will be coupled with controlled experimental investigations of electrodeposition. Controlled experimental studies of the electrode interface will provide data for parameterization, and validation of the model; while the computational models will guide experimental studies and provide further insight into the fundamental physical phenomena that lead to observed experimental behavior. By integrating the experimental and computational research, the project will develop a fundamental understanding of the physical-chemical processes that drive unstable or stable electrodeposition including interfacial transport, surface features, such as engineered surface roughness, changing surface reactivity through dopants, and structured interfaces.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.