He Xin, Larson Jonathan M, Bechtel Hans A, Kostecki Robert
Energy Storage and Distributed Resources Division, Lawrence Berkeley National Laboratory, Berkeley, CA, 94720, USA.
School of Chemical Engineering, Sichuan University, 610017, Chengdu, PR China.
Nat Commun. 2022 Mar 17;13(1):1398. doi: 10.1038/s41467-022-29103-z.
Solid-state batteries possess the potential to significantly impact energy storage industries by enabling diverse benefits, such as increased safety and energy density. However, challenges persist with physicochemical properties and processes at electrode/electrolyte interfaces. Thus, there is great need to characterize such interfaces in situ, and unveil scientific understanding that catalyzes engineering solutions. To address this, we conduct multiscale in situ microscopies (optical, atomic force, and infrared near-field) and Fourier transform infrared spectroscopies (near-field nanospectroscopy and attenuated total reflection) of intact and electrochemically operational graphene/solid polymer electrolyte interfaces. We find nanoscale structural and chemical heterogeneities intrinsic to the solid polymer electrolyte initiate a cascade of additional interfacial nanoscale heterogeneities during Li plating and stripping; including Li-ion conductivity, electrolyte decomposition, and interphase formation. Moreover, our methodology to nondestructively characterize buried interfaces and interphases in their native environment with nanoscale resolution is readily adaptable to a number of other electrochemical systems and battery chemistries.
固态电池具有通过实现多种益处（如提高安全性和能量密度）来对储能行业产生重大影响的潜力。然而，电极/电解质界面的物理化学性质和过程仍然存在挑战。因此，非常需要对这种界面进行原位表征，并揭示能够催化工程解决方案的科学认识。为了解决这个问题，我们对完整的和电化学运行的石墨烯/固体聚合物电解质界面进行了多尺度原位显微镜（光学、原子力和红外近场）和傅里叶变换红外光谱（近场纳米光谱和衰减全反射）研究。我们发现，固体聚合物电解质固有的纳米级结构和化学不均匀性在锂电镀和剥离过程中引发了一系列额外的界面纳米级不均匀性；包括锂离子传导率、电解质分解和界面相形成。此外，我们在纳米尺度分辨率下无损表征其原生环境中埋藏界面和界面相的方法很容易适用于许多其他电化学系统和电池化学体系。
