Kröger Till-Niklas, Wölke Mathis Jan, Harte Patrick, Beuse Thomas, Winter Martin, Nowak Sascha, Wiemers-Meyer Simon
MEET Battery Research Center, University of Münster, Corrensstraße 46, 48149, Münster, Germany.
Helmholtz-Institute Münster, IEK-12, FZ Jülich, Corrensstraße 46, 48149, Münster, Germany.
ChemSusChem. 2022 Nov 8;15(21):e202201169. doi: 10.1002/cssc.202201169. Epub 2022 Oct 1.
The electrochemical response of layered lithium transition metal oxides LiMO [M=Ni, Mn, Co; e. g., Li(Ni Mn Co )O (NMC532)] with single-crystalline architecture to slow and fast charging protocols and the implication of incomplete and heterogeneous redox reactions on the active material utilization during cycling were the subject of this work. The role of the active material size and the influence of the local microstructural and chemical ramifications in the composite electrode on the evolution of heterogeneous state of charge (SOC) distribution were deciphered. For this, classification-single-particle inductively coupled plasma optical emission spectroscopy (CL-SP-ICP-OES) was comprehensively supplemented by various post mortem analytical techniques. The presented results question the impact of surface-dependent failure mechanisms of single crystals for the evolution of SOC heterogeneity and identify the deficient structural flexibility of the composite electrode framework as the main driver for the observed non-uniform active material utilization.
具有单晶结构的层状锂过渡金属氧化物LiMO[M = Ni、Mn、Co;例如,Li(NiMnCo)O(NMC532)]对慢速和快速充电协议的电化学响应以及不完全和非均相氧化还原反应对循环过程中活性材料利用率的影响是本工作的主题。研究了解活性材料尺寸的作用以及复合电极中局部微观结构和化学分支对非均相电荷状态(SOC)分布演变的影响。为此,通过各种事后分析技术对分类单颗粒电感耦合等离子体发射光谱法(CL-SP-ICP-OES)进行了全面补充。所呈现的结果质疑了单晶表面依赖性失效机制对SOC非均质性演变的影响,并确定复合电极框架缺乏结构灵活性是观察到的活性材料利用不均匀的主要驱动因素。