Chemical Engineering Journal ( IF 13.3 ) Pub Date : 2020-09-15 , DOI: 10.1016/j.cej.2020.127031 Zhikun Zhao , Ziyue Wen , Xinghui Liu , Hao Yang , Shi Chen , Chunli Li , Haijian Lv , Feng Wu , Borong Wu , Daobin Mu
Poor interfacial contact and severe polarization of nickel-rich cathode materials are crucial problems that must be solved in the development of nickel-rich cathode/garnet-type electrolyte solid-state batteries. Herein, a binder-like Li3PO4 is introduced via an in-situ calcination process to build a compatible and Li+-conductive self-integrated layer of Li6.4La3Zr1.4Ta0.6O12-Li3PO4 on LiNi0.8Co0.1Mn0.1O2 cathode material, with a newly calculation method for estimating the interface compatibility theoretically. In addition, the routine helps weaken the space charge layer of active material commonly inevitable in the case, as demonstrated by calculation of Density Functional Theory and Atomic force microscopy analysis. With the interface engineering, the in-situ generated Li3PO4 tightly fix Li6.4La3Zr1.4Ta0.6O12 on LiNi0.8Co0.1Mn0.1O2, improving the compatibility between LiNi0.8Co0.1Mn0.1O2 cathode material and the solid electrolyte Li6.4La3Zr1.4Ta0.6O12. As a result, the interface-engineered LiNi0.8Co0.1Mn0.1O2/ Li6.4La3Zr1.4Ta0.6O12 solid state battery exhibits an initial discharge capacity of 188.8mAh/g at 0.2C (40 mA g-1). Even at 1C, its retention still remained 91.6% (initial value of 130mAh g-1) after 100 cycles. The SSBs could also work well under high temperature, delivering high initial discharge capacities of 153.4 mAh g-1 (55 ℃) and 149.6 mAh g-1 (80 ℃) at 1C, respectively. The work provides an effective strategy to improve NCM811-LP-LLZTO SSBs.
中文翻译:
调整与集成在正极材料上的LLZTO兼容的接口,以改善NCM811 / LLZTO固态电池
富镍正极材料的不良界面接触和严重极化是在开发富镍正极/石榴石型电解质固态电池中必须解决的关键问题。在此,通过原位煅烧工艺引入粘合剂状的Li 3 PO 4,以在LiNi上构建相容的且Li +导电的Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12 -Li 3 PO 4的Li +导电自结合层。0.8 Co 0.1 Mn 0.1 O 2阴极材料,采用一种新的计算方法从理论上估算界面相容性。此外,该程序有助于减弱通常情况下不可避免的活性材料的空间电荷层,如通过密度泛函理论的计算和原子力显微镜分析所证明的。通过界面工程,原位生成的Li 3 PO 4将Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12牢固地固定在LiNi 0.8 Co 0.1 Mn 0.1 O 2上,提高了LiNi 0.8 Co 0.1 Mn 0.1之间的相容性。O 2正极材料和固体电解质Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12。结果,界面工程LiNi 0.8 Co 0.1 Mn 0.1 O 2 / Li 6.4 La 3 Zr 1.4 Ta 0.6 O 12固态电池在0.2C(40 mA g -1)时的初始放电容量为188.8mAh / g。。即使在1C时,其保留率仍保持91.6%(初始值为130mAh g -1)100个周期后。这些SSB在高温下也能很好地工作,在1C时可提供153.4 mAh g -1(55℃)和149.6 mAh g -1(80℃)的高初始放电容量。这项工作为改进NCM811-LP-LLZTO SSB提供了有效的策略。