Kopuklu Buse Bulut, Esen Ekin, Gomez-Martin Aurora, Winter Martin, Placke Tobias, Schmuch Richard, Gursel Selmiye Alkan, Yurum Alp
Faculty of Engineering and Natural Sciences (FENS), Sabancı University, Üniversite Caddesi 27, 34956 Istanbul, Turkey.
IEK-12, Forschungszentrum Jülich GmbH, Helmholtz Institute Münster, Münster, Corrensstraße 46, 48149 Münster, Germany.
ACS Appl Mater Interfaces. 2022 Aug 3;14(30):34665-34677. doi: 10.1021/acsami.2c06328. Epub 2022 Jul 25.
We report the performance of a conversion-type magnetite-decorated partially reduced graphene oxide (FeO@PrGO) negative electrode material in full-cell configuration with LiNiCoAlO (NCA) positive electrodes. To enable practical implementation of the conversion-type negative electrodes in full cells, the beneficial impact of electrochemical prelithiation on mitigating active lithium losses and improving cycle life is shown here for the first time in the literature. The initial Coulombic efficiency (ICE) of the full cells is improved from 70.8 to 91.2% by prelithiation of the negative electrode to 35% of its specific delithiation capacity. The prelithiation is shown to improve the surface passivation of the FeO@PrGO electrodes, leading to less electrolyte reduction on their surface which is prominent from the significantly lowered accumulated Coulombic inefficiency values, lower polarization growth, and doubled capacity retention by the 100th cycle. The reduced surface reactions of the negative electrode by prelithiation also aids in reducing the extent of aging of the NCA positive electrode. Overall, the prelithiation leads to a longer cycle life, where a retained capacity of 60.4% was achieved for the prelithiated cells by the end of long-term cycling, which is 3 times higher than the capacity retention of the non-prelithiated cells. Results reported herein indicate for the first time that the electrochemical prelithiation of the FeO@PrGO electrode is a promising approach for making conversion negative electrode materials more applicable in lithium-ion batteries.
我们报道了一种转换型磁铁矿修饰的部分还原氧化石墨烯（FeO@PrGO）负极材料与LiNiCoAlO（NCA）正极组成的全电池的性能。为了使转换型负极在全电池中得到实际应用，本文首次在文献中展示了电化学预锂化对减轻活性锂损失和改善循环寿命的有益影响。通过将负极预锂化至其特定脱锂容量的35%，全电池的初始库仑效率（ICE）从70.8%提高到了91.2%。结果表明，预锂化改善了FeO@PrGO电极的表面钝化，导致其表面的电解质还原减少，这从显著降低的累积库仑效率值、较低的极化增长以及第100次循环时容量保持率翻倍可以明显看出。预锂化减少了负极的表面反应，也有助于降低NCA正极的老化程度。总体而言，预锂化导致了更长的循环寿命，在长期循环结束时，预锂化电池的容量保持率达到了60.4%，这是非预锂化电池容量保持率的3倍。本文报道的结果首次表明，FeO@PrGO电极的电化学预锂化是使转换型负极材料在锂离子电池中更具适用性的一种有前景的方法。
