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In this work, the concentration gradient design is applied to Ni-rich cathodes to study the mechanical properties of the particles. Ni-rich NMCs with enhanced cycle stability that uses our concentration gradient design are fabricated via one-step chemical bath deposition (CSBD) method (Fig. 1). The optimized concentrations of Mn and Co are determined based on the electrochemical impedance spectroscopy (EIS) results. Afterwards, the performance of these concentration gradient cathodes are investigated in Li metal coin cells to gain an understanding of the impact of composition gradient on the particle mechanical stability. Moreover, we use ex situ and in situ measurements to study the structure changes of cathodes upon the repeated volume changes. We verify that the Co-enriched cathodes with gradient design can effectively improve the Li-ion storage capacity and restrain particle cracking during volume change. Based on this understanding, we also establish the composition gradient–targeted design rule for mechanical stability. Co-enriched cathodes with gradient design provide a feasible route to enhance structural and morphological stability of Ni-rich NMCs for Li-ion batteries.
We fabricate cathodes with different Co and Mn concentrations to study the impacts of composition gradient on the mechanical properties of the particles. The evolution of particle microstructure during the initial charge-discharge cycles is studied via X-ray diffraction (XRD) ex situ and in situ characterizations. We first evaluate the effects of composition gradient on the Ni-rich cathode’s structure stability, and the corresponding electrochemical performance and morphology evolution are also investigated. Finally, based on the improved understanding of the composition gradient and structural stability, we establish the concentration gradient–targeted design rule for mechanical stability. The optimized concentration gradient provides Ni-rich cathodes with enhanced cycle stability. As an example, Co-enriched cathodes with gradient design exhibit excellent cycling performance and retain a high capacity of 144 mAh g−1 at 0.2 C after 400 cycles. The concentration gradient–targeted design rule can be summarized as follows: (1) Ni-rich cathodes with a Co-enriched surface exhibit low surface stiffness and are beneficial for suppressing particle cracking, and (2) Ni-rich cathodes with a Mn-enriched core and Co-enriched surface are beneficial for structural reversibility.
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