Capacity fading and voltage decay is one of the biggest obstacles for the practical application of Li‐rich layered oxides due to the serious surface‐related detrimental reactions. Herein, we develop a versatile and scalable method to construct a robust surface‐integrated structure. All the designed samples deliver outstanding capacity and voltage stability, among which the Zn‐treated sample possesses the best electrochemical performance. Its capacity retention is larger than 90 % after 400 cycles with a voltage decay ratio as small as 0.73 mV per cycle. What is more, the rules of surface‐integrated structure with different cations in terms of capacity and voltage stability is further deciphered by combining with density function theory (DFT) calculations. It is found that to obtain advanced Li‐rich layered oxide cathodes, cations in Li‐sites should firstly ensure the binding energy of the surface‐integrated structure in a lower level and then provide Bader charge for the nearest O atoms as small as possible.

With the explosive growth of the electric energy storage industry, it is urgent to develop cathode materials with wide working voltage, high capacity, and low cost. Li-rich layered oxides have...

Capacity fading and voltage decay is one of the biggest obstacles for the practical application of Li‐rich layered oxides due to the serious surface‐related detrimental reactions. Herein, we develop a versatile and scalable method to construct a robust surface‐integrated structure. All the designed samples deliver outstanding capacity and voltage stability, among which the Zn‐treated sample possesses the best electrochemical performance. Its capacity retention is larger than 90 % after 400 cycles with a voltage decay ratio as small as 0.73 mV per cycle. What is more, the rules of surface‐integrated structure with different cations in terms of capacity and voltage stability is further deciphered by combining with density function theory (DFT) calculations. It is found that to obtain advanced Li‐rich layered oxide cathodes, cations in Li‐sites should firstly ensure the binding energy of the surface‐integrated structure in a lower level and then provide Bader charge for the nearest O atoms as small as possible.

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