Tao, Yayuan, Li, Zhi, Tang, Linbin, Pu, Xiaoming, Cao, Tong, Cheng, Danhong, Xu, Qunjie, Liu, Haimei, Wang, YongGang, and Xia, Yongyao
Rechargeable aqueous zinc-ion batteries (ZIBs) are possible future replacements for large-scale energy storage devices because of their safety, low cost, and abundance of materials. Finding a competitive cathode material suitable for zinc-ion insertion/de-insertion, needed to achieve high reversible capacity and long cycle stability, is one of the most important and arduous challenges. For the first time, nickel and cobalt co-substituted spinel ZnMn 2 O 4 nanoparticles, homogeneously loaded onto N-doped reduced graphene oxide (ZnNi x Co y Mn 2-x-y O 4 @N-rGO), were synthesised through a one-step hydrothermal method and applied as a cathode material to accommodate the intercalation of zinc ions. The as-prepared ZnNi x Co y Mn 2-x-y O 4 @N-rGO displayed excellent electrochemical performance, with a reversible capacity of 95.4 mA h g−1, achieved at 1000 mA g−1 after 900 cycles, and a capacity retention ratio of 79%. When the current density increased from 10 mA g−1 to 1500 mA g−1, high capacity (200.5 mA h g−1 to 93.5 mA h g−1) was achieved, which was much higher than that of ZMO@N-rGO without nickel and cobalt co-substituting (184 mA h g−1 to 59.2 mA h g−1), demonstrating excellent rate performance. These excellent electrochemical properties are attributed to the co-substituting of nickel and cobalt elements, which is an effective approach to promote Zn2+ de-intercalation and to stabilize the spinel structure in order to suppress the Jahn-Teller distortion of Mn3+. Therefore, nickel and cobalt co-substituting of spinel ZnMn 2 O 4 @N-rGO with a stable structure opens up new possibilities for large-scale application of rechargeable, aqueous ZIBs. Image 1 • Nickel and cobalt co-substituted spinel ZnMn 2 O 4 nanoparticles were synthesised • The ultrafine ZnNi 0.39 Co 0.59 Mn 0.98 O 4 loaded onto N-doped reduced graphene oxide. • The ZnNi 0.39 Co 0.59 Mn 0.98 O 4 @N-rGO exhibited excellent performance as a cathode for SIBs. • Nickel and cobalt co-substituting stabilized the spinel structure. • The N-doped graphene network ensured highly electronic conductivity. [ABSTRACT FROM AUTHOR]