Journal
ACS APPLIED MATERIALS & INTERFACES
Volume 11, Issue 6, Pages 5966-5977Publisher
AMER CHEMICAL SOC
DOI: 10.1021/acsami.8b18607
Keywords
Mg-Li dual-salt electrolyte; POM; MOF; NENU-5; chalcogenide cathodes; Mg-based batteries
Funding
- National Key R&D Program of China [2016YFB0901600]
- National Natural Science Foundation of China [51772313, U1830113]
- Hundred Talents Program of Chinese Academy of Sciences
- Thousand Talents Program of Shanghai
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Mg anode has pronounced advantages in terms of high volumetric capacity, resource abundance, and dendrite-free electrochemical plating, which make rechargeable Mg-based batteries stand out as a representative next-generation energy storage system utilized in the field of large-scale stationary electric grid. However, sluggish Mg2+ diffusion in cathode lattices and facile passivation on the Mg anode hinder the commercialization of Mg batteries. Exploring a highly electroactive cathode prototype with hierarchical nanostructure and compatible electrolyte system with the capability of activating both an anode and a cathode is still a challenge. Here, we propose a POM subset of MOF (NENU-5) core-shell architecture as a hybrid precursor template to achieve the stacking of tailored, chalcogenide nanosheets around MoO2-C conductive stakes, which can be employed as conversion-insertion cathodes (Cu1.96S-MoS2-MoO2 and Cu2Se-MoO2) for Mg-Li dual-salt batteries. Li-salt modulation further activates the capacity and rate performance at the cathode side by preferential Li-driven displacement reaction in Cu+ extrusible lattices. The heterogeneous conductive network and conformal dual-doped carbon coating enable a reversible capacity as high as 200 mAh/g with a coulombic efficiency close to 100%. The composite cathode can endure a long-term cycling up to 400 cycles and a high current density up to 2 A/g. The diversity of MOF-based materials infused by functional molecules or clusters would enrich the nanoengineering of electrodes to meet the performance demand for future multivalent batteries.
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