Heterostructured NiS 2 /ZnIn 2 S 4 Realizing Toroid-like Li 2 O 2 Deposition in Lithium–Oxygen Batteries with Low-Donor-Number Solvents

The aprotic lithium–oxygen (Li–O 2 ) battery has triggered tremendous efforts for advanced energy storage due to the high energy density. However, realizing toroid-like Li 2 O 2 deposition in low-donor-number (DN) solvents is still the intractable obstruction. Herein, a heterostructured NiS 2 /ZnIn 2 S 4 is elaborately developed and investigated as a promising catalyst to regulate the Li 2 O 2 deposition in low-DN solvents. The as-developed NiS 2 /ZnIn 2 S 4 promotes interfacial electron transfer, regulates the adsorption energy of the reaction intermediates, and accelerates O–O bond cleavage, which are convincingly evidenced experimentally and theoretically. As a result, the toroid-like Li 2 O 2 product is achieved in a Li–O 2 battery with low-DN solvents via the solvation-mediated pathway, which demonstrates superb cyclability over 490 cycles and a high output capacity of 3682 mA h g –1 . The interface engineering of heterostructure catalysts offers more possibilities for the realization of toroid-like Li 2 O 2 in low-DN solvents, holding great promise in achieving practical applications of Li–O 2 batteries as well as enlightening the material design in catalytic systems.