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Interfacial Electron Redistribution on Lattice-Matching NiS_2/NiSe_2 Homologous Heterocages with Dual-Phase Synergy to Tune the Formation Routes of Li_2O_2

机译:Interfacial Electron Redistribution on Lattice-Matching NiS_2/NiSe_2 Homologous Heterocages with Dual-Phase Synergy to Tune the Formation Routes of Li_2O_2

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摘要

Li–O_2 batteries (LOBs) exhibit ultrahigh theoretical energy density, but sluggishreaction kinetics and adverse parasitic reactions seriously hinder their furtherdevelopment. It is thus urgent to exploit cost-effective and durable electrocatalyststo perfect LOBs performance and promote their practical application. Inthis work, lattice-matching composites are synthesized based on homologousheterostructure (HHS) with hollow nanocage-like architecture. As expected,the unique architecture with built-in electric fields of NiS_2/NiSe_2 HHS enablesthe rapid transfer of electron/ions, favorable electrolyte permeation onthe cathode surfaces, and provides sufficient active sites for oxygen evolutionreaction and oxygen reduction reaction. Moreover, the constructs NiS2/NiSe_2 HHS can evidently catalyze the formation of dispersed platelet-shape andfluffy film-like Li_2O_2 discharge products via the surface/solution routes due tothe greatly reduced adsorption energy of the LiO_2 intermediates on the built-inelectric fields, while the NiS_2 and NiSe_2 counterparts induce the formation ofLi2O2 films by the surface path, limiting its electrocatalytic activities. Theseresults suggest that lattice-matching HHS engineering of cathode catalysts canbe an effective approach to tuning the Li_2O_2 formation, which holds attractiveand great application prospects in the development of high-performance LOBs.

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