Abstract
Current aqueous Zn batteries (ZBs) seriously suffer from dendrite issues caused by rough electrode surfaces. Despite significant efforts in prolonging battery lifespans, minimum effort has been devoted to dendrite elimination in commercial-grade cathode loading mass. Instead, demonstrations have only been done at the laboratory level (≤2 mg cm-2). Additionally, new dilemmas regarding change of proton-storage behavior and interface pulverization have emerged in turn. Herein, hydrogen-substituted graphdiyne (HsGDY) with sub-ångström level ion tunnels and robust chemical stability was designed as an artificial interface layer to address these issues. This strategy prolonged the symmetric cell lifespan to >2400 h (100 days), which is 37-times larger than the one without protection (63 h). The simulation of dual-fields uncovered that HsGDY could redistribute the Zn2+ concentration field by spatially forcing Zn2+ to deviate from the irregular electric field. During practical use, the as-assembled full batteries delivered a long lifespan 50 000 cycles and remained stable even at a commercial-grade cathode loading mass of up to 22.95 mg cm-2. This HsGDY-protection methodology represents a great progress in Zn dendrite protection and demonstrates enormous potential in metal batteries.
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