Deep Multiphase Conversion Derived from NiTe₂ Nanosheets with Preferred Kinetics for Highly Reversible Mild Aqueous Zinc–Tellurium Batteries

Abstract

Conversion‐type tellurium‐based cathodes have attracted great attention in aqueous zinc‐ion batteries (AZIBs) due to potentially high capacity with impressive Te4+/Te0/Te2− conversion. However, impeded by the low‐conductivity Te4+ species and unpreferred kinetics, realizing deep zinc‐tellurium redox remains a major challenge. Herein, energetic NiTe2 nanosheets are first proposed and implemented as preprepared tellurium‐based deep redox cathodes in AZIBs with accelerated electron transport and favorable kinetics. Operando synchrotron X‐ray diffraction and comprehensive ex situ characterizations demonstrate that Te4+ species from direct oxidation of NiTe2 in dilute mild‐aqueous electrolyte undergo a thermodynamic two‐step TeO2→Te→ZnTe discharge process, while the intertwined tellurium oxides and high‐conductivity nickel monomers derived in situ from NiTe2 nanosheets promote a kinetics‐preferred one‐step ZnTe→TeO2 charging conversion with significantly boosted reversibility. Therefore, a high capacity of 510 mAh g−1 at 50 mA g−1 and 93% capacity retention over 400 cycles at 2000 mA g−1 are established. Operando pH tracking and electrode‐electrolyte engineering analyses define that the mild electrolyte environment rich in moisture and electrode conductivity optimization are both critical for achieving reversible tellurium deep redox conversion.