Activating sulfur oxidation reactionviasix-electron redox mesocrystal NiS2 for sulfur-based aqueous batteries

Abstract

Sulfur-based aqueous batteries (SABs) are deemed promising candidates for safe, low-cost, and high-capacity energy storage. However, despite their high theoretical capacity, achieving high reversible value remains a great challenge due to the thermodynamic and kinetics problems of elemental sulfur. Here, the reversible six-electron redox electrochemistry is constructed by activating sulfur oxidation reaction (SOR) process of the elaborate mesocrystal NiS2 (M-NiS2). Through the unique 6e− solid-to-solid conversion mechanism, the SOR efficiency can reach an unprecedented degree of ca. 96.0%. The SOR efficiency is further revealed to be closely associated with the kinetics feasibility and thermodynamic stability of the M-NiS2 intermedium in the formation of elemental sulfur. Benefiting from the boosted SOR, compared with the bulk electrode, the M-NiS2 electrode exhibits a high reversible capacity (1258 mAh g−1), ultrafast reaction kinetics (932 mAh g−1 at 12 A g−1), and long-term cyclability (2000 cycles at 20 A g−1). As a proof of concept, a new M-NiS2||Zn hybrid aqueous battery exhibits an output voltage of 1.60 V and an energy density of 722.4 Wh kgcath−1, which opens a new opportunity for the development of high-energy aqueous batteries.

Reconstructing the Anode Interface and Solvation Shell for Reversible Zinc Anodes

“…Recently, the demand for environmentally friendly and sustainable energy storage resources, especially the electrochemical energy storage devices, has been rapidly increasing, owing to the environmental pollution and fossil energy consumption. − Among various electrochemical technologies, lithium-ion batteries have been widely utilized as the power sources for various devices and electric vehicles because of the excellent cycling stability and energy density. − However, the safety hazards derived from the flammable electrolyte and expensive lithium resource have greatly impeded their application in the grid-scale energy storage field. , Preferably, aqueous zinc-ion batteries (ZIBs) have stood out now due to their high theoretical capacity, abundant zinc (Zn) resource, and nonflammable aqueous electrolyte. , To pursue high-performance ZIBs, various advanced cathodes like manganese-based oxides, , vanadium-based oxides, , organic molecules, , etc., have been proposed. Nevertheless, the practical applications of ZIBs are still hindered by the poor Coulombic efficiency (CE) and severe Zn dendrites, and the above obstacles of ZIBs are ascribed to the following two aspects.…”

Advanced Aqueous Ammonium-Ion Batteries Enabled by Hydrogen Bond Modulation

“…Aqueous ion batteries (AIBs) appear attractive in the energy storage field, particularly in large-scale energy storage, because of their intrinsic merits such as cost-effectiveness and high safety. − Conventionally, metallic ions, that is, Li + , Na + , K + , Zn 2+ , Mg 2+ , Ca 2+ , and Al 3+ , are considered as charge carriers and have been well-studied. − Nevertheless, potential problems such as earth abundance and metal contamination have somewhat raised people’s concerns about metal-ion batteries . Alternatively, the nonmetallic ammonium ion is being energetically investigated for AIBs because of its reproducible and environmentally friendly nature. − In addition, the NH 4 + ion exhibits exciting physicochemical properties, including low molar mass (18 g mol –1 ) and small hydrated radius (3.31 Å). , To date, several pioneering works have proved the possibility of aqueous ammonium-ion batteries (AAIBs) by developing Prussian blue analogues, metal oxides, and organic materials as electrodes. − However, these AAIBs still suffer from low working voltage window and capacity, which hinder the further application of AAIBs.…”

Defect engineering of two-dimensional materials for advanced energy conversion and storage

“…[379][380][381] Apart from the natural abundance and eco-friendliness, the zinc anode also has relatively low redox potential and high safety in the aqueous electrolytes. [382][383][384][385][386] For various MIBs, suitable electrode materials are the critical components toward well-electrochemical performance with favorable reaction kinetics. Besides LIBs, the electrode design and modification in SIBs and ZIBs have also been extensively studied to alleviate the current energy anxiety.…”