| Autor: |
Lyu, Lulu, Hu, Xu, Lee, Suwon, Fan, Wenqi, Kim, Gilseob, Zhang, Jiliang, Zhou, Zhen, Kang, Yong-Mook |
| Zdroj: |
Journal of the American Chemical Society; February 2024, Vol. 146 Issue: 7 p4803-4813, 11p |
| Abstrakt: |
The design of temperature-adaptive Zn–air batteries (ZABs) with long life spans and high energy efficiencies is challenging owing to sluggish oxygen reduction reaction (ORR) kinetics and an unstable Zn/electrolyte interface. Herein, a quasi-solid-state ZAB is designed by combining atomically dispersed Fe–N–C catalysts containing pyridinic N vacancies (FeNC-VN) with a polarized organo-hydrogel electrolyte. First-principles calculation predicts that adjacent VNsites effectively enhance the covalency of Fe–Nxmoieties and moderately weaken *OH binding energies, significantly boosting the ORR kinetics and stability. In situRaman spectra reveal the dynamic evolution of *O2–and *OOH on the FeNC-VNcathode in the aqueous ZAB, proving that the 4e–associative mechanism is dominant. Moreover, the ethylene glycol-modulated organo-hydrogel electrolyte forms a zincophilic protective layer on the Zn anode surface and tailors the [Zn(H2O)6]2+solvation sheath, effectively guiding epitaxial deposition of Zn2+on the Zn (002) plane and suppressing side reactions. The assembled quasi-solid-state ZAB demonstrates a long life span of over 1076 h at 2 mA cm–2at −20 °C, outperforming most reported ZABs. |
| Databáze: |
Supplemental Index |
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