Coupling interfaces between hollow carbon dodecahedrons and layered double hydroxides for high-performance rechargeable zinc−air batteries

doi:10.15302/frontphys.2025.014210

2025, Vol. 20

Issue (1) : 14210 https://doi.org/10.15302/frontphys.2025.014210

Coupling interfaces between hollow carbon dodecahedrons and layered double hydroxides for high-performance rechargeable zinc−air batteries

Jing Zhang^1,², Luo Xu², Yan Lin³, Baojian Xie^1,², Chunjie Li², Tao Hu³, Ulla Lassi³(

), Ruguang Ma²(

), Chang Ming Li²(

)

¹. School of Physical Science and Technology, Suzhou University of Science and Technology, Suzhou 215009, China
². School of Materials Science and Engineering, Suzhou University of Science and Technology, Suzhou 215009, China
³. Research Unit of Sustainable Chemistry, University of Oulu, Oulu 90570, Finland

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Abstract

The rational design of high-performance bifunctional electrocatalysts toward both oxygen reduction reaction (ORR) and oxygen evolution reaction (OER) is critical for the development of high-efficiency zinc−air batteries (ZABs). Herein, we report a facile method to synthesize a bifunctional electrocatalyst (FeNC/LDHs), which consists of Fe-doped hollow carbon dodecahedron (FeNC) coupling with NiFe-layered double hydroxides (LDHs). The coupling integration of FeNC dodecahedra and LDH nanosheets enriches the electrochemically active surface area and modulates the electron redistribution via oxygen bridges between FeNC and LDHs, thus effectively improving electrocatalytic activity and exhibiting a small potential difference of ΔE = 0.68 V during the ORR and OER process. The optimized FeNC/LDH-21 as a cathode in zinc-air batteries demonstrates a specific capacity of 810 mAh·g⁻¹ at 10 mA·cm⁻² and a power density of 85 mW·cm⁻², and stable operation over 160 h. Moreover, the as-assembled solid-state flexible ZAB reaches a power density of 32.4 mW·cm⁻² and maintains a stable charge-discharge process at different bending or hammering states. This work opens an avenue for the facile and large-scale synthesis of bifunctional electrocatalysts and would propel the practical application of ZABs.

Keywords metal−organic framework bifunctional electrocatalyst rechargeable zinc−air battery

Corresponding Author(s): Ulla Lassi,Ruguang Ma,Chang Ming Li

About author:

Issue Date: 11 October 2024

Cite this article:

Jing Zhang,Luo Xu,Yan Lin, et al. Coupling interfaces between hollow carbon dodecahedrons and layered double hydroxides for high-performance rechargeable zinc−air batteries[J]. Front. Phys. , 2025, 20(1): 14210.

URL:

https://academic.hep.com.cn/fop/EN/10.15302/frontphys.2025.014210
https://academic.hep.com.cn/fop/EN/Y2025/V20/I1/14210

Fig.1 (a) Schematic illustration for synthesizing FeNC and FeNC/LDH-21. (b) SEM image, (c) TEM image, (d) enlarged TEM image, (e) HRTEM image and SAED pattern. (f, g) HAADF-STEM image of FeNC/LDH-21 and corresponding EDS mapping images on C, Fe, O and Ni elements in FeNC/LDH-21.

Fig.2 (a) XRD patterns, (b) Raman spectra of FeNC, FeNC/LDH-21 and FeNC/LDH-11, respectively; (c) C 1s, (d) N 1s, (e) Ni 2p, and (f) Fe 2p high-resolution XPS spectra of FeNC/LDH-21 and FeNC/LDH-11, respectively.

Fig.3 (a) LSV curves of FeNC/LDH-21, FeNC/LDH-11, FeNC, NiFe-LDH and Pt/C in O₂-saturated 0.1 mol/L KOH solution. (b) Tafel plots derived from the LSV curves in (a). (c) LSV curves of FeNC/LDH-21 at different rotation speeds and (inset) Koutecky-Levich plots. (d) H₂O₂ yield and the calculated electron-transferred number of FeNC/LDH-21 from the RRDE test in (e). i–t chronoamperometric responses of FeNC/LDH-21 and Pt/C. (f) LSV curves of FeNC/LDH-21, FeNC/LDH-11, NiFe-LDH and RuO₂ in O₂-saturated 0.1 mol/L KOH towards OER. (g) Tafel plots derived from the LSV curves in (f). (h) LSV curves of both OER and ORR for different catalysts. (i) Nyquist plots of FeNC/LDH-21, FeNC/LDH-11, FeNC and Pt/C.

Fig.4 Total DOS of (a) FeNC, (b) NiFe-LDH, (c) FeNC/LDH (Fe?O?Fe) and (d) FeNC/LDH (Fe?O?Ni). Differential charge density of (e) FeNC/LDH (Fe?O?Fe) and (f) FeNC/LDH (Fe?O?Ni).

Fig.5 Performance of rechargeable ZABs. (a) Schematic of the rechargeable a ZAB. (b) Photo of two ZABs in series to power a red LED light in ambient air. (c) Rate performance. (d) Charge and discharge curves. (e) Polarization and power density profiles. (f) Specific capacity of a rechargeable ZAB. (g) Cycling performance at 10 mA·cm^?2 and (h) enlarged voltage profiles of charge and discharge at the beginning and after cycling.

Fig.6 Performance of flexible ZABs. (a) Schematic of the rechargeable flexible ZABs. (b) Open circuit voltage of a sandwich-type flexible ZAB. (c) Polarization and power density profiles. (d) Rate performances. (e) Cycling performance at 2 mA·cm^?2. (f) Photo of flexible ZABs in series to power a red LED at the folding or hammering state.

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