2D Mesoporous Naphthalene‐Based Conductive Heteroarchitectures toward Long‐Life, High‐Capacity Zinc‐Iodine Batteries

Abstract

Nowadays, rechargeable aqueous zinc‐iodine batteries have attracted extensive attention due to their low cost, high safety, and high theoretical capacity. However, the poor electrical conductivity of iodine and the shuttling effect of soluble polyiodide ions impose an insurmountable constraint on their performance. Here, a facile soft‐hard‐templated co‐assembly strategy is proposed to fabricate naphthalene‐based heteroarchitectured conductive nanosheets with ordered mesopore arrays (≈10 nm), uniform thickness (24.5 nm), high specific surface area (221.5 m2 g−1), and good electronic conductivity (3.9 × 10−3 S cm−1). Density function theory calculation and systematic experimental results show that the complementary combination of the 2D polar semiconducting polymer chains and conductive carbon framework enables the highly efficient immobilization of iodine and then constrains their shuttling effect through strong physicochemical interactions. Accordingly, the resultant zinc‐iodine batteries deliver a high specific capacity of 271.4 mAh g−1, excellent rate capability, and impressive long‐term cycling stability (35 000 cycles at a high current density of 10 A g−1), superior to most of the previous reports. This study opens new venues for rationally constructing heteroarchitectured porous materials for energy storage applications.

Activating and Stabilizing a Reversible four Electron Redox Reaction of I−/I+ for Aqueous Zn‐Iodine Battery

“…The reversible capacity of Ni−Fe−I electrode in the ZnSO 4 +ZnBr 2 electrolyte is retained about 94.6 % after 10000 cycles, which is much higher than the Ni−Fe mixed I 2 electrode (Figure S12). These results are superior to many previous reports about Zn‐I 2 battery (Figure 4f), such as AC‐I 2 , [46] PBA‐I 2 [47] and so on [23,48–53] . The long‐cycle stability shows the excellent iodine fixation ability of this host electrode.…”

Activating and Stabilizing a Reversible four Electron Redox Reaction of I−/I+ for Aqueous Zn‐Iodine Battery

“…The reversible capacity of Ni−Fe−I electrode in the ZnSO 4 +ZnBr 2 electrolyte is retained about 94.6 % after 10000 cycles, which is much higher than the Ni−Fe mixed I 2 electrode (Figure S12). These results are superior to many previous reports about Zn‐I 2 battery (Figure 4f), such as AC‐I 2 , [46] PBA‐I 2 [47] and so on [23,48–53] . The long‐cycle stability shows the excellent iodine fixation ability of this host electrode.…”

“…These results are superior to many previous reports about Zn-I 2 battery (Figure 4f), such as AC-I 2 , [46] PBA-I 2 [47] and so on. [23,[48][49][50][51][52][53] The long-cycle stability shows the excellent iodine fixation ability of this host electrode. It is due to that the interlayer redox reaction greatly suppresses the dissolution of iodide species, thus effectively inhibiting the shuttle effect.…”

Electrochemical performance and degradation mechanism of rechargeable aqueous Al2O3@Zn//MnO2 battery

“…Another challenge is related to the chemical decomposition of the aqueous‐based electrolyte that reacts with the zinc anode, impeding ion transport by forming passivation layers on the electrode surface, resulting in diminished battery lifespan 15 . Many research efforts have been made to address these challenges and enhance the cycling performance of the AZIBs, which encompass various engineering strategies such as anode surface modification and coating, and electrolyte development 16–19 . Among them, Zinc anode coating has been extensively studied for its ability to suppress dendrite formation during charge/discharge cycles, thereby improving cycling performance 20 .…”

“…15 Many research efforts have been made to address these challenges and enhance the cycling performance of the AZIBs, which encompass various engineering strategies such as anode surface modification and coating, and electrolyte development. [16][17][18][19] Among them, Zinc anode coating has been extensively studied for its ability to suppress dendrite formation during charge/discharge cycles, thereby improving cycling performance. 20 Also, the exploration of robust cathode materials exhibiting excellent electrochemical stability between zinc plating and dissolution can provide reliable cycle life and improved durability throughout charge/discharge cycles.…”