High-Voltage and Ultrastable Aqueous Zinc–Iodine Battery Enabled by N-Doped Carbon Materials: Revealing the Contributions of Nitrogen Configurations

Abstract

The rechargeable aqueous zinc–iodine (Zn–I2) battery has emerged as a promising electrochemical energy storage technology. However, poor cycling stability caused by the dissolution of iodine species into the electrolyte limited its practical application. Herein, we report a nitrogen-doped porous carbon (NPC) material in gram scales. Performed as an iodine host in the Zn–I2 battery, the NPC shows a high specific capacity (345.3 mAh g–1 at 0.2 C), superior rate capability (53.2% capacity retention at 10 C), and remarkable cycling stability (10 000 cycles at 10 C with a capacity retention of 80.9%). More importantly, DFT computations reveal that the graphitic-N (N-Q) exhibits the strongest adsorption of iodine; however, pyridinic-N (N-6) shows the weakest adsorption of iodine. Moreover, the N-6/N-Q ratio is an essential parameter that significantly determined the electrochemical performance of Zn–I2 batteries. Therefore, the improved long-term cycling stability and rate capability of the as-designed Zn–I2 battery are attributable to the decrease of the N-6/N-Q ratio. This work is of great significance for devolving highly reversible Zn–I2 batteries.

A renewable biomass-based lignin film as an effective protective layer to stabilize zinc metal anodes for high-performance zinc–iodine batteries

“…48 Besides, the presence of I-O is probably because of partial oxidation of I 2 . 49 During the charge process, I À ions are oxidized to I 2 , while the disproportionation reaction occurs between I 2 and I À to form I 3 À ions (2I À À 2e À / I 2 , I 2 + I À / I 3 À ). During the discharge process, I 3 À ions are reduced to I À (I 3 À + 2e À / 3I À ).…”

Electrochemical reaction behavior of MnS in aqueous zinc ion battery

“…[5][6][7] Among them, the rechargeable zinc ion battery has aroused considerable attention due to its admirable safety, cost-effectiveness, moderate redox potential (−0.76 V vs. SHE), and decent theoretical capacity (∼820 mA h g −1 ) of the Zn anode. 6,8,9 However, the zinc ion battery is still in its infancy, and one of the core tasks aim to prompt the development of the zinc ion battery is to screen out competent cathode materials that can sustainably serve for repeated Zn 2+ intercalation/deintercalation. 5,6 The past several years have witnessed a considerable increase in the research efforts for cathode materials' screening and great progresses have been achieved.…”

Eutectic electrolyte based on N-methylacetamide for highly reversible zinc–iodine battery

“…, boron, nitrogen) were also adopted to promote interface redox reactions or reduce the adsorption energy of iodine. 15–17 On the other hand, the polyaniline-I 2 cathode was proposed and proved the electrostatic interaction between amine (–NH–), imine (–NH+) and iodine, effectively, inhibited the dissolution and shuttle effect. 18 Benefiting from the local electron transfer and trapping effect of the MXene host and the reduced reaction energy barrier in Prussian blue analogue, one-step I − /I 0 conversion was further realized in Nb 2 AlT x and Co[Co 1/4 Fe 3/4 (CN)] 6 .…”