MXene‐Boosted Imine Cathodes with Extended Conjugated Structure for Aqueous Zinc‐Ion Batteries

Wang, Xiaoshuang; Liu, Yanan; Wei, Zengyan; Hong, Jingzhe; Liang, Hongbo; Song, Meixiu; Zhou, Yu; Huang, Xiaoxiao

doi:10.1002/adma.202206812

Cited by 82 publications

(35 citation statements)

References 68 publications

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“…The ex-situ 1 H solid-state NMR (Fig. 4c) spectrum shows that the discharged electrode exhibits a new peak at ~3.02 ppm, which is related to the H resonances in the N-H bonds 54 , further confirming that the protons could coordinate with the C=N bonds through oxidation reaction and the C-N-H bonds are significantly generated. This observation is also certificated by the ex-situ XPS analysis (Fig.…”

Section: Resultsmentioning

confidence: 83%

A long-range planar polymer with efficient π-electron delocalization for superior proton storage

Wang

Shi

et al. 2023

Preprint

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Due to the unique "Grotthus mechanism", aqueous proton batteries (APBs) are promising energy devices with intrinsic safety and sustainability. Although polymers with tunable molecular structures are expected as ideal electrode materials, their unsatisfactory proton-storage redox behaviors hinder the practical application in APB devices. Herein, a novel planar phenazine (PPHZ) polymer with a robust and extended imine-rich skeleton based on phenazine units is synthesized and used for APB application for the first time. The long-range planar configuration achieves ordered molecular stacking and reduced conformational disorder, while the high conjugation with strong π-electron delocalization optimizes energy bandgap and electronic properties, enabling to the polymer with ultra-low proton diffusion barriers (≤ 0.12 eV), high redox activity and superior electron affinity. As such, the PPHZ polymer as an electrode material exhibits fast, stable and unrivaled proton-storage redox behaviors with a record capacity of 254.5 mAh g-1 in aqueous acidic electrolyte, which is the highest value among all proton-inserted organic electrodes. Dynamic in-situ monitoring techniques confirm the high redox reversibility upon proton uptake/removal, and the corresponding protonation pathways are elucidated by multiple theoretical calculations. Moreover, a soft-packaged APB cell using PPHZ electrode exhibits an ultralong lifespan over 30,000 cycles, further verifying its promising application prospect.

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Section: Resultsmentioning

confidence: 83%

A long-range planar polymer with efficient π-electron delocalization for superior proton storage

Wang

Shi

et al. 2023

Preprint

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“…The rapid kinetics of the NI-DAQ electrode accounts for the higher capacitive-controlled contribution. 18 Furthermore, the galvanostatic intermittent titration technique (GITT) was used to calculate the ion diffusion coefficient To reveal the intercalation/extraction mechanism of Zn cations in the NI-DAQ electrode, CV curves in a 1 M aq H 2 SO 4 solution (vs Ag/AgCl) in a three-electrode system and a 2 M aq ZnSO 4 solution (vs Zn 2+ /Zn) for AZIBs (Figure 4a) were further implemented. It can be clearly seen that the CV curve of NI-DAQ shows two peaks at ∼−0.09/−0.08 and 0.01/0.04 V in the 1 M aq H 2 SO 4 solution, respectively.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…The superior kinetic mechanism can facilitate ion diffusion and equilibrium during cycling, which further leads to the great rate properties and cycling performance of the NI-DAQ electrode. , In addition, the capacitive-controlled contributions at various scan rates are calculated in Figure d, which gradually increase from 38.0 to 67.0% with the scan rate increasing from 0.1 to 1.0 mV s –1 . The rapid kinetics of the NI-DAQ electrode accounts for the higher capacitive-controlled contribution …”

Section: Resultsmentioning

confidence: 99%

“…Rechargeable aqueous zinc-ion batteries (AZIBs) have been in the spotlight for their high specific capacity (∼820.0 mA h g –1 ), small toxicity, and high economic efficiency. − In addition, the low redox potential (∼0.76 V vs SHE) of Zn 2+ /Zn promotes its application in electrodes . More importantly, water, as the aqueous electrolyte, has excellent ionic conductivity, high specific heat capacity, and inherent nonflammability, which can deliver unparalleled safety and allow cycling at large current densities.…”

Section: Introductionmentioning

confidence: 99%

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Organic Nanosheets of Imide-Linked Cathodes for High-Performance Aqueous Zinc-Ion Batteries

Feng

Cao

Guo

et al. 2023

ACS Appl. Energy Mater.

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Organic electrodes have been identified as promising energy-storage materials for aqueous zinc-ion batteries (AZIBs). Small molecular materials have ideal redox properties, high specific capacity, and structural diversity, making them a category of cathode candidates for AZIBs. However, the instability and dissolution during the extraction and insertion of H+/Zn2+ limit their application of the long-cycle stability for AZIBs. Herein, a small-molecule nanosheet (NI-DAQ, ∼14 nm in thickness) with imide linkage is designed and synthesized by the condensation of anthraquinones and anhydrides. It not only inhibits the dissolution of monomer electrodes but also boosts the reactivity and conductivity of the whole molecule by the introduction of π-conjugated imide groups and extended aromatic planes. Therefore, the NI-DAQ electrode obtains a large initial capacity of 191.9 mA h g–1 at 50 mA g–1 and superior cyclability after 3000 cycles at 500 mA g–1 with a minor average capacity fading rate of 0.01% per cycle. Moreover, in situ Fourier transform infrared (FT-IR) and ex situ X-ray photoelectron spectroscopy (XPS) characterization techniques have been implemented to investigate the redox mechanism of CO units in AZIBs for the NI-DAQ electrode. Thus, a promising conductive molecule is developed and explored in this paper, which can provide insights into the application of organic materials in AZIBs.

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“…Developing a durable and economical energy storage device is still a challenge for collecting energy from wind, solar, tide, and so on. Compared to commercial lithium-ion batteries, aqueous zinc-ion batteries (AZIBs) possess enormous potential on large-scale energy storage devices due to many merits [ 1 – 6 ]. However, the energy density and cycling life of AZIBs are further limited by the lack of robust cathode materials.…”

Section: Introductionmentioning

confidence: 99%

Molecular Engineering Design for High-Performance Aqueous Zinc-Organic Battery

et al. 2023

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Novel small sulfur heterocyclic quinones (6a,16a-dihydrobenzo[b]naphtho[2′,3′:5,6][1,4]dithiino[2,3-i]thianthrene-5,7,9,14,16,18-hexaone (4S6Q) and benzo[b]naphtho[2′,3′:5,6][1,4]dithiino[2,3-i]thianthrene-5,9,14,18-tetraone (4S4Q)) are developed by molecule structural design method and as cathode for aqueous zinc-organic batteries. The conjugated thioether (–S–) bonds as connected units not only improve the conductivity of compounds but also inhibit their dissolution by both extended π-conjugated plane and constructed flexible molecular skeleton. Hence, the Zn//4S6Q and Zn//4S4Q batteries exhibit satisfactory electrochemical performance based on 3.5 mol L−1 (M) Zn(ClO4)2 electrolyte. For instance, the Zn//4S6Q battery obtains 240 and 208.6 mAh g−1 of discharge capacity at 150 mA g−1 and 30 A g−1, respectively. The excellent rate capability is ascribed to the fast reaction kinetics. This system displays a superlong life of 20,000 cycles with no capacity fading at 3 A g−1. Additionally, the H+-storage mechanism of the 4S6Q compound is demonstrated by ex situ analyses and density functional theory calculations. Impressively, the battery can normally work at − 60 °C benefiting from the anti-freezing electrolyte and maintain a high discharge capacity of 201.7 mAh g−1, which is 86.2% of discharge capacity at 25 °C. The cutting-edge electrochemical performances of these novel compounds make them alternative electrode materials for Zn-organic batteries.

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MXene‐Boosted Imine Cathodes with Extended Conjugated Structure for Aqueous Zinc‐Ion Batteries

Cited by 82 publications

References 68 publications

A long-range planar polymer with efficient π-electron delocalization for superior proton storage

A long-range planar polymer with efficient π-electron delocalization for superior proton storage

Organic Nanosheets of Imide-Linked Cathodes for High-Performance Aqueous Zinc-Ion Batteries

Molecular Engineering Design for High-Performance Aqueous Zinc-Organic Battery

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