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            -Heterocycles Extended π-Conjugation Enables Ultrahigh Capacity, Long-Lived, and Fast-Charging Organic Cathodes for Aqueous Zinc Batteries

Peng, Huiling; Xiao, Jin; Wu, Zhonghan; Zhang, Lei; Geng, Yaheng; Xin, Wenli; Li, Junwei; Yan, Zichao; Zhang, Kai; Zhu, Zhiqiang

doi:10.31635/ccschem.022.202202276

Cited by 44 publications

(22 citation statements)

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“…However, when the energy density is calculated using the total mass of the cathode (DPT + KB + binder) and consumed Zn, the Zn//DPT cell with 10 wt % KB in the cathode delivers a specific energy density of up to 149.7 Wh kg –1 at a power density of 40.9 W kg –1 , which exceeds that of the Zn//DPT cell with 30 wt % KB in the cathode. In addition to the extensive use of conductive additives, ,,,, organic electrodes have also been investigated with low mass loading (typically less than 2 mg cm –2 ) − (Table S6), resulting in low areal capacity (mAh cm –2 ). This approach aims to reduce the absolute current of the tested electrode [i.e., areal current density (mA cm –2 ) = mass loading (g cm –2 ) × current density (mA g –1 )], thereby lowering resistance-induced energy loss.…”

Section: Resultsmentioning

confidence: 99%

Activating Organic Electrode via Trace Dissolved Organic Molecules

Huang,

Qiu,

Wang

et al. 2023

J. Am. Chem. Soc.

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Organic electrode materials have gained attention for their tunable structures and sustainability, but their low electronic conductivity requires the use of large amounts of carbon additives (30 wt %) and low mass loadings (<2 mg cm–2) in electrodes. Here, we synthesize dibenzo[b,i]phenazine-5,7,12,14-tetrone (DPT) as a cathode active material for an aqueous Zn battery and find that Zn2+ storage dominates the cathode reaction. This battery demonstrates high capacity (367 mAh g–1), high-rate performance, and superlong life (12000 cycles). Remarkably, despite DPT’s insulative nature, even with a high mass loading (10 mg cm–2) and only 10 wt % carbon additives, the DPT-based cathode exhibits promising performance due to trace dissolved discharge product (DPT x–). During discharge, the DPT is reduced to trace amounts of dissolved DPT x– at the cathode surface, which in turn reduces the remaining solid DPT as a redox mediator. Furthermore, dissolution–redeposition results in the reduction of DPT size and the formation of pores, further activating the electrode.

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Section: Resultsmentioning

confidence: 99%

Activating Organic Electrode via Trace Dissolved Organic Molecules

Huang,

Qiu,

Wang

et al. 2023

J. Am. Chem. Soc.

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“…Previous studies have shown that the electrochemistry at the cathode side does not only involve the Zn 2+ ions but also that protons (H + ) function as charge carriers in slightly acidic electrolytes. ,,,,,,, Accommodating H + ions by carbonyl units during the discharge process leads to a local pH increase, which promotes the precipitation of zinc hydroxy sulfate [Zn 4 SO 4 (OH) 6 · n H 2 O] as a byproduct on the cathode surface. Thus, the reversible H + co-(de)insertion can be followed by the precipitation and dissolution of zinc hydroxy sulfate on the cathode surface during discharging and charging, respectively.…”

Section: Resultsmentioning

confidence: 99%

“…In addition, the applicability of some of these conventional inorganic cathode materials is constrained by their high cost and toxicity due to the nature of the metal they contain . Researchers have recently recognized the potential of redox-active organic compounds as alternatives for inorganic electrode materials due to their sustainability, cost, and versatility in molecular design. − Among various organic groups, carbonyl-containing organic compounds, such as calix[4]quinone, phenanthraquinone, p-chloranil, and 1,4,5,8-naphthalene diimide, show promising redox activity in rechargeable aqueous ZIBs and reversibly host Zn 2+ ions by coordination reactions. Nevertheless, the high solubility of their discharged products in aqueous electrolytes and their poor conductivity hinder their electrochemical performances regarding cycle stability and rate capability.…”

Section: Introductionmentioning

confidence: 99%

Ultralong-Life Quinone-Based Porous Organic Polymer Cathode for High-Performance Aqueous Zinc-Ion Batteries

Buyukcakir,

Yuksel,

Begar

et al. 2023

ACS Appl. Energy Mater.

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We synthesized and studied a redox-active quinonebased porous organic polymer (rPOP) and found ultralong cycle life: it is a promising organic cathode for aqueous zinc-ion batteries (ZIBs). It has high physicochemical stability and enhanced intrinsic conductivity from its fused-aromatic conjugated skeleton. rPOP's high porosity allows for efficient Zn 2+ infiltration through the pores during charging−discharging cycles and contributes to the efficient utilization of redox-active quinone units. It delivers a specific capacity of 120 mAh g −1 at a current density of 0.1 A g −1 with a flat and long discharge plateau, which is critically important to provide a stable voltage output. It provides ultralong cycle life at a current density of 1.0 A g −1 for 1000 and at 2.0 A g −1 for 30 000 cycles, with initial capacity retention of 95 and 66%, respectively. The coinsertion (Zn 2+ and H + ) charge storage mechanism was investigated using various electrochemical measurements and ex/in situ structural characterization techniques, and is explained herein. These findings contribute to a better understanding of the structure− property relationship for rPOP and open a new avenue for new organic cathode materials for high-performance next-generation aqueous batteries.

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“…Aqueous zinc-based energy storage devices, such as zinc ion batteries (ZIBs) or hybrid zinc ion capacitors (ZICs), are of great signicance in the construction of intrinsically safe electrochemical energy storage systems, which have good application prospects in the future large-scale energy storage eld. [1][2][3][4][5][6][7] However, the practical development of high-performance zincbased energy storage devices is seriously impeded by a series of problems in the Zn metal anode, such as side reactions, dendrite growth, and the low utilization rate of zinc anode. 3,4,6 Zn metal has several forms, including Zn foil/plate, Zn powder, Zn mesh, and Zn foam, which can be used as Zn metal anode.…”

Section: Introductionmentioning

confidence: 99%