4.8 Article

Activating Organic Electrode via Trace Dissolved Organic Molecules

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JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
卷 145, 期 47, 页码 25604-25613

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AMER CHEMICAL SOC
DOI: 10.1021/jacs.3c06668

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Organic electrode materials with tunable structures and sustainability have gained attention. In this study, dibenzo[b,i]phenazine-5,7,12,14-tetrone (DPT) is synthesized as a cathode active material for an aqueous Zn battery, exhibiting high capacity, high-rate performance, and superlong life. Despite DPT's insulative nature, the presence of trace dissolved discharge product DPTx- enables promising performance even with high mass loading and low carbon additives.
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 (DPTx-). During discharge, the DPT is reduced to trace amounts of dissolved DPTx- 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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