Linear Polymer Cathode Materials for Highly Efficient Aqueous Zinc-Ion Batteries: Is the High Active Sites Density Necessary?

用于高效水系锌离子电池的线性聚合物阴极材料:高活性位点密度是必要的吗?

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Abstract

Recently, research on aqueous zinc-ion batteries (AZIBs) has always focused on improving the energy storage performance by increasing the number of active sites, particularly in designing organic/polymer materials with a high density of active sites. However, does a higher density of active sites necessarily induce enhanced energy storage performance? To verify this issue, we have designed two linear polymers, where TAPT-DHBQ contains an additional pair of active sites (carbonyl groups) compared to TABQ-DHBQ, with theoretical specific capacities of 545.26 and 379.14 mAh g(-1), respectively. Interestingly, the experimental results have deviated with the specific capacities of these polymers being comparable, measuring to be 325 mAh g(-1) (TABQ-DHBQ) and 280 mAh g(-1) (TAPT-DHBQ). This is attributed to the competition effect between neighboring active sites, which leads to decreased utilization of active sites. As a result, the Zn//TABQ-DHBQ batteries with ZnI(2) electrolyte additive have exhibited high specific capacities of 618 and 360 mAh g(-1) at the current densities of 1 and 10 A g(-1), along with a high energy density of 678.6 Wh kg(-1) (1 A g(-1)). The finding underscores the importance of uniform electron cloud distribution in cathode materials for achieving efficient AZIBs.

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