“Co-coordination force” assisted rigid-flexible coupling crystalline polymer for high-performance aqueous zinc-organic batteries

Organic electrode materials (OEMs) have attracted substantial attention for aqueous zinc-ion batteries (AZIBs) due to their advantages in relieving resource and environmental anxiety. However, the potential of OEMs is plagued by their low achievable capacity and high solubility. Here, we have proposed a new concept of "co-coordination force" and designed a rigid-flexible coupling crystalline polymer that can overcome the abovementioned limitations. The obtained crystalline polymer (BQSPNs) with multiredox centres makes the BQSPNs exist intermolecular hydrogen bonds (HB) among -C=O, -C=N, and -NH and consequently exhibits transverse two-dimensional arrays and longitudinal π-π stacking structure. Additionally, in-situ FTIR, Raman, variable temperature FTIR spectra, and 2D nuclear overhauser effect spectroscopy (NOESY) well capture the existence and evolution process of HB during the electrochemistry reaction process of BQSPNs, uncovering the effect of HB in stabilizing the structure and promoting the reaction kinetics. As a result, the BQSPNs with rationally designed "co-coordination force" deliver a high capacity of 459.6 mAh/g and a stable cycling lifetime for more than 100,000 cycles at 10 A/g in AZIBs. Our results disclose the HB effect and provide a brand-new strategy for high-performance OEMs design.