Abstract
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 poten-tial 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 multire-dox 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 electrochem-istry 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.
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