Aqueous zinc ion hybrid capacitors (ZIHCs) hold great potential for large-scale energy storage applications owing to their high safety and low cost, but suffer from low capacity and energy density. Herein, pyridinic nitrogen enriched porous carbon (nPC) was successfully synthesized via the growth, subsequent annealing and acid etching of bimetal organic frameworks for high capacity and safe ZIHCs with exceptional rate capability. Benefiting from the mesopores for easy ion diffusion, high electrical conductivity enabled by in-situ grown carbon nanotubes matrix and residual metal Co nanoparticles for fast electron transfer, sufficient micropores and high N content (8.9 at%) with dominated pyridinic N (54%) for enhanced zinc ion storage, the resulting nPC cathodes for ZIHCs achieved high capacities of 302 and 137 mAh g⁻¹ at 1 and 18 A g⁻¹, outperforming most reported carbon based cathodes. Theoretical results further disclosed that pyridinic N possessed larger binding energy of −4.99 eV to chemically coordinate with Zn²⁺ than other N species. Moreover, quasi-solid-state ZIHCs with gelatin based gel electrolytes exhibited high energy density of 157.6 Wh kg⁻¹ at 0.69 kW kg⁻¹, high safety and mechanical flexibility to withstand mechanical deformation and drilling. This strategy of developing pyridinic nitrogen enriched porous carbon will pave a new avenue to construct safe ZIHCs with high energy densities.

水性锌离子混合电容器（ZIHC）的安全性高，成本低，因此在大规模储能应用中具有巨大潜力，但容量和能量密度低。本文中，通过双金属有机骨架的生长，随后的退火和酸蚀刻，成功地合成了吡啶二氮富集的多孔碳（nPC），以具有高倍率性能的高容量和安全ZIHC。得益于介孔易于离子扩散，原位生长的碳纳米管基质和残余金属Co纳米颗粒可实现快速电子转移的高电导率，足够的微孔和高氮含量（8.9 at％）和占主导地位的吡啶吡啶N（54％）为了增强锌离子存储，所得的ZIHC的nPC阴极实现了302和137 mAh g ^-1的高容量在1和18 A g ^-1下，性能优于大多数报道的碳基阴极。理论结果进一步公开了吡啶二氮比其他N具有更大的-4.99 eV与Zn ²⁺化学配位的结合能。此外，具有基于明胶的凝胶电解质的准固态ZIHCs在0.69 kW kg ^-1时表现出157.6 Wh kg ^-1的高能量密度，具有很高的安全性和机械柔韧性以承受机械变形和钻孔。开发吡啶氮富集多孔碳的这一策略将为构建高能量密度的安全ZIHC铺平一条新途径。