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Abstract Zn metal has shown promise as an anode material for grid‐level energy storage, yet is challenged by dendritic growth and low Coulombic efficiency. Herein, an ultrafast, stable, and high‐loading polymer anode for aqueous Zn‐ion batteries and capacitors (ZIBs and ZICs) is developed by engineering both the electrode and electrolyte. The anode polymer is rationally prepared to have a suitable electronic structure and a large π‐conjugated structure, whereas the electrolyte is manufactured based on the superiority of triflate anions over sulfate anions, as analyzed and confirmed via experiments and simulations. This dual engineering results in an optimal polymer anode withmore » a low discharge potential, near‐theoretical capacity, ultrahigh‐loading capability (≈50 mg cm ⁻² ), ultrafast rate (100 A g ⁻¹ ), and ultralong lifespan (one million cycles). Its mechanism involves reversible Zn ²⁺ /proton co‐storage at the carbonyl site. When the polymer anode is coupled with cathodes for both ZIB and ZIC applications, the devices demonstrate ultrahigh power densities and ultralong lifespans, far surpassing those of corresponding Zn‐metal‐based devices.« less

Silicon has the potential to revolutionize the energy storage capacities of lithium-ion batteries to meet the ever increasing power demands of next generation technologies. To avoid the operational stability problems of silicon-based anodes, we propose synergistic physicochemical alteration of electrode structures during their design. This capitalizes on covalent interaction of Si nanoparticles with sulfur-doped graphene and with cyclized polyacrylonitrile to provide a robust nanoarchitecture. This hierarchical structure stabilized the solid electrolyte interphase leading to superior reversible capacity of over 1,000 mAh g^-1 for 2,275 cycles at 2 A g^-1. Furthermore, the nanoarchitectured design lowered the contact of the electrolyte tomore » the electrode leading to not only high coulombic efficiency of 99.9% but also maintaining high stability even with high electrode loading associated with 3.4 mAh cm^-2. As a result, the excellent performance combined with the simplistic, scalable and non-hazardous approach render the process as a very promising candidate for Li-ion battery technology.« less