Aqueous rechargeable zinc-ion batteries (ARZIBs) are promising energy storage systems owing to their ecofriendliness, safety, and cost-efficiency. However, the sluggish Zn2+ diffusion kinetics originated from its inherent large atomic mass and high polarization remains an ongoing challenge. To this end, electrodes with 3D architectures and high porosity are highly desired. This work reports a rational design and fabrication of hierarchical core-shell structured cathodes (3D@V2 O5 ) for ARZIBs by integrating fused deposition modeling (FDM) 3D-printing with atomic layer deposition (ALD). The 3D-printed porous carbon network provides an entangled electron conductive core and interconnected ion diffusion channels, whereas ALD-coated V2 O5 serves as an active shell without sacrificing the porosity for facilitated Zn2+ diffusion. This endows the 3D@V2 O5 cathode with high specific capacity (425 mAh g-1 at 0.3 A g-1 ), competitive energy and power densities (316 Wh Kg-1 at 213 W kg-1 and 163 Wh Kg-1 at 3400 W kg-1 ), and good rate performance (221 mAh g-1 at 4.8 A g-1 ). The developed 3D@V2 O5 cathode provides a promising model for customized and scalable battery electrode engineering technology. As the ALD-coated layer determines the functional properties, the proposed strategy shows a promising prospect of FDM 3D printing using 1D carbon materials for future energy storage.

D Printing and Innovation Hub Department of Chemistry Mendel University in Brno Zemedelska 1 Brno CZ 613 00 Czech Republic

Department of Chemical and Biomolecular Engineering Yonsei University 50 Yonsei ro Seodaemun gu Seoul 03722 Korea

Department of Medical Research China Medical University Hospital China Medical University No 91 Hsueh Shih Road Taichung 40402 Taiwan

Future Energy and Innovation Laboratory Central European Institute of Technology Brno University of Technology Brno 61600 Czech Republic

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Anode Free Zinc-Metal Batteries (AFZMBs): A New Paradigm in Energy Storage