3D-Printed Hierarchically Porous MOF-Derived Cathodes for Realizing High-Performance Flexible Quasi-Solid-State Aqueous Zinc-Cobalt Batteries.
basic_science · Level V
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- Record sourced from PubMed, PMID 40763332.
- Also identified by DOI 10.1021/acsnano.5c05876.
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Abstract
Rechargeable aqueous Zn-ion batteries hold significant promise for wearable electronics due to their intrinsic safety and eco-friendliness, yet cobalt-based cathodes remain constrained by poor conductivity and sluggish kinetics. Addressing these limitations, we developed 3D-printed (3DP) hierarchically porous MOF-derived cathodes for aqueous zinc-cobalt (Zn-Co) batteries via three synergistic innovation technology pathways: (i) ZIF-67-derived nitrogen-doped carbon-coated Co<sub>3</sub>O<sub>4</sub> nanoparticles (Co<sub>3</sub>O<sub>4</sub>-NC NPs) were synthesized using a scalable hydrothermal method and subsequent annealing process; (ii) a dual-ion (Zn<sup>2+</sup>/Mn<sup>2+</sup>)-optimized hybrid electrolyte system, that is, the dual-ion synergy from Mn<sup>2+</sup> additive enhanced Zn<sup>2+</sup> desolvation kinetics while suppressing dendrite formation; and (iii) 3D printing hierarchically porous microlattice architecture integrating reduced graphene oxide/carbon nanotubes-based (rGO/CNTs-based) to establish bicontinuous ion/electron transport networks. The 3DP button Zn-Co cells (thickness: 0.8 mm) delivered an exceptional areal capacity (∼0.30 mAh cm<sup>-2</sup> at 2 mA cm<sup>-2</sup>) and excellent cycling stability (near-zero decay over 750 cycles). Specially, a 4 mm thick 3DP flexible quasi-solid-state Zn-Co battery (3DP f-QSS Zn-Co) device employing PVA/(ZnSO<sub>4</sub> + MnSO<sub>4</sub>) gel electrolyte achieved an enhanced areal capacity (∼0.16 mAh cm<sup>-2</sup> at 1 mA cm<sup>-2</sup>), a high energy density (∼151.0 Wh kg<sup>-1</sup> at a power of 975 W kg<sup>-1</sup>), and an ultralong cyclability (∼87.5% retention after 2500 cycles at 1 A g<sup>-1</sup>). Furthermore, the 3DP f-QSS Zn-Co devices enabled scalable voltage output through a series integration, successfully powering high-power LEDs and miniature motors. This work introduced an MOF-derived hierarchical porous architecture synergistically integrated with advanced 3D printing, enabling the development of high-performance 3DP-f-QSS Zn-Co batteries specifically engineered for next-generation wearable electronic systems.