Zn Powder Anodes With Stabilized Interfacial Chemistry via Facet-Selective ZnTCPP Adsorption for Aqueous Zn-Ion...

Zn powder anodes are regarded as promising alternatives to Zn foil for the scalable fabrication of aqueous Zn-ion batteries, yet their large specific surface area inevitably induces severe interfacial instability, including uncontrolled dendrite growth and aggravated parasitic reactions. Herein, a porphyrin-based metal-organic framework ZnTCPP is in situ constructed on Zn powder to engineer both surface crystallography and interfacial chemistry. Benefiting from its facet-selective adsorption behavior, the ZnTCPP preferentially anchors onto the Zn(101) and Zn(100) facets, thereby thermodynamically suppressing their participation in Zn deposition. Meanwhile, the porphyrin ligands serve as effective Zn²⁺ affinity centers that homogenize Zn²⁺ flux and redirect Zn nucleation toward the low-energy Zn(002) plane, enabling compact and dendrite-free Zn growth. Moreover, the ZnTCPP layer promotes the desolvation of hydrated Zn²⁺ at the electrode surface and mitigates interfacial side reactions, leading to a stabilized Zn-electrolyte interface. Consequently, the ZnTCPP-modified Zn powder anode exhibits significantly enhanced electrochemical reversibility and durability, delivering an average Coulombic efficiency of 99.7%, maintaining stable plating/stripping behavior for over 500 h, and supporting high critical current densities up to 500 mA g^-1. Furthermore, full cells assembled with the modified anode demonstrate superior cycling stability and rate capability compared with those using the pristine Zn powder anode.