Mitigating Intraphase Catalytic‐Domain Transfer via CO₂ Laser for Enhanced Nitrate‐to‐Ammonia Electroconversion and Zn‐Nitrate Battery Behavior

Developing sustainable energy solutions is critical for addressing the dual challenges of energy demand and environmental impact. In this study, a zinc‐nitrate (Zn−NO 3 − ) battery system was designed for the simultaneous production of ammonia (NH 3 ) via the electrocatalytic NO 3 − reduction reaction (NO 3 RR) and electricity generation. Continuous wave CO 2 laser irradiation yielded precisely controlled CoFe 2 O 4 @nitrogen‐doped carbon (CoFe 2 O 4 @NC) hollow nanocubes from CoFe Prussian blue analogs (CoFe‐PBA) as the integral electrocatalyst for NO 3 RR in 1.0 M KOH, achieving a remarkable NH 4 + production rate of 10.9 mg h −1 cm −2 at −0.47 V versus Reversible Hydrogen Electrode with exceptional stability. In situ and ex situ methods revealed that the CoFe 2 O 4 @NC surface transformed into high‐valent Fe/CoOOH active species, optimizing the adsorption energy of NO 3 RR (*NO 2 and *NO species) intermediates. Furthermore, density functional theory calculations validated the possible NO 3 RR pathway on CoFe 2 O 4 @NC starting with NO 3 − conversion to *NO 2 intermediates, followed by reduction to *NO. Subsequent protonation forms the *NH and *NH 2 species, leading to NH 3 formation via final protonation. The Zn−NO 3 − battery utilizing the CoFe 2 O 4 @NC cathode exhibits dual functionality by generating electricity with a stable open‐circuit voltage of 1.38 V versus Zn/Zn 2+ and producing NH 3 . This study highlights the innovative use of CO 2 laser irradiation to transform Prussian blue analogs into cost‐effective catalysts with hierarchical structures for NO 3 RR‐to‐NH 3 conversion, positioning the Zn−NO 3 − battery as a promising technology for industrial applications.