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Among various charge‐carrier ions for aqueous batteries, non‐metal hydronium (H3O+) with small ionic size and fast diffusion kinetics empowers H3O+‐intercalation electrodes with high rate performance and fast‐charging capability. However, pure H3O+ charge carriers for inorganic electrode materials have only been observed in corrosive acidic electrolytes, rather than in mild neutral electrolytes. Herein, we report how selective H3O+ intercalation in a neutral ZnCl2 electrolyte can be achieved for water‐proton co‐intercalated α‐MoO3 (denoted WP‐MoO3). H2O molecules located between MoO3 interlayers block Zn2+ intercalation pathways while allowing smooth H3O+ intercalation/diffusion through a Grotthuss proton‐conduction mechanism. Compared to α‐MoO3 with a Zn2+‐intercalation mechanism, WP‐MoO3 delivers the substantially enhanced specific capacity (356.8 vs. 184.0 mA h g−1), rate capability (77.5 % vs. 42.2 % from 0.4 to 4.8 A g−1), and cycling stability (83 % vs. 13 % over 1000 cycles). This work demonstrates the possibility of modulating electrochemical intercalating ions by interlayer engineering, to construct high‐rate and long‐life electrodes for aqueous batteries. [ABSTRACT FROM AUTHOR]

Among various charge‐carrier ions for aqueous batteries, non‐metal hydronium (H3O+) with small ionic size and fast diffusion kinetics empowers H3O+‐intercalation electrodes with high rate performance and fast‐charging capability. However, pure H3O+ charge carriers for inorganic electrode materials have only been observed in corrosive acidic electrolytes, rather than in mild neutral electrolytes. Herein, we report how selective H3O+ intercalation in a neutral ZnCl2 electrolyte can be achieved for water‐proton co‐intercalated α‐MoO3 (denoted WP‐MoO3). H2O molecules located between MoO3 interlayers block Zn2+ intercalation pathways while allowing smooth H3O+ intercalation/diffusion through a Grotthuss proton‐conduction mechanism. Compared to α‐MoO3 with a Zn2+‐intercalation mechanism, WP‐MoO3 delivers the substantially enhanced specific capacity (356.8 vs. 184.0 mA h g−1), rate capability (77.5 % vs. 42.2 % from 0.4 to 4.8 A g−1), and cycling stability (83 % vs. 13 % over 1000 cycles). This work demonstrates the possibility of modulating electrochemical intercalating ions by interlayer engineering, to construct high‐rate and long‐life electrodes for aqueous batteries. [ABSTRACT FROM AUTHOR]