Aqueous zinc-ion batteries have drawn increasing attention due to the intrinsic safety, costeffectiveness and high energy density. However, parasitic reactions and non-uniform dendrite growth on the Zn anode side impede their application. Herein, a multifunctional additive, ammonium dihydrogen phosphate (NHP), is introduced to regulate uniform zinc deposition and to suppress side reactions. The results show that the NH 4 + tends to be preferably absorbed on the Zn surface to form a "shielding effect" and blocks the direct contact of water with Zn. Moreover, NH 4 + and (H 2 PO 4 ) À jointly maintain pH values of the electrode-electrolyte interface. Consequently, the NHP additive enables highly reversible Zn plating/stripping behaviors in Zn//Zn and Zn//Cu cells. Furthermore, the electrochemical performances of Zn//MnO 2 full cells and Zn//active carbon (AC) capacitors are improved. This work provides an efficient and general strategy for modifying Zn plating/stripping behaviors and suppressing side reactions in mild aqueous electrolyte.

Theoretical calculations unveil that the formation of Os‐OsSe2 heterostructures with neutralized work function (WF) perfectly balances the electronic state between strong (Os) and weak (OsSe2) adsorbents and bidirectionally optimizes the hydrogen evolution reaction (HER) activity of Os sites, significantly reducing thermodynamic energy barrier and accelerating kinetics process. Then, heterostructural Os‐OsSe2 is constructed for the first time by a molten salt method and confirmed by in‐depth structural characterization. Impressively, due to highly active sites endowed by the charge balance effect, Os‐OsSe2 exhibits ultra‐low overpotentials for HER in both acidic (26 mV @ 10 mA cm−2) and alkaline (23 mV @ 10 mA cm−2) media, surpassing commercial Pt catalysts. Moreover, the solar‐to‐hydrogen device assembled with Os‐OsSe2 further highlights its potential application prospects. Profoundly, this special heterostructure provides a new model for rational selection of heterocomponents.

Aqueous zinc‐ion batteries are highly desirable for large‐scale energy storage because of their low cost and high‐level safety. However, achieving high energy and high power densities simultaneously is challenging. Herein, a VOx sub‐nanometer cluster/reduced graphene oxide (rGO) cathode material composed of interfacial VOC bonds is artificially constructed. Therein, a new mechanism is revealed, where Zn2+ ions are predominantly stored at the interface between VOx and rGO, which causes anomalous valence changes compared to conventional mechanisms and exploits the storage ability of non‐energy‐storing active yet highly conductive rGO. Further, this interface‐dominated storage triggers decoupled transport of electrons/Zn2+ ions, and the reversible destruction/reconstruction allows the interface to store more ions than the bulk. Finally, an ultrahigh rate capability (174.4 mAh g−1 at 100 A g−1, i.e., capacity retention of 39.4% for a 1000‐fold increase in current density) and a high capacity (443 mAh g−1 at 100 mA g−1, exceeding the theoretical capacities of each interfacial component) are achieved. Such interface‐dominated storage is an exciting way to build high‐energy‐ and high‐power‐density devices.

Conversion-type anodes with multielectron reactions are beneficial for achieving a high capacity in sodium-ion batteries. Enhancing the electron/ion conductivity and structural stability are two key challenges in the development of high-performance sodium storage. Herein, a novel multidimensionally assembled nanoarchitecture is presented, which consists of V O nanoparticles embedded in amorphous carbon nanotubes that are then coassembled within a reduced graphene oxide (rGO) network, this materials is denoted V O ⊂C-NTs⊂rGO. The selective insertion and multiphase conversion mechanism of V O in sodium-ion storage is systematically demonstrated for the first time. Importantly, the naturally integrated advantages of each subunit synergistically provide a robust structure and rapid electron/ion transport, as confirmed by in situ and ex situ transmission electron microscopy experiments and kinetic analysis. Benefiting from the synergistic effects, the V O ⊂C-NTs⊂rGO anode delivers an ultralong cycle life (72.3% at 5 A g after 15 000 cycles) and an ultrahigh rate capability (165 mAh g at 20 A g , ≈30 s per charge/discharge). The synergistic design of the multidimensionally assembled nanoarchitecture produces superior advantages in energy storage.

Routine electrolyte additives are not effective enough for uniform zinc (Zn) deposition, because they are hard to proactively guide atomic-level Zn deposition. Here, based on underpotential deposition (UPD), we propose an "escort effect" of electrolyte additives for uniform Zn deposition at the atomic level. With nickel ion (Ni 2 + ) additives, we found that metallic Ni deposits preferentially and triggers the UPD of Zn on Ni. This facilitates firm nucleation and uniform growth of Zn while suppressing side reactions. Besides, Ni dissolves back into the electrolyte after Zn stripping with no influence on interfacial charge transfer resistance. Consequently, the optimized cell operates for over 900 h at 1 mA cm À 2 (more than 4 times longer than the blank one). Moreover, the universality of "escort effect" is identified by using Cr 3 + and Co 2 + additives. This work would inspire a wide range of atomic-level principles by controlling interfacial electrochemistry for various metal batteries.