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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 (Ni2+ ) 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-2 (more than 4 times longer than the blank one). Moreover, the universality of "escort effect" is identified by using Cr3+ and Co2+ additives. This work would inspire a wide range of atomic-level principles by controlling interfacial electrochemistry for various metal batteries.

The corrosion, parasitic reactions, and aggravated dendrite growth severely restrict development of aqueous Zn-ion batteries. Here, we report a novel strategy to break the hydrogen bond network between water molecules and construct the sulfolane-H2O deep eutectic solvents. This strategy cuts off the transfer of protons/hydroxides and inhibits the activity of H2O, as reflected in a much lower freezing point (-80 °C), a significantly larger electrochemical stable window (3 V), and suppressed evaporative water from electrolytes. Stable Zn plating/stripping for over 9600 h was obtained. Based on experimental characterizations and theoretical simulations, it has been proved that sulfolane can effectively regulate solvation shell and simultaneously build the multifunctional Zn-electrolyte interface. Moreover, the multi-layer homemade modular cell and 1.32 Ah pouch cell further confirm its prospect for practical application.

Increasing the energy density of electrochemical double layer capacitors (EDLCs) can broaden their applications in energy storage but remains a formidable challenge. Herein, micropore-rich yolk-shell structured N-doped carbon spheres (YSNCSs) were constructed by a one-pot surfactant-free self-assembly method in aqueous solution. The resultant YSNCSs after activation possessed an ultrahigh surface area of 2536 m2 g-1 , among which 80 % was contributed from micropores. When applied in EDLCs, the activated YSNCSs demonstrated an unprecedentedly high capacitance (270 F g-1 at 1 A g-1 ) in 1-ethyl-3-methylimidazolium tetrafluoroborate ([EMIM][BF4 ]) ionic liquid, affording an ultrahigh energy density (133 Wh kg-1 at 943 W kg-1 ). The present contribution provides insight into engineering porous carbons for capacitive energy storage.

The unsatisfactory conductivity and large volume variation severely handicap the application of SnO(2)in sodium-ion batteries (SIBs). Herein, we design unique three-layer structured SnO2@C@TiO(2)hollow spheres to tackle the above-mentioned issues. The hollow cavity affords empty space to accommodate the volume variation of SnO2, while the C and TiO(2)protecting shells strengthen the structural integrity and enhances the electrical conductivity. As a result, the three-layer structured SnO2@C@TiO(2)hollow spheres demonstrate enhanced Na storage performances. The SnO2@C@TiO(2)manifests a reversible capacity two times to that of pristine SnO(2)hollow spheres. In addition,Ex situXRD reveals highly reversible alloying and conversion reactions in SnO2@C@TiO(2)hollow spheres. This study suggests the introduction of a hollow cavity and robust protecting shells is a promising strategy for constructing SIB anode materials.

The next best thing: In this Editorial, we present the body of work of this Special Collection, which aims at highlighting the dynamic research environment surrounding the next-generation electrochemical energy storage technologies, bringing together the latest research conducted on “beyond lithium-ion batteries”. It was about thirty years ago, with the first successful commercialization of lithium-ion batteries (LIBs), that a new era begun. These new electrochemical energy storage systems were about to transform the way society communicates, moves, and lives. The journey that led to this success started back in the early 70s until the mid 1980 paving the way for LIBs commercialization in 1991.1 LIBs undoubtably represent the most successful example of secondary battery. Their importance is reflected in the 2019 Nobel Prize for Chemistry awarded to Dr. Yoshino, Prof. Whittingham, and Prof. Goodenough for their pioneering work toward the development of the LIB technology.2

The electrochemical reduction of CO2 to hydrocarbons involves a multistep proton-coupled electron transfer (PCET) reaction. Second coordination sphere engineering is reported to be effective in the PCET process; however, little is known about the actual catalytic active sites under realistic operating conditions. We have designed a defect-containing metal-organic framework, HKUST-1, through a facile "atomized trimesic acid" strategy, in which Cu atoms are modified by unsaturated carboxylate ligands, producing coordinatively unsaturated Cu paddle wheel (CU-CPW) clusters. We investigate the dynamic behavior of the CU-CPW during electrochemical reconstruction through the comprehensive analysis of in situ characterization results. It is demonstrated that Cu2 (HCOO)3 is maintained after electrochemical reconstruction and that is behaves as an active site. Mechanistic studies reveal that CU-CPW accelerates the proton-coupled multi-electron transfer (PCMET) reaction, resulting in a deep CO2 reduction reaction.

It is extremely desirable to explore high-efficient, affordable and robust oxygen electrocatalysts toward rechargeable Zn-air batteries (ZABs). A 3D porous nitrogen-doped graphene encapsulated metallic Ni3 Fe alloy nanoparticles aerogel (Ni3 Fe-GA1 ) was constructed through a facile hydrothermal assembly and calcination process. Benefiting from 3D porous configuration with great accessibility, high electrical conductivity, abundant active sites, optimal nitrogen content and strong electronic interactions at the Ni3 Fe/N-doped graphene heterointerface, the obtained aerogel showed outstanding catalytic performance toward the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR). Specifically, it exhibited an overpotential of 239 mV to attain 10 mA cm-2 for OER, simultaneously providing a positive onset potential of 0.93 V within a half-wave potential of 0.8 V for ORR. Accordingly, when employed in the aqueous ZABs, Ni3 Fe-GA1 achieved higher power density and superior reversibility than Pt/C-IrO2 catalyst, making it a potential candidate for rechargeable ZABs.

Tuning the uniformity and size of binary metal oxide nanodots on graphene oxide (BMO NDs@GO) is significant but full of challenges in wet-chemistry, owing to the difficulties of controlling the complicated cation/anion co-adsorption, heterogeneous nucleation, and overgrowth processes. Herein, the aim is to tune these processes by understanding the functions of various alcohol solvents for NDs growth on GO. It is found that the polyol solvation effect is beneficial for obtaining highly uniform BMO NDs@GO. Polyol shell capped metal ions exhibit stronger hydrogen-bond interactions with the GO surface, leading to a uniform cation/anion co-adsorption and followed heterogeneous nucleation. The polyol-solvated ions with large diffusion energy barrier drastically limit the ion diffusion kinetics in liquids and at the solid/liquid interface, resulting in a slow and controllable growth. Moreover, the synthesis in polyol systems is highly controllable and universal, thus eleven BMO and polynary metal oxide NDs@GO are obtained by this method. The synthetic strategy provides improved prospects for the manufacture of inorganic NDs and their expanding electrochemical applications.

Rationally designed catalysts hold the key to address the sluggish kinetics of oxygen evolution reaction (OER). However, engineering the active sites of such catalysts still faces grand challenges. This study proposes a feasible ligand modulation strategy to boost the OER catalytic activity of cobalt-iron oxyhydroxide ((Fe,Co)OOH). The 2-methylimidazole (MI) ligand coordination on (Fe,Co)OOH reduces the orbital overlap between the Fe/Co 3d and O 2p, which weakens the adsorption to oxygen-containing intermediates and thus facilitates the unfavorable O