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Aqueous sodium-ion batteries (ASIBs) represent a promising battery technology for stationary energy storage, due to their attractive merits of low cost, high abundance, and inherent safety. Recently, a variety of advanced cathode, anode, and electrolyte materials have been developed for ASIBs, which not only enhance our fundamental understanding of the Na insertion mechanism, but also facilitate the research and development of practical ASIB systems. Among these electrode materials, iron-based materials are of particular importance because of the high abundance, low price, and low toxicity of Fe elements. However, to our knowledge, there are no review papers that specifically discuss the properties of Fe-based materials for ASIBs yet. In this review, we present the recent research progress on Fe-based cathode/anode materials, which include polyanionic compounds, Prussian blue, oxides, carbides, and selenides. We also discuss the research efforts to build Fe-based ASIB full cells. Lastly, we share our perspectives on the key challenges that need to be addressed and suggest alternative directions for aqueous Na-ion batteries. We hope this review paper can promote more research efforts on the development of low-cost and low-toxicity materials for aqueous battery applications. 

Despite the various strategies for achieving metal–nitrogen–carbon (M–N–C) single-atom catalysts (SACs) with different microenvironments for electrochemical carbon dioxide reduction reaction (CO 2 RR), the synthesis–structure–performance correlation remains elusive due to the lack of well-controlled synthetic approaches. Here, we employed Ni nanoparticles as starting materials for the direct synthesis of nickel (Ni) SACs in one spot through harvesting the interaction between metallic Ni and N atoms in the precursor during the chemical vapor deposition growth of hierarchical N-doped graphene fibers. By combining with first-principle calculations, we found that the Ni-N configuration is closely correlated to the N contents in the precursor, in which the acetonitrile with a high N/C ratio favors the formation of Ni-N 3 , while the pyridine with a low N/C ratio is more likely to promote the evolution of Ni-N 2 . Moreover, we revealed that the presence of N favors the formation of H-terminated edge of sp 2 carbon and consequently leads to the formation of graphene fibers consisting of vertically stacked graphene flakes, instead of the traditional growth of carbon nanotubes on Ni nanoparticles. With a high capability in balancing the *COOH formation and *CO desorption, the as-prepared hierarchical N-doped graphene nanofibers with Ni-N 3 sites exhibit a superior CO 2 RR performance compared to that with Ni-N 2 and Ni-N 4 ones. 

Aqueous zinc-ion batteries, in terms of integration with high safety, environmental benignity, and low cost, have attracted much attention for powering electronic devices and storage systems. However, the interface instability issues at the Zn anode caused by detrimental side reactions such as dendrite growth, hydrogen evolution, and metal corrosion at the solid (anode)/liquid (electrolyte) interface impede their practical applications in the fields requiring long-term performance persistence. Despite the rapid progress in suppressing the side reactions at the materials interface, the mechanism of ion storage and dendrite formation in practical aqueous zinc-ion batteries with dual-cation aqueous electrolytes is still unclear. Herein, we design an interface material consisting of forest-like three-dimensional zinc-copper alloy with engineered surfaces to explore the Zn plating/stripping mode in dual-cation electrolytes. The three-dimensional nanostructured surface of zinc-copper alloy is demonstrated to be in favor of effectively regulating the reaction kinetics of Zn plating/stripping processes. The developed interface materials suppress the dendrite growth on the anode surface towards high-performance persistent aqueous zinc-ion batteries in the aqueous electrolytes containing single and dual cations. This work remarkably enhances the fundamental understanding of dual-cation intercalation chemistry in aqueous electrochemical systems and provides a guide for exploring high-performance aqueous zinc-ion batteries and beyond.

 

Electrochemical energy systems such as batteries, water electrolyzers, and fuel cells are considered as promising and sustainable energy storage and conversion devices due to their high energy densities and zero or negative carbon dioxide emission. However, their widespread applications are hindered by many technical challenges, such as the low efficiency and poor long-term cyclability, which are mostly affected by the changes at the reactant/electrode/electrolyte interfaces. These interfacial processes involve ion/electron transfer, molecular/ion adsorption/desorption, and complex interface restructuring, which lead to irreversible modifications to the electrodes and the electrolyte. The understanding of these interfacial processes is thus crucial to provide strategies for solving those problems. In this review, we will discuss different interfacial processes at three representative interfaces, namely, solid–gas, solid–liquid, and solid–solid, in various electrochemical energy systems, and how they could influence the performance of electrochemical systems. 

Abstract Developing efficient catalysts is of paramount importance to oxygen evolution, a sluggish anodic reaction that provides essential electrons and protons for various electrochemical processes, such as hydrogen generation. Here, we report that the oxygen evolution reaction (OER) can be efficiently catalyzed by cobalt tetrahedra, which are stabilized over the surface of a Swedenborgite-type YBCo 4 O 7 material. We reveal that the surface of YBaCo 4 O 7 possesses strong resilience towards structural amorphization during OER, which originates from its distinctive structural evolution toward electrochemical oxidation. The bulk of YBaCo 4 O 7 composes of corner-sharing only CoO 4 tetrahedra, which can flexibly alter their positions to accommodate the insertion of interstitial oxygen ions and mediate the stress during the electrochemical oxidation. The density functional theory calculations demonstrate that the OER is efficiently catalyzed by a binuclear active site of dual corner-shared cobalt tetrahedra, which have a coordination number switching between 3 and 4 during the reaction. We expect that the reported active structural motif of dual corner-shared cobalt tetrahedra in this study could enable further development of compounds for catalyzing the OER.