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  1. Abstract

    Oxygen reduction reaction (ORR) is an electrochemical reaction in which dissolved oxygen in an electrolyte is reduced to OH/H2O when receiving electrons. This reaction plays a crucial role in shaping the efficiency of both metal–air batteries and fuel cells, and precious metals are the dominant catalysts carrying out the ORR in their cathodes. However, how to manipulate the electronic structure of precious metals as active sites to further promote ORR performance and maximize the utilization rate is still under development. Metal oxide serves as suitable and promising support that can strongly interact with precious metals for both activity and durability enhancement. Herein, we present recent research updates on strong precious metal–metal oxide interaction (SPMMOI) utilized in ORR. We start by introducing the background of ORR, the issues to be solved, and its practical applications followed by a thorough discussion of the reaction mechanism and comprehensive evaluation protocols of performance. We then provide a complete understanding of the working principle of SPMMOI and highlight the related advances. Finally, we summarize the merits of the precious metal–metal oxide system and propose the research direction as well as some urgent problems to be addressed in the future.

     
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  2. Abstract

    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.

     
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  3. Abstract

    Uncontrollable dendrite growth is closely related to non‐uniform reaction environments. However, there is a lack of understanding and analysis methods to probe the localized electrochemical environment (LEE). Here the effects of the LEE are investigated, including localized ion concentrations, current density, and electric potential, on metal plating/stripping dynamics and dendrite minimization. A novel in situ 3D microscopy technique is developed to image the morphology dynamics and deposition rate of Zn plating/stripping processes on 3D Zn–Mn anodes. Using the in situ 3D microscope, the electrode morphology changes during the reactions are directly imaged and Zn deposition rate maps at different time points are obtained. It is found that reaction kinetics are highly correlated to LEE and electrode morphology. To further quantify the LEE effects, the digital twin technique is employed that allows the accurate calculation of the electrochemical environments, such as localized ion concentrations, current density, and electric potential, which cannot be directly measured from experiments. It is found that the curvature of the 3D electrode surface determines the LEE and significantly influences reaction kinetics. This provides a new strategy to minimize the dendrite formation by designing and optimizing the 3D geometry of the electrode to control the LEE.

     
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  4. Abstract

    Metal anode instability, including dendrite growth, metal corrosion, and hetero-ions interference, occurring at the electrolyte/electrode interface of aqueous batteries, are among the most critical issues hindering their widespread use in energy storage. Herein, a universal strategy is proposed to overcome the anode instability issues by rationally designing alloyed materials, using Zn-M alloys as model systems (M = Mn and other transition metals). An in-situ optical visualization coupled with finite element analysis is utilized to mimic actual electrochemical environments analogous to the actual aqueous batteries and analyze the complex electrochemical behaviors. The Zn-Mn alloy anodes achieved stability over thousands of cycles even under harsh electrochemical conditions, including testing in seawater-based aqueous electrolytes and using a high current density of 80 mA cm−2. The proposed design strategy and the in-situ visualization protocol for the observation of dendrite growth set up a new milestone in developing durable electrodes for aqueous batteries and beyond.

     
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  5. Abstract

    The metallic tin (Sn) anode is a promising candidate for next‐generation lithium‐ion batteries (LIBs) due to its high theoretical capacity and electrical conductivity. However, Sn suffers from severe mechanical degradation caused by large volume changes during lithiation/delithiation, which leads to a rapid capacity decay for LIBs application. Herein, a Cu–Sn (e.g., Cu3Sn) intermetallic coating layer (ICL) is rationally designed to stabilize Sn through a structural reconstruction mechanism. The low activity of the Cu–Sn ICL against lithiation/delithiation enables the gradual separation of the metallic Cu phase from the Cu–Sn ICL, which provides a regulatable and appropriate distribution of Cu to buffer volume change of Sn anode. Concurrently, the homogeneous distribution of the separated Sn together with Cu promotes uniform lithiation/delithiation, mitigating the internal stress. In addition, the residual rigid Cu–Sn intermetallic shows terrific mechanical integrity that resists the plastic deformation during the lithiation/delithiation. As a result, the Sn anode enhanced by the Cu–Sn ICL shows a significant improvement in cycling stability with a dramatically reduced capacity decay rate of 0.03% per cycle for 1000 cycles. The structural reconstruction mechanism in this work shines a light on new materials and structural design that can stabilize high‐performance and high‐volume‐change electrodes for rechargeable batteries and beyond.

     
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  6. Free, publicly-accessible full text available February 21, 2025
  7. Free, publicly-accessible full text available January 1, 2025
  8. Free, publicly-accessible full text available August 14, 2024
  9. Free, publicly-accessible full text available June 1, 2024
  10. This review revisits critical descriptors to assess the performance of Zn–air batteries. The recent progress of inorganic nanoporous metal films as self-standing air electrodesfor Zn–air batteries is systematically summarized and analyzed.

     
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    Free, publicly-accessible full text available May 11, 2024