A high-performance energy storage device plays an important role in controlling carbon emissions. The emerging additive manufacturing techniques bring a great revolution of electrode fabrication process and promote the performance of energy storage devices through the advanced electrode architecture design. In this paper, recent studies on the three-dimensional (3D)-printed electrode with advanced architecture have been mainly reviewed, including interdigitated structure, through-thickness aligned structure, hierarchical porous structure and fiber and fibric structure of electrodes, and expectations for the development of novel advanced electrode architecture generated and optimized by computational simulation and machine learning.The strategy of advanced electrode architecture design and fabrication enabled by the 3D printing technique represents a promising direction toward future energy storage devices with high electrochemical and mechanical performance.
Future renewable energy supply and a cleaner Earth greatly depend on various crucial catalytic reactions for the society. Atomically dispersed metal site electrocatalysts (ADMSEs) have attracted tremendous research interest and are considered as the next-generation promising oxygen reduction reaction (ORR) electrocatalysts due to the maximum atom utilization efficiency, tailorable catalytic sites, and tunable electronic structures. Despite great efforts have been devoted to the development of ADMSEs, the systematic summary for design principles of high-efficiency ADMSEs is not sufficiently highlighted for ORR. In this review, the authors first summarize the fundamental ORR mechanisms for ADMSEs, and further discuss the intrinsic catalytic mechanism from the perspective of theoretical calculation. Then, the advanced characterization techniques to identify the active sites and effective synthesis methods to prepare catalysts for ADMSEs are also showcased. Subsequently, a special emphasis is placed on effective strategies for the rational design of the advanced ADMSEs. Finally, the present challenges to be addressed in practical application and future research directions are also proposed to overcome the relevant obstacles for developing high-efficiency ORR electrocatalysts. This review aims to provide a deeper understanding for catalytic mechanisms and valuable design principles to obtain the advanced ADMSEs for sustainable energy conversion and storage techniques.
Lithium metal anode holds an important position in fast‐charging batteries. But lithium dendrite issues tend to exacerbate at high currents. LiF can be considered as an effective way to improve the Li metal surface electrochemical stability to achieve high power and high energy. However, most of reported work are relying on in situ formation of a 2D LiF on Li metal in liquid electrolyte, which limits the scalability and plated Li quantity. Here, we address this challenge and report a scalable synthesis of LiF‐rich 3D architected Li metal anode via a direct pyrolysis of molten lithium and fluoropolymer to enable fast Li charging with high current density (20 mA cm−2) and high areal capacity (20 mAh cm−2). The 3D structure is synthesized by the pyrolysis of fluoropolymer with Li metal and results show high similarity to the pristine electrolyte‐derived solid‐electrolyte‐interphase (SEI). This concept using pyrolysis of fluoropolymer with Li‐containing active materials could be also extended to modify Li metal oxide cathode (e.g., LiNi0.5Mn1.5O4) for mixed conductive interphase and engineer Li solid ion conductors (e.g., Li garnet‐type oxides) for interface stabilization and framework design.
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