Zn metal anode has garnered growing scientific and industrial interest owing to its appropriate redox potential, low cost, and high safety. Nevertheless, the instability of Zn anode caused by dendrite formation, hydrogen evolution, and side reactions has greatly hampered its commercialization. Herein, an in situ grown ZnSe overlayer is crafted over one side of commercial Zn foil via chemical vapor deposition in a scalable manner, aiming to achieve optimized electrolyte/Zn interfaces with large‐scale viability. Impressively, thus‐derived ZnSe coating functions as a cultivator to guide oriented growth of Zn (002) plane at the infancy stage of stripping/plating cycles, thereby inhibiting the formation of Zn dendrites and the occurrence of side reactions. As a result, high cyclic stability (1530 h at 1.0 mA cm−2/1.0 mAh cm−2; 172 h at 30.0 mA cm−2/10.0 mAh cm−2) in symmetric cells is harvested. Meanwhile, when paired with V2O5 based cathode, assembled full cell achieves an outstanding capacity (194.5 mAh g−1) and elongated lifespan (a capacity retention of 84% after 1000 cycles) at 5.0 A g−1. The reversible Zn anode enabled by the interfacial manipulation strategy via ZnSe cultivator is anticipated to satisfy the demand of commercial use.
Lithium–sulfur (Li–S) batteries are promising candidates for next‐generation energy storage, yet they are plagued by the notorious polysulfide shuttle effect and sluggish redox kinetics. While rationally designed redox mediators can facilitate polysulfide conversion, favorable bidirectional sulfur electrocatalysis remains a formidable challenge. Herein, selective dual‐defect engineering (i.e., introducing both N‐doping and Se‐vacancies) of a common MoSe2 electrocatalyst is used to manipulate the bidirectional Li2S redox. Systematic theoretical prediction and detailed electrokinetic analysis reveal the selective electrocatalytic effect of the two types of defects, thereby achieving a deeper mechanistic understanding of the bidirectional sulfur electrochemistry. The Li–S battery using this electrocatalyst exhibits excellent cyclability, with a low capacity decay rate of 0.04% per cycle over 1000 cycles at 2.0 C. More impressively, the potential for practical applications is highlighted by a high areal capacity (7.3 mAh cm−2) and the construction of a flexible pouch cell. Such selective electrocatalysis created by dual‐defect engineering is an appealing approach toward working Li–S systems.
Using the ultrafast pump-probe transient absorption spectroscopy, the femtosecond-resolved plasmon-exciton interaction of graphene-Ag nanowire hybrids is experimentally investigated, in the VIS-NIR region. The plasmonic lifetime of Ag nanowire is about 150 ± 7 femtosecond (fs). For a single layer of graphene, the fast dynamic process at 275 ± 77 fs is due to the excitation of graphene excitons, and the slow process at 1.4 ± 0.3 picosecond (ps) is due to the plasmonic hot electron interaction with phonons of graphene. For the graphene-Ag nanowire hybrids, the time scale of the plasmon-induced hot electron transferring to graphene is 534 ± 108 fs, and the metal plasmon enhanced graphene plasmon is about 3.2 ± 0.8 ps in the VIS region. The graphene-Ag nanowire hybrids can be used for plasmon-driven chemical reactions. This graphene-mediated surface-enhanced Raman scattering substrate significantly increases the probability and efficiency of surface catalytic reactions co-driven by graphene-Ag nanowire hybridization, in comparison with reactions individually driven by monolayer graphene or single Ag nanowire. This implies that the graphene-Ag nanowire hybrids can not only lead to a significant accumulation of high-density hot electrons, but also significantly increase the plasmon-to-electron conversion efficiency, due to strong plasmon-exciton coupling.
Witnessingc ompositional evolution and identifying the catalytically active moiety of electrocatalysts is of paramount importance in Li-S chemistry.N evertheless,t his field remains elusive.Wereport the scalable salt-templated synthesis of Se-vacancy-incorporated MoSe 2 architecture (SeVs-MoSe 2 ) and reveal the phase evolution of the defective precatalyst in working Li-S batteries.T he interaction between lithium polysulfides and SeVs-MoSe 2 is probed to induce the transformation from SeVs-MoSe 2 to MoSeS.F urthermore,o perando Raman spectroscopya nd ex situ X-rayd iffraction measurements in combination with theoretical simulations verify that the effectual MoSeS catalyst could help promote conversion of Li 2 S 2 to Li 2 S, thereby boosting the capacity performance.The Li-S battery accordingly exhibits asatisfactory rate and cycling capability even with and elevated sulfur loading and lean electrolyte conditions (7.67 mg cm À2 ; 4.0 mLmg À1 S ). This work elucidates the design strategies and catalytic mechanisms of efficient electrocatalysts bearing defects.
Separator modification has recently blossomed as an effective strategy to enable dendrite‐free Zn metal anodes. Nonetheless, the explored avenues are not conducive to mass production by far, and little attention is paid to the essence of separator regulation. Herein, a scalable Ti3C2Tx MXene‐decorated Janus separator is designed by spray‐printing MXene nanosheets over one side of commercial glass fibre (GF). The thus‐derived MXene‐GF separator affords abundant surface polar groups, good electrolyte wettability, and high ionic conductivity, which is beneficial to homogenizing local current distribution and promoting Zn nucleation kinetics. It is noted that MXene‐GF displays adjustable dielectric constants with an optimized value of 53.5, offering a directional electrical field to expedite Zn‐ion flux and repel anions. Accordingly, dendrite‐free Zn anode equipped within symmetric cells can be achieved with MXene‐GF, enabling a stable cycling for 1180 h at 1 mA cm−2 and 1200 h at 5 mA cm−2. More impressively, the assembled aqueous Zn‐ion battery full cell with Janus MXene‐GF separator realizes a favorable capacity retention ratio (77.9%) upon cycling for 1000 cycles at 5.0 A g−1. This strategy with scalability and effectiveness offers a new insight into high‐performance metal anodes.
The burgeoning Li‐ion battery is regarded as a powerful energy storage system by virtue of its high energy density. However, inescapable issues concerning safety and cost aspects retard its prospect in certain application scenarios. Accordingly, strenuous efforts have been devoted to the development of the emerging aqueous Zn‐ion battery (AZIB) as an alternative to inflammable organic batteries. In particular, the instability from the anode side severely impedes the commercialization of AZIB. Constructing an artificial interphase layer (AIL) has been widely employed as an effective strategy to stabilize the Zn anode. This review specializes in the state‐of‐the‐art of AIL design for Zn anode protection, encompassing the preparation methods, mechanism investigations, and device performances based on the classification of functional materials. To begin with, the origins of Zn instability are interpreted from the perspective of electrical field, mass transfer, and nucleation process, followed by a comprehensive summary with respect to functions of AIL and its designing criteria. In the end, current challenges and future outlooks based upon theoretical and experimental considerations are included.
Recent years have witnessed the renaissance of aqueous Zn-ion batteries (AZIBs). Nevertheless, current development of high-performance AZIBs is confronted by rapid capacity decay and irreversible cycling of Zn anodes, whose...
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