Abstract:Achieving high-current-density and high-areacapacity operation of Li metal anodes offers promising opportunities for high-performing next-generation batteries. However, high-rate Li deposition suffers from undesired Liion depletion especially at the electrolyte-anode interface, which compromises achievable capacity and lifetime. Here, electronegative graphene quantum dots are synthesized and assembled into an ultra-thin overlayer capable of efficient Liion adsorbing at the nanoscale on Li-metal to fully reliev… Show more
“…CE performance was first examined in the half-cell configuration assembled by pairing the routine Li metal with D-Cu@CuSe, while B-Cu-and D-Cu-based half cells were also constructed for comparison. [37][38][39] It is interesting to note that an apparent discharge platform can be observed at %0.8 V (vs. Li/Li þ ) during the initial electrochemical activation process (Figure S9, Supporting Information). Correspondingly, the characteristic peaks assigned to Li 2 Se in the XRD pattern further verify the in situ generation of the Li 2 Se protective layer (Figure S10, Supporting Information).…”
Li metal is regarded as one of the most promising anodes for next‐generation rechargeable batteries. Nonetheless, infinite volume change and severe dendrite growth impede its practicability. To date, unremitting efforts have been devoted to stabilizing Li metal anode via the rational design of 3D current collectors. In this sense, optimizing Li nucleation behavior plays a pivotal role in alleviating the dendrite formation. Herein, a practically viable route is devised by in situ crafting lithiophilic CuSe granules on the dealloyed Cu skeleton (D‐Cu@CuSe). Persuasive electrochemical analysis and systematic theoretical calculation disclose the underlying Li nucleation mechanism on the CuSe overlayer. Impressively, the D‐Cu@CuSe‐Li symmetric cell can sustain a stable plating/stripping operation over 1000 h at a high depth of discharge at 62.5%. More crucially, when paired with high‐loading sulfur cathodes, D‐Cu@CuSe‐Li||S batteries harvest advanced areal capacity and stable cycling performance even under stringent working conditions of low negative‐to‐positive (N/P) (≈2) and electrolyte‐to‐sulfur (8 μL mgs−1) ratios. Overall, a fresh perspective into rationalizing current collector design is afforded, which extends Li utilization and cycling durability in the pursuit of pragmatic Li metal anodes.
“…CE performance was first examined in the half-cell configuration assembled by pairing the routine Li metal with D-Cu@CuSe, while B-Cu-and D-Cu-based half cells were also constructed for comparison. [37][38][39] It is interesting to note that an apparent discharge platform can be observed at %0.8 V (vs. Li/Li þ ) during the initial electrochemical activation process (Figure S9, Supporting Information). Correspondingly, the characteristic peaks assigned to Li 2 Se in the XRD pattern further verify the in situ generation of the Li 2 Se protective layer (Figure S10, Supporting Information).…”
Li metal is regarded as one of the most promising anodes for next‐generation rechargeable batteries. Nonetheless, infinite volume change and severe dendrite growth impede its practicability. To date, unremitting efforts have been devoted to stabilizing Li metal anode via the rational design of 3D current collectors. In this sense, optimizing Li nucleation behavior plays a pivotal role in alleviating the dendrite formation. Herein, a practically viable route is devised by in situ crafting lithiophilic CuSe granules on the dealloyed Cu skeleton (D‐Cu@CuSe). Persuasive electrochemical analysis and systematic theoretical calculation disclose the underlying Li nucleation mechanism on the CuSe overlayer. Impressively, the D‐Cu@CuSe‐Li symmetric cell can sustain a stable plating/stripping operation over 1000 h at a high depth of discharge at 62.5%. More crucially, when paired with high‐loading sulfur cathodes, D‐Cu@CuSe‐Li||S batteries harvest advanced areal capacity and stable cycling performance even under stringent working conditions of low negative‐to‐positive (N/P) (≈2) and electrolyte‐to‐sulfur (8 μL mgs−1) ratios. Overall, a fresh perspective into rationalizing current collector design is afforded, which extends Li utilization and cycling durability in the pursuit of pragmatic Li metal anodes.
“…In this regard, we synthesized zero-dimensional quantum-sized graphene dots and then constructed an ultrathin Li + adsorbing layer (LAL) on Li metal surface (Figure 6c, d). [68] The graphene quantum dots exhibited typical sizes of 3-5 nm, and they were comprised of nanocrystalline carbon cores with surface polar functional groups (e. g., À OH, À NH 2 , C=O/C=N, and C=S). This unique quantum-sized graphene dots could localize the sp 2electrons that induced attraction forces toward Li + .…”
Section: Carbonaceous Materialsmentioning
confidence: 99%
“…e) Schematic of the preparation process and design rationale of the graphene quantum dot building blocks for the LAL. Reproduced with permission [68] . Copyright 2021, Wiley‐VCH.…”
Section: Carbonaceous Materialsmentioning
confidence: 99%
“…Reducing the size of carbonaceous building blocks for protective overlayers demonstrates an effective strategy to enhance the Li + diffusion and homogenize Li + distribution. In this regard, we synthesized zero‐dimensional quantum‐sized graphene dots and then constructed an ultrathin Li + adsorbing layer (LAL) on Li metal surface (Figure 6c, d) [68] . The graphene quantum dots exhibited typical sizes of 3‐5 nm, and they were comprised of nanocrystalline carbon cores with surface polar functional groups (e. g., −OH, −NH 2 , C=O/C=N, and C=S).…”
The main limitation of lithium (Li) metal anodes lies in their severe dendrite growth due to nonuniform Li+ flux and sluggish Li+ transportation at the anode surface. Fabricating artificial protective overlayer with tunable surficial properties on Li metal is a precise and effective strategy to relieve this problem. In this Concept article, we focus on the basic principles of regulating interfacial Li+ through artificial protective overlayers and summarize the material preparation as well as structural design of these overlayers. The remaining challenges and promising directions of artificial protective overlayers are then highlighted to provide clues for the practical application of Li metal anodes.
“…Yang et al [ 33 ] reported that 2D MnZnO nanosheets/CNF infused with molten Li maintained 40 h at 50 mA cm −2 and 10 mAh cm −2 . Nevertheless, the modified Li anodes with high areal capacities (> 10 mAh cm −2 ) can only be performed (< 1000 h) at limited current densities (< 10 mA cm −2 ) [ 53 – 55 ]. Therefore, a rational design of lithiophilic material remains unclear for protecting Li metal anode toward practical application (especially at ultrahigh current density and areal capacity).…”
Lithium metal anode has been demonstrated as the most promising anode for lithium batteries because of its high theoretical capacity, but infinite volume change and dendritic growth during Li electrodeposition have prevented its practical applications. Both physical morphology confinement and chemical adsorption/diffusion regulation are two crucial approaches to designing lithiophilic materials to alleviate dendrite of Li metal anode. However, their roles in suppressing dendrite growth for long-life Li anode are not fully understood yet. Herein, three different Ni-based nanosheet arrays (NiO-NS, Ni3N-NS, and Ni5P4-NS) on carbon cloth as proof-of-concept lithiophilic frameworks are proposed for Li metal anodes. The two-dimensional nanoarray is more promising to facilitate uniform Li+ flow and electric field. Compared with the NiO-NS and the Ni5P4-NS, the Ni3N-NS on carbon cloth after reacting with molten Li (Li-Ni/Li3N-NS@CC) can afford the strongest adsorption to Li+ and the most rapid Li+ diffusion path. Therefore, the Li-Ni/Li3N-NS@CC electrode realizes the lowest overpotential and the most excellent electrochemical performance (60 mA cm−2 and 60 mAh cm−2 for 1000 h). Furthermore, a remarkable full battery (LiFePO4||Li-Ni/Li3N-NS@CC) reaches 300 cycles at 2C. This research provides valuable insight into designing dendrite-free alkali metal batteries.
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