Long-Life Dendrite-Free Lithium Metal Electrode Achieved by Constructing a Single Metal Atom Anchored in a Diffusion Modulator Layer

Abstract

Lithium metal electrodes have shown great promise for high capacity and the lowest potential. However, wide application is restricted by uncontrollable plating/stripping lithium behaviors, an uneven solid electrolyte interphase, and a lithium dendrite. Herein, the highly active single metal atom anchored in vacant catalyst is synthesized on the hierarchical porous nanocarbon (SACo/ADFS@HPSC). Acting as an artificial protective modulation layer on the lithium surface, the numerous atomic sites show the superiority in modulating lithium ion behaviors and smoothing the lithium surface without dendrite growth. As a consequence, the SACo/ADFS@HPSC-modified Li electrode lowers nucleation barrier (15 mV), extends the smooth plating lifespan (1600 h), and improves Coulombic efficiency, significantly accelerating the horizonal deposition of plated lithium. Coupled with a sulfur cathode, the fabricated pouch cell with 5.4 mg cm −2 delivers a high capacity of 3.78 mA h cm −2 corresponding to 1505 Wh kg −1 , showing the promising practical application.

Insulative Ion-Conducting Lithium Selenide as the Artificial Solid–Electrolyte Interface Enabling Heavy-Duty Lithium Metal Operations

“…By contrast, the BL electrode exhibited severe voltage fluctuations, possibly due to the poor ionic conductivity of natural SEI formed on the BL surface . We note that with respect to the cycling stability at extreme working conditions, LLS-710 outperforms most of the reported Li metal anodes comprising artificial SEI layers (Figure e). ,− Taken together, the observations made here strongly endorse the potential applications of LLS in heavy-duty conditions.…”

Isolated Single-Atom Ni–N5 Catalytic Site in Hollow Porous Carbon Capsules for Efficient Lithium–Sulfur Batteries

“…In addition, no other peaks related to metallic Ni or other Ni compounds are observed in the Ni–N 5 /HNPC sample, demonstrating the single-atom nature of Ni. Raman spectroscopy (Figure S7) implies an enrichment of defective graphene in Ni–N 5 /HNPC, which is ascribed to the N dopants in the carbon structure and the embedded single-atom Ni in the sample. − In addition, the Ni–N 5 /HNPC sample has a large Brunauer–Emmett–Teller (BET) surface area of 467 m 2 g –1 , a broadening pore size distribution, and a pore volume of 0.65 cm 3 g –1 (Figure S8). The high porosity of Ni–N 5 /HNPC is expected, and its large surface area can offer more active interfaces for sulfur conversion reactions; furthermore, the abundance of hierarchical pores can afford sufficient space to host sulfur particles, thereby enhancing LiPSs trapping, accelerating the ion transport, and improving the sulfur utilization of the sulfur electrode. ,, …”

Electrochemical Kinetic Modulators in Lithium–Sulfur Batteries: From Defect‐Rich Catalysts to Single Atomic Catalysts

“…Apart from the high‐energy barriers in both SRRs and SORs in sulfur cathode, the uncontrollable plating lithium behaviors also will result in uneven surface and lithium dendrite growth, which hampers the commercial viability of Li–S batteries. [ 35,165 ] Constructing artificial solid electrolyte interphase on lithium surface or introducing electrolyte additives can significantly prolong the lifespan of lithium. However, the uncontrollable lithium‐ion behavior may be responsible for inducing lithium dendrite growth.…”

“…Recently, a novel synthesized strategy of using defected sites to anchor single atomic catalyst (SACs‐in‐defects) was proposed and reported by our groups. [ 35 ] Briefly, the highly active single cobalt atoms are anchored in vacant‐rich iron sulfide nanoparticle catalyst supported by hierarchical porous sulfur‐doped nanocarbon (SACo/ADFS@HPSC), as presented in Figure a. Acting as a kinetics modulator on the lithium surface, the active SACo can interact with the Li atom to significantly lower the initial nucleation barrier of plated lithium.…”

“…a) Schematic illustration of the active SACo/ADFS modulator; b) galvanostatic plating/stripping performance of SACo/ADFS@HPSC‐Li at 0.5 mA cm −2 ; c) mechanism illustration of function of the SACo/ADFS@HPSC in modulating lithium‐ion kinetics; d) schematic configuration of large areal pouch cell, series of LED lights, and smart cars with many sensors are powered by the as‐prepared large areal pouch cell; e) cycling stability of the large areal pouch cell with high sulfur loading at 1 mA cm −2 . Reproduced with the permission [ 35 ] Copyright 2021, American Chemical Society.…”