N‐Doped Graphdiyne Coating for Dendrite‐Free Lithium Metal Batteries

Abstract

Nonuniform nucleation is one of the major reasons for the dendric growth of metallicl ithium, whichl eads to intractable problems in the efficiency,r eversibility,a nd safety in Li-based batteries. To improve the deposition of metallic Li on Cu substrates, herein, af reestandingc urrent collector (NGDY@CuNW) is formed by coatingpyridinic nitrogen-doped graphdiyne (NGDY) nanofilms on 3D Cu nanowires (CuNWs). Theoretical predictions reveal that the introductiono fn itrogen atoms in the 2D GDY can enhance the binding energy between the Li atom and GDY,t herefore improving thel ithiophilicity on the surface for uniform lithium nucleation and deposition. Accordingly,the deposited metallic Li on the NGDY@CuNW electrode exhibitsadendrite-free morphology,r esultingi ns ignificant improvements in terms of the reversibility with ah igh coulombic efficiency (CE) and along lifespana thigh currentd ensity.Our research provides an efficient methodt oc ontrol the surfacep roperty of Cu, which also will be instructive for other metal batteries.Supporting information and the ORCID identification number(s) for the author(s) of this articlecan be found under: https://doi.

Strategies in Structure and Electrolyte Design for High‐Performance Lithium Metal Batteries

“…The coating of a homogenous, ion‐conductive, chemically and mechanically stable protective layer has been proven to be an effective approach to mitigating the uncontrollable lithium dendrite growth and accommodate the infinite volume change of lithium metal. [ 30–32 ] Various artificial coating materials such as LiF, [ 33,34 ] Al 2 O 3 , [ 35 ] graphdiyne, [ 36 ] polyethylene oxide, [ 37 ] and so on have been investigated to improve the cycling performance in LMBs. All studies have attempted to optimize the mechanical strength and Li‐ion conductivity of artificial SEI to achieve the high Coulombic efficiency, long lifetime, and low overpotential of LMBs.…”

Controlled Lithium Deposition

“…The pores that can guide lithium deposition are not limited to the artificially prepared micro-pores. Various natural nano-pores such as the gaps or cracks between nanowires (Lu et al, 2017;Yan K. et al, 2018;Shang et al, 2020) and nanoparticles Ma et al, 2019;Qiu et al, 2019) were also proved feasible in controlling the location of the lithium deposition. The 3D current collectors composed of Cu nanofibers (Yang et al, 2015) and nanoparticles (Ma et al, 2019) were used to effectively improve the lithium plating/stripping performance.…”

Research Progress on Copper-Based Current Collector for Lithium Metal Batteries

“…On this basis, the characteristics of pyridine nitrogen-doped graphdiyne-coated copper nanowire current collector were further studied. 132 Theoretical calculations show that the introduction of pyridine N atoms in graphdiyne can enhance the bond energy of graphdiyne and lithium atoms, improve the lithophilic characteristics of the graphdiyne surface, and make the lithium metal nucleate and deposit uniformly. Zhou et al fabricated a copper-clad carbon framework (CuCF) via high-temperature pyrolysis of melamine-formaldehyde foam (MF) as substrate and followed by Cu electroplating.…”