High‐Capacity, Dendrite‐Free, and Ultrahigh‐Rate Lithium‐Metal Anodes Based on Monodisperse N‐Doped Hollow Carbon Nanospheres

Abstract

To unlock the great potential of lithium metal anodes for high‐performance batteries, a number of critical challenges must be addressed. The uncontrolled dendrite growth and volume changes during cycling (especially, at high rates) will lead to short lifespan, low Coulombic efficiency (CE), and security risks of the batteries. Here it is reported that Li metal anodes, employing the monodisperse, lithiophilic, robust, and large‐cavity N‐doped hollow carbon nanospheres (NHCNSs) as the host, show remarkable performances—high areal capacity (10 mAh cm−2), high CE (up to 99.25% over 500 cycles), complete suppression of dendrite growth, dense packing of Li anode, and an extremely smooth electrode surface during repeated Li plating/stripping. In symmetric cells, a highly stable voltage hysteresis over a long cycling life >1200 h is achieved, and a low and stable voltage hysteresis can be realized even at an ultrahigh current density of 64 mA cm−2. Furthermore, the NHCNSs‐based anodes, when paired with a LiFePO4 (LFP) cathode in full cells, give rise to highly improved rate capability (104 mAh g−1 at 10 C) and cycling stability (91.4% capacity retention for 200 cycles), enabling a promising candidate for the next‐generation high energy/power density batteries.

Chemical modification of ordered/disordered carbon nanostructures for metal hosts and electrocatalysts of lithium‐air batteries

“…Reproduced with permission: Copyright 2014, Springer Nature. (B) Schematic description of Li growth on Cu foil and 3D NHCNSs host 98 . Reproduced with permission, Copyright 2020, Wiley‐VCH.…”

Remedies to Avoid Failure Mechanisms of Lithium-Metal Anode in Li-Ion Batteries

“…Nano-carbon skeleton has been proposed under the form of graphene matrix [180][181][182][183][184][185], carbon nanotubes (CNTs) [183][184][185][186][187][188][189], graphene-CNT hybrid [190], carbon nanofibers [191][192][193], spherical carbon granules [194], hollow carbon fibers [195], hollow carbon nanospheres [142,196,197], or porous carbon film [198]. Zhang et al Infused molten lithium into a carbonized wood (C-wood) as a 3D, highly porous (73% porosity) conductive framework.…”

Effects of nanopores and sulfur doping on hierarchically bunched carbon fibers to protect lithium metal anode

“…Therefore, studies on how to establish a feasible LMA system have focused on minimizing the excess use of lithium metal in LMAs through sophisticated electrode design and electrolyte engineering 8–11 . Among several research approaches, 3D‐structured carbon‐based electrode materials with high active surface areas have been shown to guide homogeneous metal deposition/dissolution cycles with high CE, where the more highly functionalized carbons can provide more active surfaces for metal nucleation and growth 12–19 . The large number of nucleation sites can significantly decrease the overpotential, resulting in simultaneous growth of lithium metal on all the surfaces 20,21 .…”