A Porous Carbon Polyhedron/Carbon Nanotube Based Hybrid Material as Multifunctional Sulfur Host for High‐Performance Lithium‐Sulfur Batteries

Abstract

To develop high‐performance lithium‐sulfur (Li−S) batteries, designing and exploring an advanced sulfur cathode with a conductive and polar robust framework is highly significant to suppress the “shuttle effect” of polysulfides and enhance the utilization of active sulfur. Herein, a multifunctional conductive nanohybrid, which acts as a sulfur host, is rationally constructed by inserting/intertwining carbon nanotubes (CNTs) onto Co‐embedded N‐doped porous dual carbon polyhedrons derived from a resorcinol‐formaldehyde (RF) polymer layer enwrapping ZIF‐67 metal‐organic frameworks (MOFs) (Co, N−C@RFC/CNTs). The porous carbon polyhedrons can accommodate a high amount of sulfur owing to their large inner void space; the RF coating carbon layer and the CNTs effectively increase the conductivity and build a network for providing smooth ions/e− pathways; In addition, the polar Co particles and electronegative N heteroatoms synergistically strengthen the chemical adsorption of polysulfides and accelerate the redox reaction of the sulfur cathode. Benefiting from these advantages, the as‐fabricated Co, N−C@RFC/CNTs/S cathode delivers a high reversible capacity of 1373.7 mAh g−1 at 0.1 C, an impressive rate performance with 659.2 mAh g−1 at 2.0 C, and an outstanding cycling stability with an ultralow capacity decay rate of 0.041 % per cycle for 500 cycles at 1.0 C. This work provides a facile and high‐efficiency approach to fabricating excellent‐performance storage materials based on an MOF precursor.

Co−Ni Binary‐Metal Oxide Coated with Porous Carbon Derived from Metal‐Organic Framework as Host of Nano‐Sulfur for Lithium‐Sulfur Batteries

“…[9][10][11][12][13] In particular, porous carbon materials, including graphene, carbon nano-tubes, meso or microporous carbons, and hollow carbon spheres, have been used as hosts of sulfur and exhibited improved electrochemical performance originate from improved electronic conductivity of sulfur and void space to accommodate the volumetric changes during charging and discharging reaction. [9][10][11][12][13] In particular, porous carbon materials, including graphene, carbon nano-tubes, meso or microporous carbons, and hollow carbon spheres, have been used as hosts of sulfur and exhibited improved electrochemical performance originate from improved electronic conductivity of sulfur and void space to accommodate the volumetric changes during charging and discharging reaction.…”

“…To address the mentioned problems above, many researchers have made great efforts in the past few decades. [9][10][11][12][13] In particular, porous carbon materials, including graphene, carbon nano-tubes, meso or microporous carbons, and hollow carbon spheres, have been used as hosts of sulfur and exhibited improved electrochemical performance originate from improved electronic conductivity of sulfur and void space to accommodate the volumetric changes during charging and discharging reaction. [14,15] However, the porous carbon materials are less effective in trapping LiPS species owing to the weak intermolecular interactions between non-polar carbonaceous materials and polar LiPS species.…”

Recent Progress on Zeolitic Imidazolate Frameworks and Their Derivatives in Alkali Metal–Chalcogen Batteries

“…Carbon skeletons are characterized by high specific surface areas originating from the abundant pores formed by gas evaporation. [ 56 ] Meanwhile, the N species in imidazolate ligands are converted into N‐doped carbon components. There are three types of N species: pyrrolic, quaternary, and pyridinic.…”

“…Commercial CNTs can be introduced into the synthesis processes, aiming to connect the carbon polyhedra to form an integrated conductive network for fast electron transfer. [ 56,127–131 ] Ma et al. prepared CNT‐connected yolk–shell carbon polyhedra with Co and N doping as a sulfur immobilizer.…”

Rational Design of Metal–Organic Framework‐Based Materials for Advanced LiS Batteries

“…The complexation of MOFs with conductive materials is an efficient strategy to facilitate electron transfer and enhance structural stability. 50 Nitrogen-doped carbon/graphene (NPC/G) derived from the in situ grown ZIF-8 and ZIF-67 was used as a sulfur host in Li S batteries. The substrate material and graphene both provide fast electron transfer and robust support as building units.…”