Built-In Catalysis in Confined Nanoreactors for High-Loading Li–S Batteries

Abstract

A cathode host with strong sulfur/polysulfide confinement and fast redox kinetics is a challenging demand for high-loading lithium−sulfur batteries. Recently, porous carbon hosts derived from metal−organic frameworks (MOFs) have attracted wide attention due to their unique spatial structure and customizable reaction sites. However, the loading and rate performance of Li−S cells are still restricted by the disordered pore distribution and surface catalysis in these hosts.Here, we propose a concept of built-in catalysis to accelerate lithium polysulfide (LiPSs) conversion in confined nanoreactors, i.e., laterally stacked ordered crevice pores encompassed by MoS 2 -decorated carbon thin layers. The functions of Sfixability and LiPS catalysis in these mesoporous cavity reactors benefit from the 2D interface contact between ultrathin catalytic MoS 2 and conductive C pyrolyzed from Al-MOF. The integrated function of adsorption−catalysis−conversion endows the sulfur-infused C@MoS 2 electrode with a high initial capacity of 1240 mAh g −1 at 0.2 C, long life cycle stability of at least 1000 cycles at 2 C, and high rate endurance up to 20 C. This electrode also exhibits commercial potential in view of considerable capacity release and reversibility under high sulfur loading (6 mg cm −2 and ∼80 wt %) and lean electrolyte (E/S ratio of 5 μL mg −1 ). This study provides a promising design solution of a catalysis−conduction 2D interface in a 3D skeleton for high-loading Li−S batteries.

MnO‐Inlaid hierarchically porous carbon hybrid for lithium‐sulfur batteries

“…[ 15 ] Another relatively weak peak at 169.5 eV is commonly attributed to the formation of sulfate. [ 16 ] The XPS result confirms the elemental composition result as obtained from XRD and TEM measurements.…”

Implanting Cobalt Atom Clusters within Nitrogen‐Doped Carbon Network as Highly Stable Cathode for Lithium–Sulfur Batteries

“…[ 24,32 ] The peaks at 168.03 and 169.19 eV correspond to S O (S‐oxide), [ 23b ] including thiosulfate, polythionate, and sulfate. [ 5,33 ] Polythionate and thiosulfate are generally considered intermediates of the polysulfide redox reaction when Co/PNC is used as the cathode in Li–S batteries. [ 15b ] The peak positions and intensities of S T −1 , S B 0 , and S O in the S2p XPS spectra are listed in Table S2 (Supporting Information).…”

Hierarchical porous N,S‐codoped carbon material derived from halogenated polymer for battery applications

“…The capacities of S@NS‐C at 0.5 C, 1 C, 2 C, and 5 C are respectively 784.7, 656.9, 511.7, and 397.6 mAh g –1 , implying very good high‐rate performance, which can be attributed to the large SSA for the rich active interface for current exchange and the well‐defined hierarchical porosity for significantly improved mass transportation property. [ 53,54 ] Furthermore, resetting the rate to 0.1 C results in a large capacity retention of 92.7%, reaching 849.0 mAh g –1 relative to the capacity of 916.2 mAh g –1 after full activation at 0.1 C. Remarkably, the S@NS‐C can be cycled for over 200 times at a large rate of 2 C and receives the lowest capacity loss of 19.5% (Figure S4B,D,F, Figure S5 and Figure 4D), rendering a loss ratio of 0.097% pre cycle. S@NS‐C composite with higher S loading was also measured for long‐term use, as shown in Figure S6A, a higher S percentage of 80% was used for measurement.…”