Thiol-Containing Metal–Organic Framework-Decorated Carbon Cloth as an Integrated Interlayer–Current Collector for Enhanced Li–S Batteries

Abstract

Lithium–sulfur (Li–S) batteries hold great promise for new-generation energy storage technologies owing to their overwhelming energy density. However, the poor conductivity of active sulfur and the shuttle effect limit their widespread use. Herein, a carbon cloth decorated with thiol-containing UiO-66 nanoparticles (CC@UiO-66­(SH)2) was developed to substitute the traditional interlayer and current collector for Li–S batteries. One side of CC@UiO-66­(SH)2 acts as a current collector to load active materials, while the other side serves as an interlayer to further restrain polysulfide shuttling. This two-in-one integrated architecture endows the sulfur cathode with fast electron/ion transport and efficient chemical confinement of polysulfides. More importantly, rich thiol groups in the pores of UiO-66­(SH)2 serve to tether polysulfides by both covalent interactions and lithium bonding. Therefore, the Li–S battery equipped with this integrated interlayer–current collector not only delivers an enhanced specific capability (1209 mAh g–1 at 0.1 C) but also exhibits prominent cycling stability (an attenuation rate of 0.037% per cycle for 1000 cycles at 1 C). Meanwhile, the battery achieves a high discharge capacity of 795 mAh g–1 at a sulfur loading of 3.83 mg cm–2. The new metal–organic framework (MOF)-based electrode material reported in this study undoubtedly provides insights into the exploration of functional MOFs for robust Li–S batteries.

Covalently introducing sulfur in a thiol-rich metal-organic framework toward advanced lithium-sulfur batteries

“…[31] Besides, compared with the spectrum of UiO-66@CNT, a new characteristic peak of the thiol groups (-SH) can be seen in the spectrum of UiO-66(SH)2@CNT. [32] Subsequently, S-UiO-66(SH)2@CNT was prepared by covalent connection between sulfur powder and UiO-66(SH)2@CNT. When the mixture of sulfur and UiO-66(SH)2@CNT was heated at 185 °C, the circular S8 could cleave into linear sulfur species with radical chain end and covalently connect with UiO-66(SH)2 to form a MOF-sulfur copolymer.…”

Thiol and thioether-based metal–organic frameworks: synthesis, structure, and multifaceted applications

“…5). 150 A Ni 2 P nanoparticle-incorporated thioether-based MOF composite was synthesized by Li et al by an in situ impregnation technique (Table 7, entry no. 6), which was utilized for photocatalytic hydrogen evolution reactions (Fig.…”

“…Thiol MOF-based composite CC@UiO-66(SH) 2 combined with a Li–S battery exhibits a better discharge capacity of 1209 mA h g −1 at 0.1 C, outstanding cyclic stability, and high efficiency. 150 Recently, Mandal and co-workers reported the HER activity (hydrogen evolution reaction) of Au and Ag nanoparticle immobilized thiol NU-1000-SH. 138,139 The composite material Au@NU-1000-SH exhibits an overpotential of 101 mV at a current density of 10 mA cm −2 with a Tafel slope of 44 mV dec −1 .…”

Donor–Acceptor Conjugated Microporous Polymer toward Enhanced Redox Kinetics in Lithium–Sulfur Batteries

“…During the past few decades, many strategies have been proposed to address the problems, including design of nanostructured sulfur hosts, − modification of the commercial separator − and addition of the multifunctional interlayers. − Among them, the modification of separator has been regarded as a simple and straightforward way to improve the sulfur chemistry of Li–S battery and strenuous efforts have been made to coat functional materials on the surface of separator in recent years. − Initially, carbonaceous materials are preferred for modifier, since they can increase the conductivity of cathode and physically confine the dissolved LiPSs at the same time. , However, owing to the weak interaction between nonpolar carbon and polar LiPSs, the carbon based materials displayed limited capability in anchoring LiPSs. In this regard, tremendous attention has been shifted to the modification of the separator by casting polar materials (e.g., heteroatom-doped carbon − and metal oxides , ) with strong chemical adsorption of LiPSs onto the cathodic side, through which active species can be confined within the cathodic area.…”