Hierarchical Porous Carbon Membrane Embedded with Pyrolyzed Co‐Based Metal−Organic Frameworks as Multifunctional Interlayers for Advanced Li−SeS₂ Batteries

Abstract

Selenium disulfide (SeS2) possesses competitive advantages over pure sulfur or selenium as an electrode material for lithium storage. However, the shutting effect and slow conversion rate of soluble lithium polysulfides/polyselenides (LiPSs/LiPSes) compromise the practical application of Li−SeS2 batteries. Herein, a ZIF‐67@PAN‐derived Co−N−C@C multifunctional porous membrane as the LiPSs/LiPSes trapping barrier for Li−SeS2 batteries is proposed. The hierarchical porous conductive network facilitates the transport of electrons/lithium ions. Meanwhile, the Co−N−C architecture not only has chemical interaction for trapping the mobile LiPSs/LiPSes, but also catalyzes the LiPSs/LiPSes conversion reaction during the cycling process. Benefiting from the multifunctional capabilities, the constructed Li−SeS2 cells with the aforementioned interlayer exhibit a high capacity utilization of 978 mAh g−1 at 0.2 A g−1, together with an excellent rate capacity of 532 mAh g−1 at 3 A g−1 and also superior cycle life with a capacity of 557 mAh g−1 after 300 cycles at 1 A g−1. More strikingly, they show promising capacity with stable cell performance with a mass loading of 4 mg cm−2.

Solid Carbon Spheres with Interconnected Open Pore Channels Enabling High-Efficient Polysulfide Conversion for High-Rate Lithium–Sulfur Batteries

“…Before the Li 2 S 6 adsorption, the high-resolution N 1s (Figure b) XPS spectrum of PNCS/NG show four N peaks at 398.3, 399.8, 401.5, and 405.0 eV, corresponding to the pyridinic-N, pyrrolic-N, graphitic-N, and oxidized-N, respectively. After the Li 2 S 6 adsorption, the pyridinic N and pyrrolic N peaks move to higher binding energy of ∼399.1 and ∼400.2 eV, respectively, and a new characteristic peak at 397.8 eV corresponding to the N–Li bonding is observed, which is due to the dipole–dipole interaction between LiPSs and the doped N on the carbon materials. , The high-resolution O 1s (Figure c) XPS spectra also indicate the chemical adsorption of LiPSs on PNCS/NG based on the shift of C–OH and O–CO peaks to higher binding energy as well as the appearance of Li–O binding at 529.48 eV . The chemical interaction of LiPSs for the PNCS and NG are also observed in the corresponding N 1s and O 1s XPS spectra after the Li 2 S 6 adsorption (Figure S6).…”

“…46,47 The high-resolution O 1s (Figure 2c) XPS spectra also indicate the chemical adsorption of LiPSs on PNCS/NG based on the shift of C− OH and O−C�O peaks to higher binding energy as well as the appearance of Li−O binding at 529.48 eV. 48 The chemical interaction of LiPSs for the PNCS and NG are also observed in the corresponding N 1s and O 1s XPS spectra after the Li 2 S 6 adsorption (Figure S6).…”

High-Entropy Metal Oxide-Coated Carbon Cloth as Catalysts for Long-Life Li–S Batteries

“…As shown in Figure a, the significant discoloration of the Li 2 S 6 solution by CC/HEO and corresponding UV–vis spectra results suggest strong adsorption of HEO to polysulfides. , In addition, the underlying chemical interaction mechanism between HEO and LiPSs is revealed by XPS results. The transition metal 2p peaks shift to lower binding energy after adsorption of Li 2 S 6 (Figure S5), demonstrating the electron transfer from Li 2 S 6 to HEO. − Figure b shows the cyclic voltammogram (CV) profiles of the symmetric cells via CC and CC/HEO with a scanning rate of 2 mV s –1 . Clearly, the symmetrical CC/HEO cell displays a much larger redox current than the CC cell, suggesting the enhanced catalytic reaction of HEO. − Even at a 30 mV s –1 scan rate (Figure S6), the redox peaks can still be observed, indicating strong catalytic capability of HEO.…”