Calixarene‐Functionalized Porous Carbon Aerogels for Polysulfide Capture: Cathodes for High Performance Lithium‐Sulfur Batteries

Abstract

A cage‐type composite was successfully prepared by attaching p‐sulfonatocalix[4]arene to a porous activated carbon aerogel (ACA). The resulting composite showed a high specific surface area of 1620.7 m2 g−1 and a high sulfur loading of 2.5 mg cm−2. The calixarene is uniformly dispersed on the carbon spheres and efficiently captures polysulfides by interaction with the sulfonate groups. Meanwhile, the cross‐linked porous structure of the composite restricts the migration of polysulfides. The cathode delivers an outstanding electrochemical performance with an initial capacity of 1304.7 mAh g−1 at 0.2 C. Furthermore, it displays excellent long‐term cycling stability, maintaining 884.7 mAh g−1 after 300 cycles at 0.5 C. Density functional theory (DFT) adsorption calculations support the strong interaction between the calixarenes and polysulfides and reveal the capture mechanism.

Polymer derived ceramic aerogels

“…Aerogels have recently drawn considerable attention in energy storage applications, for example, carbon-based aerogels are used both as anodes and cathodes for lithium-ion [99][100][101], lithium-sulfur [102][103][104], and sodium-ion [105,106] batteries. Alternatively, they also find use in supercapacitors [107][108][109][110][111], an example for Mxene-rGO (Ti 3 Cr 2 T x -reduced graphene oxide) aerogel is given in Fig.…”

In Situ Nitrogen‐Doping Carbon Aerogel as an Effective Sulfur Host to Immobilize Polysulfides for High Performance Lithium‐Sulfur Battery

“…[8] Furthermore, LSB has been regarded as one of the most popular systems for the post-lithium secondary battery compared with traditional lithium-ion battery. [9,10] However, there are still several serious issues hampering the development of LSB including "shuttle phenomenon", [11] low Coulombic efficiency [12] and low sulfur utilization. [13] The "shuttle phenomenon" caused by LiPSs intermediates(Li 2 S n , (4 � n � 8)) [14] impedes the practical application of LSB and results in electrode degradation, [15] efficiency decrease [16] and capacity reduction.…”

“…However, there are still several serious issues hampering the development of LSB including “shuttle phenomenon”, [11] low Coulombic efficiency [12] and low sulfur utilization [13] . The “shuttle phenomenon” caused by LiPSs intermediates(Li 2 S n , (4≤n≤8)) [14] impedes the practical application of LSB and results in electrode degradation, [15] efficiency decrease [16] and capacity reduction [17] .…”