Defect Engineering in a Multiple Confined Geometry for Robust Lithium–Sulfur Batteries

Abstract

The decay of lithium–sulfur (Li–S) batteries is mainly due to the shuttle effect caused by intermediate polysulfides (LiPSs). Herein, a multiple confined cathode architecture is prepared by filling graphitized Pinus sylvestris with carbon nanotubes and defective LaNiO3−x (LNO‐V) nanoparticles. The composite electrode with high areal sulfur loading of 11.6 mg cm−2 shows a high areal specific capacity of 8.5 mAh cm−2 at 1 mA cm−2 (0.05 C). Both experimental results and theoretical calculations reveal that this unique structure not only provides physical restriction on LiPSs within microchannels but also offers strong chemical immobilization and catalytic conversion of LiPSs attributed to the spin density around oxygen vacancies of LaNiO3−x. These oxygen vacancies elongate the SS and LiS bonds and make them easy to break. Furthermore, the lengthwise channels derived from cytoderm restrict the transverse diffusion of polysulfides, leading to a uniform areal current and thus homogeneous lithium infiltration. This suppresses the corrosion of the lithium anode due to polysulfides confinement. The discovery of the multiple confined structure that provides chemical adsorption, fast diffusion, and catalytic conversion for polysulfides can broaden the application of biomass materials and offer a new strategy to achieve robust Li–S batteries.

Pseudocapacitive Vanadium Nitride Quantum Dots Modified One-Dimensional Carbon Cages Enable Highly Kinetics-Compatible Sodium Ion Capacitors

“…The phase characterizations of the above samples, including FESEM, TEM, HRTEM, EDS, XRD, Raman, XPS, TGA, BET, and so on, were all measured as in our previous work …”

“…The phase characterizations of the above samples, including FESEM, TEM, HRTEM, EDS, XRD, Raman, XPS, TGA, BET, and so on, were all measured as in our previous work. 1 Electrochemical Measurements. The electrodes of three samples were all obtained from cutting the nanofibers film into circular pieces with a diameter of 12 mm and an average mass of 0.8− 1.1 mg. Additionally, the assembling and electrochemical measurements of 2032-type half-batteries and SIHC full cells were all conducted as in our previous work.…”

“…With the increasing concerns on energy crisis and environmental pollution, clean energy utilization and electrochemical energy storage have become exigent tasks of human society. , Sodium ion hybrid capacitors (SIHCs) elaborately integrate the merits of high energy density of batteries and high output power of capacitors, holding enormous possibilities for future generations of energy storage equipment. However, the mismatch of kinetics between anode and cathode is still the biggest obstacle which severely hampers the development of high-performance SIHCs. − For the purpose of overcoming this obstacle, improving kinetics compatibility of anode/cathode by rationally constructing anode materials with pseudocapacitive superiorities for rapid charge storage would be valid yet remains a huge challenge thus far.…”

Modulating Bond Interactions and Interface Microenvironments between Polysulfide and Catalysts toward Advanced Metal–Sulfur Batteries

“…Moreover, when the defective LaNO 3-x nanoparticles were further introduced to catalyze the polysulfides conversion, the as-prepared LSBs exhibited a desirable areal-specific capacity (8.5 mAh cm −2 at 0.05 C) even under an ultrahigh areal loading of 11.6 mg cm −2 . [249] The 3D freestanding N, O-codoped wood-like carbon was further decorated with carbon nanotubes forest (WLC-CNTs) and used as the sulfur host for enabling scalable high-performance LSBs. With such interconnected 3D structures, the ionic and charge-transfer resistance per unit of the electroactive surface area of the S@WLC-CNTs electrode does not change with the increase of thickness, resulting in a thickness-independent performance of LSBs.…”

Renewable biomass-derived carbon-based hosts for lithium–sulfur batteries

“…Recently, Zou et al 267 introduced a new concept of using defect engineering in multiple confined geometries to manufacture ultra-stable electrodes. Researchers designed a multicomponent cramped microchannel architecture (GP/CNT/LNO-V) by filling carbon nanotubes and LaNiO 3− x with oxygen vacancies in the microchannels of the graphitized pine substrate (Fig.…”