Solid‐State Lithium–Sulfur Battery Enabled by Thio‐LiSICON/Polymer Composite Electrolyte and Sulfurized Polyacrylonitrile Cathode

Abstract

Solid‐state lithium–sulfur battery (SSLSB) is attractive due to its potential for providing high energy density. However, the cell chemistry of SSLSB still faces challenges such as sluggish electrochemical kinetics and prominent “chemomechanical” failure. Herein, a high‐performance SSLSB is demonstrated by using the thio‐LiSICON/polymer composite electrolyte in combination with sulfurized polyacrylonitrile (S/PAN) cathode. Thio‐LiSICON/polymer composite electrolyte, which processes high ionic conductivity and wettability, is fabricated to enhance the interfacial contact and the performance of lithium metal anodes. S/PAN is utilized due to its unique electrochemical characteristics: electrochemical and structural studies combined with nuclear magnetic resonance spectroscopy and electron paramagnetic resonance characterizations reveal the charge/discharge mechanism of S/PAN, which is the radical‐mediated redox reaction within the sulfur grafted conjugated polymer framework. This characteristic of S/PAN can support alleviating the volume change in the cathode and maintaining fast redox kinetics. The assembled SSLSB full cell exhibits excellent rate performance with 1183 mAh g−1 at 0.2 C and 719 mAh g−1 at 0.5 C, respectively, and can accomplish 50 cycles at 0.1 C with the capacity retention of 588 mAh g−1. The superior performance of the SSLSB cell rationalizes the construction concept and leads to considerations for the innovative design of SSLSB.

Simultaneous MQMAS NMR Experiments for Two Half-Integer Quadrupolar Nuclei

“…We demonstrate a way to more efficiently utilize NMR instrument time to measure MQMAS experiments for half-integer quadrupolar nuclei with multiple receivers and multiply tuned probes. The experiments presented here are a demonstration of the power of multiple receivers in solid-state NMR of materials [1] , [2] , [3] , [4] , [5] , [6] , [7] , [8] , [9] , [10] , [11] , [12] , [13] , [14] , [15] , [16] , [17] , [18] , [19] , [20] , [21] , [22] , [23] , [24] , [25] , [26] , [27] with applications to biological samples also possible [12] , [13] , [65] , [66] . Embedded looping was previously presented for solution and solid-state NMR multiple receiver experiments and is a powerful tool to collect full NMR datasets for small molecules in a short time [49] , [50] , [51] , [52] , [53] , [54] .…”

“…In inorganic-materials chemistry, there are a large number of relevant NMR-active nuclei which are commonly used for this purpose. Solid-state NMR is well-suited to characterize a wide variety of material applications including cements [1] , [2] , geopolymers [3] , batteries [4] , [5] , [6] , [7] , [8] , biomaterials [9] , [10] , [11] , [12] , [13] , aluminosilicates [14] , [15] , [16] , [17] , minerals and other disordered solids [18] , [19] , [20] , [21] , [22] , [23] , [24] , [25] , [26] , [27] where nuclei such as 11 B, 17 O, 27 Al and 29 Si are important probes into the disorder present. These nuclei span the periodic table, and, accordingly, have a wide variety of quantum spin-numbers, natural abundances, sensitivities, and relaxation rates can vary by ~6 orders of magnitude [28] , [29] .…”

Polymer-based hybrid battery electrolytes: theoretical insights, recent advances and challenges

“…74 This work also reports the diffusion of the polysuldes from the Li 6 PS 5 Cl/polymer interface to the surface of Li metal, possibly enabling the use of Li-metal through formation of Li x S y -rich articial SEI. Very recently, Meirong Li et al 152 and Xue Li et al 26 Importantly, LLZO is prone to surface contamination via the formation of carbonate and oxide layers that hinder ionic transport between the inorganic and organic phases. [153][154][155] When the designed ller structure becomes complex, the removal of the insulating Li 2 CO 3 layer may require signicant effort.…”

PIM‐1 as a Multifunctional Framework to Enable High‐Performance Solid‐State Lithium–Sulfur Batteries

“…[6] Developing solidstate Li-S batteries without flammable liquid organic electrolytes is a promising route to overcome these challenges. [6][7][8][9][10] Among the various solid-state electrolytes available, poly(ethylene oxide) (PEO) has been extensively researched due to its merits of good film-forming ability, flexibility, and low interfacial resistance. [11,12] However, the intrinsic shortcoming of low ionic conductivity (10 -6 -10 -7 S cm −1 at room temperature) limits its application in commercially relevant batteries; the semi-crystalline nature of the PEO matrix hinders the formation of continuous Li + transfer pathways.…”