Recent Progress for Concurrent Realization of Shuttle‐Inhibition and Dendrite‐Free Lithium–Sulfur Batteries

Abstract

Lithium–sulfur (Li–S) batteries have become one of the most promising new‐generation energy storage systems owing to their ultrahigh energy density (2600 Wh kg−1), cost‐effectiveness, and environmental friendliness. Nevertheless, their practical applications are seriously impeded by the shuttle effect of soluble lithium polysulfides (LiPSs), and the uncontrolled dendrite growth of metallic Li, which result in rapid capacity fading and battery safety problems. A systematic and comprehensive review of the cooperative combination effect and tackling the fundamental problems in terms of cathode and anode synchronously is still lacking. Herein, for the first time, the strategies for inhibiting shuttle behavior and dendrite‐free Li–S batteries simultaneously are summarized and classified into three parts, including “two‐in‐one” S‐cathode and Li‐anode host materials toward Li–S full cell, “two birds with one stone” modified functional separators, and tailoring electrolyte for stabilizing sulfur and lithium electrodes. This review also emphasizes the fundamental Li–S chemistry mechanism and catalyst principles for improving electrochemical performance; advanced characterization technologies to monitor real‐time LiPS evolution are also discussed in detail. The problems, perspectives, and challenges with respect to inhibiting the shuttle effect and dendrite growth issues as well as the practical application of Li–S batteries are also proposed.

Carbon Nanotube‐encapsulated Chestnut Inner Shell O,N‐doped Graded Porous Carbon as Stable and High‐Sulfur Loading Electrode for Lithium‐Sulfur Batteries

“…The galvanostatic intermittent titration technique (GITT) measurement was employed to investigate the nucleation and activation process of Li 2 S. The CISC@S/CNTs battery (Figure 7a) displays a lower discharge/charge polarization voltage plateau than the CISC@S battery (Figure 7b). This observation further substantiates that the CNTs coating exerts a beneficial effect on the redox reaction of polysulfides [2c,26] . To delve deeper into the advantages conferred by CISC@S/CNTs in Li 2 S nucleation, potentiostatic discharge curves of CISC@S/CNTs and CISC@S batteries were recorded at 2.05 V employing Li 2 S 8 solution as the electrolyte (Figure 7c–d).…”

MoO2/t-C3N4 Heterogeneous Materials with Bidirectional Catalysis for the Rapid Conversion of S Species in Li–S Batteries

“…In a word, the shuttle of LiPSs can cause LSBs to have lower cycle life, excessive self-discharge, poor rate performance, and low Coulombic efficiency. 6,8 After a long period of exploration by researchers, in the current research on the modification of LSBs, the aspects of cathode design, anode protection, separator modification and electrolyte conditioning have become the consensus to enhance the performance of LSBs. 8−10 From a practical point of view, the design of the S cathode is a major priority because the energy density of LSBs is primarily dependent on the area capacity of the S cathode.…”

“…This results in a sharp drop in battery capacity. In a word, the shuttle of LiPSs can cause LSBs to have lower cycle life, excessive self-discharge, poor rate performance, and low Coulombic efficiency. , …”

“…After a long period of exploration by researchers, in the current research on the modification of LSBs, the aspects of cathode design, anode protection, separator modification and electrolyte conditioning have become the consensus to enhance the performance of LSBs. − From a practical point of view, the design of the S cathode is a major priority because the energy density of LSBs is primarily dependent on the area capacity of the S cathode . The two most common methods for reducing shuttle effects in S cathode studies are physical confinement and chemisorption .…”

Advances in research on the inhibitory effect of 3D current collector structures for lithium dendrites

“…In this regard, many researchers have conducted extensive and detailed studies on the dendrite growth of lithium metal anodes and have developed various methods to inhibit it. For example, liquid electrolyte modification (solvents, lithium salts and additives), 32–36 solid electrolytes, 37–40 artificial SEI, 41–50 separator modifications, 51–60 and 3D current collectors 61–66 have been constructed. According to Sand's time theory, the effective current density significantly influences the lithium deposition behavior during electroplating.…”