Deciphering the defectmicro‐environmentof graphene for highly efficient Li–S redox reactions

Abstract

The lithium polysulfides (LiPS) dissolution into electrolyte as well as consequent shuttle behavior seriously exacerbate the electrochemical performance of lithium–sulfur batteries. Herein, the intrinsic defect of graphene has been tailored by using plasma irradiation. The topological defective carbon structure is demystified into monovacancy and divacancy which effectively promote Li–S redox kinetics by selectively decelerating the generation of soluble high‐order LiPSs and passingly promoting the conversion to final solid products. Theoretical prediction uncovers the selective manipulation of Li–S redox kinetics by defective graphene, facilitating the reduced overpotential effect and uniform deposition of Li2S. Moreover, the divacancy presents a higher activity for Li–S chemistry in contrast with monovacancy. Therefore, the battery achieves superior cyclability with a capacity retention of 88.6% at 1.0 C over 300 cycles. Furthermore, it yields an areal capacity up to 8.5 mAh cm−2 with a sulfur loading of 13.3 mg cm−2.

Metal‐organic framework derived porous structures towards lithium rechargeable batteries

“…Current research on the next‐generation batteries can be divided into LIB‐related research, which corresponds to the mature stage, and future battery‐related fields, corresponding to the introduction/growth stage, in consideration of the technological cycle. Lithium‐sulfur battery (LSB), 17–25 lithium‐metal battery (LMB), 26–35 and lithium‐air battery (LAB) 36–48 have been studied to overcome the limitations of LIB energy density, and all‐solid‐state batteries have been developed to overcome safety issues of battery. In addition, other next‐generation battery technologies are emerging such as flexible batteries 49–62 that can bend, and sodium‐ion 63–74 and zinc‐air batteries 41,75–86 for price and supply stability.…”

Molecular engineering of sulfur‐providing materials for optimized sulfur conversion in Li‐S chemistry

“…Despite their favorable features, the commercialization of Li‐S batteries is still plagued by some fundamental challenges involving the insulating nature of elemental sulfur and lithium sulfides (e.g., Li 2 S 2 and Li 2 S), large volume expansion (up to 80%) of sulfur during cycling, dissolution of lithium polysulfides (LiPSs) in electrolyte, and lithium dendrite formation at the anode side 10,11 . In recent years, great efforts have been devoted to find solutions to improve the electrochemical performance of Li‐S batteries, among them infiltrating sulfur into functional host materials to physically or electrostatically trap the LiPSs in the cathode structures has been revealed to be a promising approach 12–25 . However, such passive confinement/entrapping strategies are not effective enough to alleviate the dissolution and shuttling of LiPSs over long‐term cycling, leading to severe loss of active materials, corrosion of lithium anode, and thus rapid capacity fading.…”

“…10,11 In recent years, great efforts have been devoted to find solutions to improve the electrochemical performance of Li-S batteries, among them infiltrating sulfur into functional host materials to physically or electrostatically trap the LiPSs in the cathode structures has been revealed to be a promising approach. [12][13][14][15][16][17][18][19][20][21][22][23][24][25] However, such passive confinement/entrapping strategies are not effective enough to alleviate the dissolution and shuttling of LiPSs over long-term cycling, leading to severe loss of active materials, corrosion of lithium anode, and thus rapid capacity fading. Another well adopted approach to improve the performance of Li-S batteries is through introducing catalytical materials on the cathode side, for example, metal compounds [26][27][28][29][30] and their heterostructures, [31][32][33] single atoms catalysts (SACs), [34][35][36][37] and soluble molecular catalysts, [38][39][40][41][42] to promote/accelerate the conversion of LiPSs.…”

TiC Nanomaterials with Varying Dimensionalities as Anode Materials for Lithium-Ion Batteries

“…Currently, lithium–sulfur batteries (LSBs), lithium metal batteries (LMBs), and lithium-ion batteries (LIBs) are the widely used energy storage devices . For LIBs, the increased demand for consumer electronic devices and electric vehicles has stimulated the development of anode materials .…”

“…Currently, lithium−sulfur batteries (LSBs), lithium metal batteries (LMBs), and lithium-ion batteries (LIBs) are the widely used energy storage devices. 1 For LIBs, the increased demand for consumer electronic devices and electric vehicles has stimulated the development of anode materials. 2 By far, the commercial anode material for LIBs is graphite, which is limited for high power applications due to its relatively low theoretical capacity (372 mA h g −1 ), insufficient electronic conductivity (∼10 5 S m −1 ), and potential safety concerns.…”