Accelerated Li⁺ Desolvation for Diffusion Booster Enabling Low‐Temperature Sulfur Redox Kinetics via Electrocatalytic Carbon‐Grazfted‐CoP Porous Nanosheets

Abstract

Lithium–sulfur (Li–S) batteries are famous for their high energy density and low cost, but prevented by sluggish redox kinetics of sulfur species due to depressive Li ion diffusion kinetics, especially under low‐temperature environment. Herein, a combined strategy of electrocatalysis and pore sieving effect is put forward to dissociate the Li+ solvation structure to stimulate the free Li+ diffusion, further improving sulfur redox reaction kinetics. As a protocol, an electrocatalytic porous diffusion‐boosted nitrogen‐doped carbon‐grafted‐CoP nanosheet is designed via forming the NCoP active structure to release more free Li+ to react with sulfur species, as fully investigated by electrochemical tests, theoretical simulations and in situ/ex situ characterizations. As a result, the cells with diffusion booster achieve desirable lifespan of 800 cycles at 2 C and excellent rate capability (775 mAh g−1 at 3 C). Impressively, in a condition of high mass loading or low‐temperature environment, the cell with 5.7 mg cm−2 stabilizes an areal capacity of 3.2 mAh cm−2 and the charming capacity of 647 mAh g−1 is obtained under 0 °C after 80 cycles, demonstrating a promising route of providing more free Li ions toward practical high‐energy Li–S batteries.

Vanadium as Auxiliary for Fe–V Dual-Atom Electrocatalyst in Lithium–Sulfur Batteries: “3D in 2D” Morphology Inducer and Coordination Structure Regulator

“…In the Li–S cells with modified separators, it is commonly believed that in the initial several cycles, the sulfur in the cathode would gradually migrate to the surface of coating layers during sulfur phase transformation, realizing a redistribution on the cathodic side of the separators. Thus, the comprehensive role of coating layers on separators is crucial in this process Figure b presents the galvanostatic discharge–charge profiles at 0.2 C between 1.7 and 2.6 V for the first cycle.…”

“…Thus, the comprehensive role of coating layers on separators is crucial in this process. 61 Figure 6b presents the galvanostatic discharge−charge profiles at 0.2 C between 1.7 and 2.6 V for the first cycle. Notably, the cell with a DAC-modified separator possesses a higher discharging voltage of 2.13 V (2.1 V for SAC), smaller polarization potential (ΔE 1 = 0.141 V, ΔE 2 = 0.186 V), and higher initial specific capacity of 1279.4 mAh g −1 (1210.3 mAh g −1 for SAC), exhibiting enhanced conversion kinetics and high sulfur utilization.…”

Versatile Composite Binder with Fast Lithium-Ion Transport for LiCoO2 Cathodes

“…The ion transport properties of the electrodes can be improved by introducing oxygen that can provide active sites for Li + . − PEO has a large number of oxygen atoms and is often used in solid-state electrolytes. Herein, we conducted a screening for a composite binder by simply blending poly­(ethylene oxide) (PEO) and PVDF.…”

High-Entropy MXene as Bifunctional Mediator toward Advanced Li–S Full Batteries

“…12 Furthermore, extensive efforts have been devoted to electrolyte composition modulation, 13 separator/interlayer modification, 14 and protection for lithium anode. 15,16 However, most methods cannot balance these aspects, and it is difficult to optimize the long-term cycling performance of LSBs. Fortunately, separator modification to obtain multifunctional separators was once deemed as the most promising shortcut to fulfill these goals.…”

“…To break this barrier, in the early stages, researchers focused on constructing a sulfur/carbon composite cathode, with carbon-based materials working as conductive networks, to provide fast electron transfer and accelerate the LiPSs redox conversion reaction . Furthermore, extensive efforts have been devoted to electrolyte composition modulation, separator/interlayer modification, and protection for lithium anode. , However, most methods cannot balance these aspects, and it is difficult to optimize the long-term cycling performance of LSBs. Fortunately, separator modification to obtain multifunctional separators was once deemed as the most promising shortcut to fulfill these goals. − The ideal modified separators should enjoy the following characteristics: (1) provide abundant and uniform chemisorption and catalytic sites, to achieve strong capture and conversion toward LiPSs; (2) possess high electron transfer and fast Li + diffusion channels, to complete efficient charge transfer and Li + diffusion; (3) exhibit favorable mechanical properties, both to maintain reaction stability during charging and discharging and meet favorable protection for Li anode .…”