Mechanistic understanding of the Sulfurized-Poly(acrylonitrile) cathode for lithium-sulfur batteries

Weret, Misganaw Adigo; Kuo, Chung‐Feng Jeffrey; Zeleke, Tamene Simachew; Beyene, Tamene Tadesse; Tsai, Meng‐Che; Huang, Chen‐Jui; Berhe, Gebregziabher Brhane; Su, Wei‐Nien; Hwang, Bing‐Joe

doi:10.1016/j.ensm.2019.11.022

Cited by 126 publications

(108 citation statements)

References 56 publications

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“…[ 12 ] The high‐resolution C 1s spectrum (Figure 3g) can be divided into four peaks at around 284.7, 285.6, 286.7, and 288.7 eV, corresponding to CC/CC/CN, CS, C‐N and CO bonds, respectively. [ 29,30 ] As displayed in Figure 3h, the S 2p spectra can be fitted into two doublets. One doublet at 163.5 eV (S 2p 3/2 ) and 164.8 eV (S 2p 1/2 ) confirms the presence of CS and SS bonds.…”

Section: Resultsmentioning

confidence: 99%

“…There is a visible high polarized cathodic peak at 1.34 V in initial cycle, due to the break of SC or SN covalent bonds needing a high activation energy. [ 30 ] The reduction peak converts into two peaks at 2.07 and 1.72 V during the subsequent cycle, corresponding to the formation of polysulfides (Li 2 S n , n < 4). [ 31 ] For anodic scanning, there is only one peak at around 2.30 V, indicating the oxidation reaction of Li 2 S n .…”

Section: Resultsmentioning

confidence: 99%

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3D Holey Graphene/Polyacrylonitrile Sulfur Composite Architecture for High Loading Lithium Sulfur Batteries

Wang

Zhang

Zhong

et al. 2021

Advanced Energy Materials

157

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Lithium sulfur (Li–S) batteries have attracted considerable interest as next‐generation high‐density energy storage devices. However, their practical application is limited by low capacity and rapid capacity fading at commerical‐level mass loadings, which is largely attributed to the inferior electron/ion conduction, as well as severe the shuttling effect of soluble polysulfide species. To address these issues, a three‐dimensional holey graphene/polyacrylonitrile sulfur (3DHG/PS) composite cathode is developed for high‐mass‐loading Li–S batteries. The unique architectural design with the 3D holey graphene framework ensures fast electron and ion transport within the thick electrode, and affords enough space for mitigating the volume expansion of the electrode. Moreover, in situ Raman results demonstrate that covalent sulfur within 3DHG/PS fundamentally avoids forming soluble lithium polysulfides, which effectively reduces the undesired shuttling effect. With these advantages, the 3DHG/PS cathode exhibits an ultra‐low capacity fading rate of 0.012% per cycle after continuous 1500 cycles, as well as high specific capacity and superior rate capability with a high mass loading of 15.2 mg cm–2, which offers a promising avenue to construct future Li–S batteries with superior performance at mass loadings that exceed commercial levels.

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Section: Resultsmentioning

confidence: 99%

Section: Resultsmentioning

confidence: 99%

3D Holey Graphene/Polyacrylonitrile Sulfur Composite Architecture for High Loading Lithium Sulfur Batteries

Wang

Zhang

Zhong

et al. 2021

Advanced Energy Materials

157

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“…[ 32,33 ] However, they shift to lower binding energy of 163.3 and 164.4 eV after cycling, respectively, which demonstrates the combining of Na + on SPAN that lowers the valence state of S. [ 45 ] The other two peaks can be attributed to adsorbed HS x C byproduct and possible oxidation/nitridation product, respectively. [ 51–53 ] The overall valence structure of S remains unchanged after cycling, further indicating the superior cycling stability of SPAN interlayer. A brief schematic illustration of the interfacial cycling process of SPAN‐NASICON based solid‐state batteries is shown in Figure 6 a.…”

Section: Resultsmentioning

confidence: 99%

Isotropous Sulfurized Polyacrylonitrile Interlayer with Homogeneous Na⁺ Flux Dynamics for Solid‐State Na Metal Batteries

Miao

Wang

Sun

et al. 2021

Advanced Energy Materials

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Inorganic solid‐state electrolyte (SSE) based Na‐metal batteries have received extensive attention in next‐generation lithium‐free energy storage systems with both high‐security and superior electrochemical performance. Herein, in contrast to the conventionally used polymer/ceramic/polymer sandwich electrolyte, an efficient green and scalable powder‐polishing synthetic method is developed to fabricate a pyrolyzed‐polyacrylonitrile modified Na super ionic conductor (NASICON) electrolyte to relieve polarization of integrated composite SSE and ameliorate interfacial contact between the electrolyte and the Na anode. Furthermore, introducing S in the preferable isotropous sulfurized polyacrylonitrile (SPAN) interlayer can trigger dehydrogenation and cyclization of polyacrylonitrile with chemically‐bonded short‐chain SS segments, which can bond with Na+ to redistribute the interfacial electric field and homogenize transported Na+ flux, leading to transition of Na deposition behavior from dendrite growth mode to lateral flat‐shape growth tendency. The conjugated polymer backbones possess delocalized radicals that can activate formed short‐chain sulfides to reconnect to the backbones, thus maintaining superior structural stability. Benefiting from the rational interfacial design, a record‐high value of 1.4 mA cm−2 for critical current density of Na/SPAN‐NASICON/Na cells is obtained. Moreover, SPAN is used as a cathode to assemble solid‐state Na/SPAN‐NASICON/SPAN Na‐organosulfur batteries, demonstrating superior capacity and cycling‐stability. The rational SPAN‐based structural design strategy may provide an avenue for potential application of solid‐state alkali metal batteries.

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“…[60] With the decreases in intensities of S 2p 1/2 and S 2p 3/2 peaks, the peak of Li 2 S emerges and its intensity becomes larger progressively, agreeing with the proposed solid-solid reaction process. [61] During the charge process, the positions of S 2p 1/2 and S 2p 3/2 peaks come back to their original locations and their intensities almost recover, implying a reversible reaction process. [62] The formation process of Li 2 S is also confirmed by the Li 1s spectra of SC@A (Figure 5d 2).…”

Section: Resultsmentioning

confidence: 89%

Mesoporous Yolk‐Shell Structured Organosulfur Nanotubes with Abundant Internal Joints for High‐Performance Lithium–Sulfur Batteries by Kinetics Acceleration

Wei

Liu

et al. 2021

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Although organosulfur compounds can protect lithium anodes, participate in the redox reaction, and suppress the shuttle effect, the sluggish electrochemical dynamics of their bulk structure and the notorious shuttle effect of covalent long‐chain sulfurs largely impede their actual applications. Herein, sulfurized carbon nanotube@aminophenol‐formaldehyde (SC@A) with covalently linked short‐chain sulfurs is firstly synthesized by in situ polymerization of aminophenol‐formaldehyde (AF) on the surface of carbon nanotubes (CNTs) followed by acetone etching and inverse sulfurization processes, forming mesoporous yolk‐shell organosulfur nanotubes with abundant internal joints between the yolk of CNTs and the shell of sulfurized AF for the first time. In situ Raman spectra, in situ XRD patterns, and ex situ XPS spectra verify that the covalent short‐chain sulfurs bring about a reversible solid‐solid conversion process of sulfur, thoroughly avoiding the shuttle effect. The mesoporous yolk‐shell structure with abundant internal joints can effectively accommodate the volume change, fully expose active sites and efficiently improve the transport of electrons and lithium ions, thus highly promoting the solid–solid electrochemical reaction kinetics. Therefore, the SC@A cathode exhibits a superior specific capacity of 841 mAh g−1 and a capacity decay of 0.06% per cycle within 500 cycles at a large current density of 5.0 C.

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Mechanistic understanding of the Sulfurized-Poly(acrylonitrile) cathode for lithium-sulfur batteries

Cited by 126 publications

References 56 publications

3D Holey Graphene/Polyacrylonitrile Sulfur Composite Architecture for High Loading Lithium Sulfur Batteries

3D Holey Graphene/Polyacrylonitrile Sulfur Composite Architecture for High Loading Lithium Sulfur Batteries

Isotropous Sulfurized Polyacrylonitrile Interlayer with Homogeneous Na⁺ Flux Dynamics for Solid‐State Na Metal Batteries

Mesoporous Yolk‐Shell Structured Organosulfur Nanotubes with Abundant Internal Joints for High‐Performance Lithium–Sulfur Batteries by Kinetics Acceleration

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Mechanistic understanding of the Sulfurized-Poly(acrylonitrile) cathode for lithium-sulfur batteries

Cited by 126 publications

References 56 publications

3D Holey Graphene/Polyacrylonitrile Sulfur Composite Architecture for High Loading Lithium Sulfur Batteries

3D Holey Graphene/Polyacrylonitrile Sulfur Composite Architecture for High Loading Lithium Sulfur Batteries

Isotropous Sulfurized Polyacrylonitrile Interlayer with Homogeneous Na+ Flux Dynamics for Solid‐State Na Metal Batteries

Mesoporous Yolk‐Shell Structured Organosulfur Nanotubes with Abundant Internal Joints for High‐Performance Lithium–Sulfur Batteries by Kinetics Acceleration

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Isotropous Sulfurized Polyacrylonitrile Interlayer with Homogeneous Na⁺ Flux Dynamics for Solid‐State Na Metal Batteries