Phosphorus-modified Fe<sub>4</sub>N@N,P co-doped graphene as an efficient sulfur host for high-performance lithium–sulfur batteries

Zhang, Meng; Wang, Lu; Wang, Bin; Zhang, Bo; Sun, Xiaoning; Wang, Debao; Kong, Zhen; Xu, Liqiang

doi:10.1039/d0ta12361g

Cited by 42 publications

(31 citation statements)

References 55 publications

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“…In sharp contrast, the platform of the cell with PP separator becomes unrecognizable, and the capacity drops dramatically at 5 C, implying sluggish kinetics of LiPSs conversion toward commercial-sulfur cathode. The ratio of Q L /Q H is considered as a significant parameter to evaluate the catalytic activity for LiPSs conversion reaction, in which the high discharge plateau capacity (corresponding to Q H ) is related to the formation of high-order soluble LiPSs and the low discharge plateau capacity (corresponding to Q L ) is related to the generation of insoluble Li 2 S 2 /Li 2 S. [49][50][51][52] As current density increases from 0.1 to 5 C, the Q H , Q L , and Q L /Q H ratio for the cell with RPM/PP separator are higher than those of PP separator, manifesting that the shuttle effect of LiPSs can be effectively inhibited and converted (Figure 2d and Figure S9, Supporting Information). Apart from the larger Q L /Q H , the cell with RPM/PP separator shows a much higher commercial-sulfur utilization than that of PP (3.8 times at 5 C) and most of the reported separator interlayers (Figure 2d).…”

Section: Electrochemical Propertiesmentioning

confidence: 99%

A Mott–Schottky Heterogeneous Layer for Li–S Batteries: Enabling Both High Stability and Commercial‐Sulfur Utilization

Shi

Zheng

Zhang

et al. 2022

Advanced Energy Materials

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electric vehicles. [1,2] However, the further scaled application of commercial LIBs encounters a "bottleneck": the overall energy density is approaching the ceiling due to the restriction of theoretical specific capacity of insertion-type oxide cathodes (≈250 mAh g −1 ) and graphite anodes (372 mAh −1 ). In order to satisfy the increasing demand for higher energy densities particularly under the extended application such as unmanned aerial vehicles, cargo aircraft, electric vehicles, and the exploration of novel storage system is of great significance. [3] Sulfur is earthabundant, low-cost, and environment friendly. More inspiring, lithium-sulfur batteries (LSBs) based on sulfur cathodes exhibit much higher theoretical specific capacity (1675 mAh g −1 ) through the multielectron redox reaction process, showing great potential for high-performance energy storage devices. [4] Despite the promising prospects, the practical application of LSBs is still impeded by several challenges, such as electrical insulation of sulfur and discharge products (Li 2 S/Li 2 S 2 ), severe shuttle effect of long-chain polysulfides (LiPSs, Li 2 S n , 4 ≤ n ≤ 8), low sulfur utilization, and large volume expansion (≈80%), which are critically fatal for the cycle stability and power density. [5] In the last decades, tremendous Lithium-sulfur batteries (LSBs) are severely impeded by their poor cycling stability and low sulfur utilization due to the inevitable polysulfide shuttle effect and sluggish reaction kinetics. This work reports a Mott-Schottky RGO-PANI/MoS 2 (RPM) heterogeneous layer modified separator for commercialsulfur-based LSBs through the vertical growth of molybdenum sulfide (MoS 2 ) arrays on the polyaniline (PANI) in situ reduced graphene oxide (RGO). Due to the synergistic effects of the "reservoir" constructed by MoS 2 and RGO-PANI, strong absorbability, high conductivity, and electrocatalytic activity, RPM exhibits a successive "trapping-interception-conversion" behavior toward lithium polysulfides. As a result, the LSBs assembled using a commercialsulfur as the cathode and RPM as modified layer exhibit high sulfur utilization (3.8 times higher than that of the unmodified separator at 5 C), excellent rate performance (553 mAh g −1 at 10 C), and outstanding high-rate cycle stability (524 mAh g −1 after 700 cycles at 5 C). Moreover, even at a high sulfur loading of 5.4 mg cm −2 , a favorable areal capacity of 3.8 mAh cm −2 is still maintained after 80 cycles. Theoretical calculations elucidate that such a systematic strategy can effectively suppress the shuttling effect and boost the catalytic conversion of intercepted polysulfides. This work may provide a feasible strategy to promote the practical application of commercial-sulfur-based LSBs.

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Section: Electrochemical Propertiesmentioning

confidence: 99%

A Mott–Schottky Heterogeneous Layer for Li–S Batteries: Enabling Both High Stability and Commercial‐Sulfur Utilization

Shi

Zheng

Zhang

et al. 2022

Advanced Energy Materials

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“…3(c), the N 1s spectra was deconvoluted into four peaks located at 398.3, 400.08, 401.5 and 399.08 eV, which could be ascribed to pyridinic N, pyrrolic N, graphitic N and the N-Fe/Ni bond, respectively. 20,36 Fig. 3(d) shows the Fe 2p XPS spectrum, in which four types of characteristic peaks were ascribed to the Fe–N bonds at 710.32 eV (2p 3/2 ) and 723.89 eV (2p 1/2 ), the Fe 2+ at 712.29 eV (2p 3/2 ), and the Fe 3+ at 725.89 eV (2p 1/2 ).…”

Section: Resultsmentioning

confidence: 99%

“…[13][14][15] In particular, g 0 -Fe 4 N has become a research hotspot in the fields of spintronic devices and magnetic energy storage due to its advantages of a high saturation magnetization (208 emu g À1 ) which is close to that of a-Fe (218 emu g À1 ), and its unique crystal structure which is similar to that of anti-perovskite. 3,[16][17][18][19][20] In general, g 0 -Fe 4 N has a facecentered cubic structure, which is equivalent to embedding a nitrogen atom in the center of the octahedron of the face-centered cubic g-Fe, which endows it with metal-like properties. 14,21,22 In addition, g 0 -Fe 4 N has attracted increasing attention in the field of electrochemical catalysis due to its special metal-like properties, and many composites associated with g 0 -Fe 4 N have been found to be efficient catalysts for the oxygen evolution reaction (OER) and oxygen reduction reaction (ORR).…”

Section: Introductionmentioning

confidence: 99%

(Fe_xNi_1−x)₄N nanoparticles: magnetism and electrocatalytic properties for the oxygen evolution reaction

et al. 2022

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“…Among them, iron derivatives are preferred due to their eco-benign, highly conductive, and high electrocatalytic activity nature. For example, Fe derivatives such as Fe/Fe 3 C supported over carbon- and phosphorus-doped FeN 4 /graphene have been reported as an effective interlayer and sulfur host for Li–S batteries, respectively . In addition, the polar nature of Fe 2 N due to the presence of the N atom with Fe could effectively mitigate the LIPS dissolution through an excellent chemical and physical immobilization of LIPSs.…”

Section: Introductionmentioning

confidence: 99%

In-situ Formed Polar Fe₂N/MCMB Hybrid Interlayer for High-Rate Li–S Batteries

Muralidharan

Kalaiselvi

2021

Energy Fuels

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Owing to its high theoretical capacity (1675 mA h g −1 ) and high theoretical energy density (2600 W h kg −1 ), lithium−sulfur (Li−S) batteries receive intense attention as an alternate to current lithium-ion batteries (LIBs). Sulfur, a surplus byproduct from petroleum industry along with an earth-abundant nature, ensures the low-cost production of Li−S batteries compared to LIBs. However, the common technical hurdles associated with sulfur such as low conductivity and poor cyclability due to the polysulfide shuttling effect hinder the realistic applications. In the current work, cashewnut sheath-derived biocarbon (CNS) is utilized as a host material for sulfur cathodes, in order to enhance the conductivity and to realize better electrochemical performance, especially at low current rates. For instance, a 50 wt % sulfur-loaded CNS cathode (CNS50S) shows a high specific capacity of 680 mA h g −1 at C/10 rate even after 700 cycles with a gravimetric energy density of 415 W h kg −1 . When the in situ formed polar Fe 2 N/MCMB was introduced as an interlayer, excellent electrochemical performance is obtained for CNS@SS cathodes even at high rates due to the effective mitigation of lithium polysulfide dissolution and efficient reutilization of absorbed polysulfides on the interlayer surface. For example, CNS50SIL and CNS60SIL cathodes deliver a specific capacity of 343 and 518 mA h g −1 at a high rate of 1C even after 120 cycles, respectively. This study offers ample scope to exploit CNS@SS composite cathodes for real-time applications and throws light on the importance of custom-designed Fe-based polar interlayers in improving the electrochemical behavior of Li−S batteries in terms of capacity at high rates.

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Phosphorus-modified Fe₄N@N,P co-doped graphene as an efficient sulfur host for high-performance lithium–sulfur batteries

Abstract: Lithium-sulfur batteries have attracted increasing attention in the field of energy storage due to their advantages of high specific energy and energy density. However, there are still many difficulties in...

Cited by 42 publications

References 55 publications

A Mott–Schottky Heterogeneous Layer for Li–S Batteries: Enabling Both High Stability and Commercial‐Sulfur Utilization

A Mott–Schottky Heterogeneous Layer for Li–S Batteries: Enabling Both High Stability and Commercial‐Sulfur Utilization

(Fe_xNi_1−x)₄N nanoparticles: magnetism and electrocatalytic properties for the oxygen evolution reaction

In-situ Formed Polar Fe₂N/MCMB Hybrid Interlayer for High-Rate Li–S Batteries

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Phosphorus-modified Fe4N@N,P co-doped graphene as an efficient sulfur host for high-performance lithium–sulfur batteries

Abstract: Lithium-sulfur batteries have attracted increasing attention in the field of energy storage due to their advantages of high specific energy and energy density. However, there are still many difficulties in...

Cited by 42 publications

References 55 publications

A Mott–Schottky Heterogeneous Layer for Li–S Batteries: Enabling Both High Stability and Commercial‐Sulfur Utilization

A Mott–Schottky Heterogeneous Layer for Li–S Batteries: Enabling Both High Stability and Commercial‐Sulfur Utilization

(FexNi1−x)4N nanoparticles: magnetism and electrocatalytic properties for the oxygen evolution reaction

In-situ Formed Polar Fe2N/MCMB Hybrid Interlayer for High-Rate Li–S Batteries

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Phosphorus-modified Fe₄N@N,P co-doped graphene as an efficient sulfur host for high-performance lithium–sulfur batteries

(Fe_xNi_1−x)₄N nanoparticles: magnetism and electrocatalytic properties for the oxygen evolution reaction

In-situ Formed Polar Fe₂N/MCMB Hybrid Interlayer for High-Rate Li–S Batteries