Metallic FeCo clusters propelling the stepwise polysulfide conversion in lithium–sulfur batteries

Li, Min-Hui; Wang, Hui; Wang, Xuyun; Ren, Jianwei; Wang, Rongfang

doi:10.1039/d2ta05273c

Cited by 18 publications

(8 citation statements)

References 55 publications

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“…This result may be attributed to the heavy aggregation of metallic Co nanoparticles with the rise in the calcination temperature, thereby leading to the formation of large-size particles, displaying a distinct diffraction peak in the XRD pattern. Therefore, we could deduce that a minor feature of Co-species in the final products at a relatively low temperature was achieved, meanwhile giving rise to strong chemical adsorption/catalyzation conversion toward polysulfides due to enhanced surface energy and abundant active sites [ 29 , 31 ].…”

Section: Resultsmentioning

confidence: 99%

“…Specifically, recent studies have demonstrated that tailoring metal compounds to an ultra-small size, such as nanocrystals, nanodots, and clusters, and even to the single-atomic scale could generate strong adsorption and excellent catalytic activity for polysulfides, owing to enhanced surface energy and more active terminations [ 16 , 29 , 30 , 31 ]. However, it is a great challenge to fabricate highly dispersed ultrafine metal compounds because the isolated ultra-small particles with high surface energy can susceptibly agglomerate into big particles in the synthesis process.…”

Section: Introductionmentioning

confidence: 99%

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Ultrafine Co-Species Interspersed g-C3N4 Nanosheets and Graphene as an Efficient Polysulfide Barrier to Enable High Performance Li-S Batteries

2023

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Lithium-sulfur (Li-S) batteries are regarded as one of the promising advanced energy storage systems due to their ultrahigh capacity and energy density. However, their practical applications are still hindered by the serious shuttle effect and sluggish reaction kinetics of soluble lithium polysulfides. Herein, g-C3N4 nanosheets and graphene decorated with an ultrafine Co-species nanodot heterostructure (Co@g-C3N4/G) as separator coatings were designed following a facile approach. Such an interlayer can not only enable effective polysulfide affinity through the physical barrier and chemical binding but also simultaneously have a catalytic effect on polysulfide conversion. Because of these superior merits, the Li-S cells assembled with Co@g-C3N4/G-PP separators matched with the S/KB composites (up to ~70 wt% sulfur in the final cathode) exhibit excellent rate capability and good cyclic stability. A high specific capacity of ~860 mAh g−1 at 2.0 C as well as a capacity-fading rate of only ~0.035% per cycle over 350 cycles at 0.5 C can be achieved. This bifunctional separator can even endow a Li-S cell at a low current density to exhibit excellent cycling capability, with a capacity retention rate of ~88.4% at 0.2 C over 250 cycles. Furthermore, a Li-S cell with a Co@g-C3N4/G-PP separator possesses a stable specific capacity of 785 mAh g−1 at 0.2 C after 150 cycles and a superior capacity retention rate of ~84.6% with a high sulfur loading of ~3.0 mg cm−2. This effective polysulfide-confined separator holds good promise for promoting the further development of high-energy-density Li-S batteries.

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Section: Resultsmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Ultrafine Co-Species Interspersed g-C3N4 Nanosheets and Graphene as an Efficient Polysulfide Barrier to Enable High Performance Li-S Batteries

2023

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“…In contrast, by alloying with different metal species, the alloy has attracted great interest in catalyzing polysulfides owing to its tunable electronic structures. [171,172,[178][179][180] The low-cost Ni-Fe alloy was shown to function as an efficient electrocatalyst to accelerate sulfur conversion kinetics in Li-S batteries. [99,181] Impressively, a reconstructed layer of Ni/ Fe sulfide was detected on the surface of Ni-Fe alloy during the charge/discharge process.…”

Section: Metals/alloysmentioning

confidence: 99%

“…Metal has a certain potential in regulating polysulfide intermediates because of their high electrical conductivity and affinity with the sulfur atoms of polysulfides. [95,171,172] The pioneering work by Arava et al first proposed the concept of electrocatalysts using noble metal platinum (Pt) for Li-S batteries. They found that the Pt nanoparticles could accelerate the conversion of dissolved polysulfides.…”

Section: Metals/alloysmentioning

confidence: 99%

In Situ Reconstruction of Electrocatalysts for Lithium–Sulfur Batteries: Progress and Prospects

Zhang

Wang

et al. 2023

Adv Funct Materials

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The current research of Li–S batteries primarily focuses on increasing the catalytic activity of electrocatalysts to inhibit the polysulfide shuttling and enhance the redox kinetics. However, the stability of electrocatalysts is largely neglected, given the premise that they are stable over extended cycles. Notably, the reconstruction of electrocatalysts during the electrochemical reaction process has recently been proposed. Such in situ reconstruction process inevitably leads to varied electrocatalytic behaviors, such as catalytic sites, selectivity, activity, and amounts of catalytic sites. Therefore, a crucial prerequisite for the design of highly effective electrocatalysts for Li–S batteries is an in‐depth understanding of the variation of active sites and the influence factors for the in situ reconstruction behaviors, which has not achieved a fundamental understanding and summary. This review comprehensively summarizes the recent advances in understanding the reconstruction behaviors of different electrocatalysts for Li–S batteries during the electrochemical reaction process, mainly including metal nitrides, metal oxides, metal selenides, metal fluorides, metals/alloys, and metal sulfides. Moreover, the unexplored issues and major challenges of understanding the reconstruction chemistry are summarized and prospected. Based on this review, new perspectives are offered into the reconstruction and true active sites of electrocatalysts for Li–S batteries.

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“…Our previous studies showed that materials composed of Fe and Co easily bonded with LiPSs, and the similar electronic structures of Fe and Co tended to exchange electrons with the outside while avoiding possible phase segmentation, which was very consistent with the basic requirements for efficient catalysis of LiPSs. 34,35 However, the choice of anions needed to be further considered. Although metal oxides and nitrides had some benets for the bidirectional catalytic kinetics of LSBs, the enhancement effect was limited.…”

Section: Introductionmentioning

confidence: 99%

Efficient immobilization and bidirectional catalysis of polysulfide conversion by FeCoP quantum dots for lithium–sulfur batteries

Wang

et al. 2023

J. Mater. Chem. A

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Metallic FeCo clusters propelling the stepwise polysulfide conversion in lithium–sulfur batteries

Abstract: Catalytic conversion of polysulfide is considered to be an important way to improving the kinetics and inhibiting the shuttle effect of lithium-sulfur batteries (LSB). In this work, the 3D FeCo/PNC...

Cited by 18 publications

References 55 publications

Ultrafine Co-Species Interspersed g-C3N4 Nanosheets and Graphene as an Efficient Polysulfide Barrier to Enable High Performance Li-S Batteries

Ultrafine Co-Species Interspersed g-C3N4 Nanosheets and Graphene as an Efficient Polysulfide Barrier to Enable High Performance Li-S Batteries

In Situ Reconstruction of Electrocatalysts for Lithium–Sulfur Batteries: Progress and Prospects

Efficient immobilization and bidirectional catalysis of polysulfide conversion by FeCoP quantum dots for lithium–sulfur batteries

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