Nitride MXenes as sulfur hosts for thermodynamic and kinetic suppression of polysulfide shuttling: a computational study

Fan, Kefeng; Ying, Yiran; Luo, Xin; Huang, Haitao

doi:10.1039/d1ta06759a

Cited by 40 publications

(42 citation statements)

References 50 publications

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“…It reported that V 2 NS 2 has a good catalytic effect for SRR with a largest positive ΔG barrier value of 0.49 eV. 23 However, at the same time, the catalytic ability of V 2 NS 2 for decomposition of Li 2 S (1.19 eV) is much larger than that of Nb 2 CO 2 (0.558 eV). In terms of diffusion of Li + , the diffusion barrier value of Li + on the Nb 2 CO 2 substrate (0.231 eV) is between that of Ti 2 CO 2 (0.256 eV) and V 2 NO 2 (0.21 eV), and the decomposition barrier of Li 2 S catalyzed by Nb 2 CO 2 (0.558 eV) is also between that of Ti 2 CO 2 (0.565 eV) and V 2 NO 2 (1.55 eV), but the catalytic effect of Nb 2 CO 2 for SRR is the best.…”

Section: ■ Results and Discussionmentioning

confidence: 99%

“…Because in addition to the anchoring ability, the effect of MXenes hosts on the SRR during discharging and the decomposition of Li 2 S during charging should also be investigated. Recently, different functional V 2 NT 2 MXenes have been investigated which could accelerate the decomposition of Li 2 S and Li ion kinetics, especially S-terminated V 2 NS 2 has the lowest Gibbs free energy barrier (Δ G ) for SRR . However, the ability of V 2 NS 2 to catalyze the decomposition of Li 2 S is limited (1.19 eV), which is much higher than that of Ti-based MXenes (such as 0.411 eV for Ti 3 C 2 O 2 and 0.351 eV for Ti 3 C 2 S 2 ).…”

Section: Introductionmentioning

confidence: 99%

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Non-Negligible Role of Multifunctional MXene Hosts for Li–S Batteries: Anchoring and Electrocatalysis

et al. 2022

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Lithium−sulfur (Li−S) batteries have attracted great enthusiasm in recent years. Nevertheless, the serious shuttle effect of lithium polysulfides (Li 2 S n ), poor conductivity of S and intermediate products, and relatively slow dynamics make its commercial application face severe challenges. Here, functionalized M 2 CT 2 MXenes (M = Ti, Nb, Cr; T = bare, O, F, OH) were used as the sulfur host to build multifunctional cathodes, in which the inhibition of the shuttle effect by the anchoring effect and accelerating discharging/charging kinetics by electrocatalysis were studied via first-principles. The strong anchoring strength of M 2 CO 2 /M 2 CF 2 to Li 2 S n could effectively suppress the shuttle behavior. The anchoring ability of MXenes is a double-edged sword, and moderate anchoring strength should be considered. Compared comprehensively, Nb 2 CO 2 has a better electrocatalysis performance for the sulfur reduction reaction during discharging. It also accelerates the decomposition of Li 2 S and migration of Li + on the cathode which increases charging kinetics. The improvement in kinetics is related to the enhancement of electronic conductivities of Nb 2 CO 2 −Li 2 S n composites. In short, Nb 2 CO 2 -based multifunctional sulfur cathodes effectively suppress the shuttle effect and improve reaction kinetics. This work expands the application of the MXene family, especially providing guidelines for the utilization of Nb-based MXene in energy storage.

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Section: ■ Results and Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Non-Negligible Role of Multifunctional MXene Hosts for Li–S Batteries: Anchoring and Electrocatalysis

et al. 2022

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“…This phenomenon is further confirmed by calculating the ratio of chemical and physical interaction (Van der Waals force) according to the formula

RvdW = ((), E_{ads}^{vdW} - E_{ads}^{italicno italicvdW}) / E_{ads}^{vdW} \times 100 %

(Figure 3G). 35 For MXene/graphene, the contribution of Van der Waals force increases sharply with sulfur atoms, approaching 100% for S 8 , which is opposite to the trend of adsorption energy.…”

Section: Resultsmentioning

confidence: 85%

In‐situ growth of ultrathin sulfur microcrystal on MXene‐based 3D matrice for flexible lithium–sulfur batteries

Xia

Chen

Yang

et al. 2022

EcoMat

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Lithium–sulfur batteries (Li‐S batteries) are promising next‐generation energy storage systems because of their high‐theoretical energy density. However, the commercialization of Li‐S batteries is still impeded by the aggregation of sulfur, low‐sulfur utilization, shuttling of dissolved polysulfides and sluggish reaction kinetics. Herein, we designed a hierarchically maple leaf‐like structured sulfur electrodes by in‐situ growth of ultrathin sulfur microcrystal on two‐dimensional MXene‐graphene‐cellulose nanofiber (MGN) matrice (denoted as IS‐MGN@S). The sulfur microcrystal as cathode can achieve improved kinetics than bulk sulfur due to its few layers of sulfur atoms, which is proved by the density functional theory calculations. The MXene not only confines polysulfides through strong chemisorption but also promotes the catalytic conversion of polysulfides. The introduction of graphene improves the conductivity and boosts the immobilization and conversion of polysulfides. As a result, the IS‐MGN@S cathode demonstrates remarkable electrochemical properties with a high‐initial capacity (1229 mAh g−1 at 0.2C), substantial improvement in rate capability (770 mAh g−1 at 2C), and stable long‐term cycling capacity. Moreover, the pouch cells with IS‐MGN@S cathode and gel electrolyte demonstrate excellent mechanical properties under mechanical damage (nail & cut tests, severe deformations), suggesting their promising applications for wearable electronic devices.

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“…37,43 DFT computations predict that non-carbide MXenes exhibit properties superior to carbide MXenes, thus exhibiting the potential to be used in various elds. [44][45][46] A comprehensive overview of the synthesis methods adopted so far in producing non-carbide MXenes and their properties will be discussed in the subsequent sections of this review.…”

Section: Challenges In Synthesismentioning

confidence: 99%

2D non-carbide MXenes: an emerging material class for energy storage and conversion

et al. 2022

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Nitride MXenes as sulfur hosts for thermodynamic and kinetic suppression of polysulfide shuttling: a computational study

Abstract: The practical applications of lithium-sulfur (Li–S) batteries are greatly hindered by the poor conductivity of sulfur, the shuttling of lithium polysulfides (LiPSs), and the sluggish kinetics in charge-discharge process. In...

Cited by 40 publications

References 50 publications

Non-Negligible Role of Multifunctional MXene Hosts for Li–S Batteries: Anchoring and Electrocatalysis

Non-Negligible Role of Multifunctional MXene Hosts for Li–S Batteries: Anchoring and Electrocatalysis

In‐situ growth of ultrathin sulfur microcrystal on MXene‐based 3D matrice for flexible lithium–sulfur batteries

2D non-carbide MXenes: an emerging material class for energy storage and conversion

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