Atomic Iron Catalysis of Polysulfide Conversion in Lithium–Sulfur Batteries

Liu, Zhenzhen; Zhou, Lei; Ge, Qi; Chen, Renjie; Ni, Mei; Utetiwabo, Wellars; Zhang, Xiaoling; Yang, Wen

doi:10.1021/acsami.8b03830

Cited by 167 publications

(140 citation statements)

References 31 publications

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“…Atomic‐scale electrocatalysts in Li–S batteries are strongly considered to enhance redox kinetics of sulfur conversion, as the atomically dispersed active sites on substrates can maximize the atom‐utilization efficiency for sulfur species modulation and curtail inert dosage in electrodes . Single cobalt and iron atoms coordinated with nitrogen have been explored as electrocatalysts to enhance kinetic conversion from LiPSs to Li 2 S and mitigate LiPS shuttle. However, kinetic understanding of the electrocatalytic capabilities of atomic electrocatalysts for Li–S batteries is rather limited, yet critically important to rational design of high‐efficiency electrocatalysts in Li–S batteries.…”

Section: Introductionmentioning

confidence: 99%

Expediting redox kinetics of sulfur species by atomic‐scale electrocatalysts in lithium–sulfur batteries

Kong

Chang-xin

et al. 2019

InfoMat

282

170

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Lithium–sulfur (Li–S) batteries have extremely high theoretical energy density that make them as promising systems toward vast practical applications. Expediting redox kinetics of sulfur species is a decisive task to break the kinetic limitation of insulating lithium sulfide/disulfide precipitation/dissolution. Herein, we proposed a porphyrin‐derived atomic electrocatalyst to exert atomic‐efficient electrocatalytic effects on polysulfide intermediates. Quantifying electrocatalytic efficiency of liquid/solid conversion through a potentiostatic intermittent titration technique measurement presents a kinetic understanding of specific phase evolutions imparted by the atomic electrocatalyst. Benefiting from atomically dispersed “lithiophilic” and “sulfiphilic” sites on conductive substrates, the finely designed atomic electrocatalyst endows Li–S cells with remarkable cycling stablity (cyclic decay rate of 0.10% in 300 cycles), excellent rate capability (1035 mAh g−1 at 2 C), and impressive areal capacity (10.9 mAh cm−2 at a sulfur loading of 11.3 mg cm−2). The present work expands atomic electrocatalysts to the Li–S chemistry, deepens kinetic understanding of sulfur species evolution, and encourages application of emerging electrocatalysis in other multielectron/multiphase reaction energy systems.

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Section: Introductionmentioning

confidence: 99%

Expediting redox kinetics of sulfur species by atomic‐scale electrocatalysts in lithium–sulfur batteries

Kong

Chang-xin

et al. 2019

InfoMat

282

170

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“…Iron carbide (Fe 3 C) is a robust material that has attracted increasing attention because of its abundance and low cost, and more importantly, its inherent characteristics of high electronic conductivity due to it being a metal-like material [33,34]. Furthermore, Fe 3 C could be an effective polysulfide adsorbent if strong Fe-S bonds can be formed between Fe 3 C and polysulfides [35,36]. Herein, a facile one-step carbonizing process is used to synthesize a porous and conductive nanocomposite where Fe 3 C nanoparticles are embedded onto nitrogen-doped porous carbon sheets (i.e.…”

Section: Introductionmentioning

confidence: 99%

Polar and conductive iron carbide@N-doped porous carbon nanosheets as a sulfur host for high performance lithium sulfur batteries

Wang

et al. 2019

Chemical Engineering Journal

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The practical application of Li-S battery is inherently limited by the low conductivity of sulphur and the dissolution of polysulfides. The enhancement of conductivity and introduction of polarity to sulphur host is an effective strategy to overcome this long-standing challenges. In this work, a facile one-step carbonizing process is used to synthesize a unique porous and conductive nanocomposite where Fe 3 C nanoparitcles is embedded in nitrogen-doped porous carbon sheets (Fe 3 C@NPCS). As demonstrated in Li 2 S 4 adsorption experiments and confirmed by density functional theory calculations, Fe 3 C nanoparticles are able to strongly adsorb polysulfides via strong Fe-S chemical bonds. Due to the remarkable conductivity, Fe 3 C nanoparticles can also accelerate the electrochemical reactions of the polysulfides through fast electron transportation. The carbon sheets prevent the aggregation of Fe 3 C nanoparticles in the synthesis, and accommodate sulfur and its volume expansion during charge/discharge. With these features, the resultant sulfur cathodes (Fe 3 C@NPCS-S) deliver an excellent cycling performance with a capacity decay of 0.036% per cycle, and high rate performance of ca. 1127, 1020, 907, 802, 731 and 647 mAh g-1 under the current density of 0.3, 0.5, 1, 2, 3 and 5 Crate , respectively.

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“…The composites delivered initial areal specific capacities of 2.22, 5.52, and 9.43 mAh cm -2 . Most interestingly, it is found statistically that the positions of the reported sulfur cathode materials are distributed in a straight line with a slope of 1090 mAh g -1 , and the Ni-N/G composite is located above the straightness, indicating its superior performance (Figure 4(d) and Table S9) [11,[13][14][15][35][36][37][38][39][40][41][42][43][44][45][46][47][48][49][50][51]. Moreover, the S@Ni-N/G cathode with high sulfur loading of 2.3 mg cm -2 under 0.1 C shows good cycling performances and deliver the discharge capacities of 734 mAh g -1 after cycling for 150 cycles, namely, 1460 h, and the corresponding capacity retentions are 76.1% compared to the initial cycle.…”

Section: Adsorption Experiments and Theoretical Calculationsmentioning

confidence: 92%

Selective Adsorption and Electrocatalysis of Polysulfides through Hexatomic Nickel Clusters Embedded in N-Doped Graphene toward High-Performance Li-S Batteries

Sha

et al. 2020

Research

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The shuttle effect hinders the practical application of lithium-sulfur (Li-S) batteries due to the poor affinity between a substrate and Li polysulfides (LiPSs) and the sluggish transition of soluble LiPSs to insoluble Li2S or elemental S. Here, we report that Ni hexatomic clusters embedded in a nitrogen-doped three-dimensional (3D) graphene framework (Ni-N/G) possess stronger interaction with soluble polysulfides than that with insoluble polysulfides. The synthetic electrocatalyst deployed in the sulfur cathode plays a multifunctional role: (i) selectively adsorbing the polysulfides dissolved in the electrolyte, (ii) expediting the sluggish liquid-solid phase transformations at the active sites as electrocatalysts, and (iii) accelerating the kinetics of the electrochemical reaction of multielectron sulfur, thereby inhibiting the dissolution of LiPSs. The constructed S@Ni-N/G cathode delivers an areal capacity of 9.43 mAh cm-2 at 0.1 C at S loading of 6.8 mg cm-2, and it exhibits a gravimetric capacity of 1104 mAh g-1 with a capacity fading rate of 0.045% per cycle over 50 cycles at 0.2 C at S loading of 2.0 mg cm-2. This work opens a rational approach to achieve the selective adsorption and expediting of polysulfide transition for the performance enhancement of Li-S batteries.

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Atomic Iron Catalysis of Polysulfide Conversion in Lithium–Sulfur Batteries

Cited by 167 publications

References 31 publications

Expediting redox kinetics of sulfur species by atomic‐scale electrocatalysts in lithium–sulfur batteries

Expediting redox kinetics of sulfur species by atomic‐scale electrocatalysts in lithium–sulfur batteries

Polar and conductive iron carbide@N-doped porous carbon nanosheets as a sulfur host for high performance lithium sulfur batteries

Selective Adsorption and Electrocatalysis of Polysulfides through Hexatomic Nickel Clusters Embedded in N-Doped Graphene toward High-Performance Li-S Batteries

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