Nitrogen-Doped CoSe<sub>2</sub> as a Bifunctional Catalyst for High Areal Capacity and Lean Electrolyte of Li–S Battery

Wang, Maoxu; Fan, Longlong; Sun, Xun; Guan, Bin; Jiang, Bo; Wu, Xian; Tian, Da; Sun, Kening; Qiu, Yue; Yin, Xiaoju; Zhang, Yu; Zhang, Naiqing

doi:10.1021/acsenergylett.0c01564

Cited by 234 publications

(180 citation statements)

References 54 publications

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“…2a) [25]. This result is in accordance with most studies on Li-S batteries, in which cathode hosts are sulfurated at 155 °C [40][41][42]. In the case of the 300S, strong peaks at 23.8°, 24.1°, 24.4°, and 28.1° are indexed to the (212), ( 130), (012), and (132) planes of crystalline S (PDF: 04-007-2069), respectively.…”

Section: Characterization Of the 155s And 300ssupporting

confidence: 89%

Understanding Sulfur Redox Mechanisms in Different Electrolytes for Room-Temperature Na–S Batteries

et al. 2021

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This work reports influence of two different electrolytes, carbonate ester and ether electrolytes, on the sulfur redox reactions in room-temperature Na–S batteries. Two sulfur cathodes with different S loading ratio and status are investigated. A sulfur-rich composite with most sulfur dispersed on the surface of a carbon host can realize a high loading ratio (72% S). In contrast, a confined sulfur sample can encapsulate S into the pores of the carbon host with a low loading ratio (44% S). In carbonate ester electrolyte, only the sulfur trapped in porous structures is active via ‘solid–solid’ behavior during cycling. The S cathode with high surface sulfur shows poor reversible capacity because of the severe side reactions between the surface polysulfides and the carbonate ester solvents. To improve the capacity of the sulfur-rich cathode, ether electrolyte with NaNO3 additive is explored to realize a ‘solid–liquid’ sulfur redox process and confine the shuttle effect of the dissolved polysulfides. As a result, the sulfur-rich cathode achieved high reversible capacity (483 mAh g−1), corresponding to a specific energy of 362 Wh kg−1 after 200 cycles, shedding light on the use of ether electrolyte for high-loading sulfur cathode.

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Section: Characterization Of the 155s And 300ssupporting

confidence: 89%

Understanding Sulfur Redox Mechanisms in Different Electrolytes for Room-Temperature Na–S Batteries

et al. 2021

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“…The cells with the MCN/S cathode can still retain 691.1 mA h g −1 , which means a very low average capacity degradation (0.019%) per cycle, which is much higher than those of recent reported literatures based on different catalysts. [7,22,[45][46][47] This outstanding cyclicity shows the superior cycling stability of MCN/S at high current densities. To further demonstrate its practicality, Li-S pouch cells were assembled and operated at the conditions required for commercial highenergy Li-S batteries.…”

Section: Resultsmentioning

confidence: 95%

In Situ Construction of Mo₂C Quantum Dots‐Decorated CNT Networks as a Multifunctional Electrocatalyst for Advanced Lithium–Sulfur Batteries

Huang

Chen

Srinivas

et al. 2021

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The slow redox kinetics during cycling process and the serious shuttle effect caused by the solubility of lithium polysulfides (LiPSs) dramatically hinder the practical application of Li‐S batteries. Herein, a facile and scalable spray‐drying strategy is presented to construct conductive polar Mo2C quantum dots‐decorated carbon nanotube (CNT) networks (MCN) as an efficient absorbent and electrocatalyst for Li‐S batteries. The results reveal that the MCN/S electrode exhibits a high specific capacity of 1303.3 mAh g−1 at 0.2 C, and ultrastable cycling stability with decay of 0.019% per cycle even at 1 C. Theoretical simulation uncovers that Mo2C exhibits much stronger binding energies for S8 and Li2Sn. The energy barrier for the conversion between Li2S4 and Li2S2 decreases from 1.02 to 0.72 eV when hybriding with Mo2C. Furthermore, in situ discharge/charge‐dependent Raman spectroscopy shows that long‐chain Li2S8 configuration is generated via S8 ring opening near the first plateaus at ≈2.36 V versus Li/Li+ and the S62− configuration in CNT/S electrode is maintained below the potential of ≈2.30 V versus Li/Li+, indicating that the shuttle of soluble LiPSs happens during the whole discharge process. This work provides deep insights into the polar nanoarchitecture design and scalable fabrication for advanced Li‐S batteries.

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Section: Intrinsic Defectmentioning

confidence: 99%

“…To this end, Wang et al innovatively developed a dual-directional N-CoSe 2 electrocatalyst via anion doping strategy. [139] Of note, the bond lengths of various sulfur species (Li c) Reproduced with permission. [137] Copyright 2020, Wiley-VCH.…”

Section: Anion-doped Compoundmentioning

confidence: 99%

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Defect Engineering for Expediting Li–S Chemistry: Strategies, Mechanisms, and Perspectives

Shi

Sun

et al. 2021

Advanced Energy Materials

168

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as well as the cost-effectiveness and environmental-friendliness of sulfur resource. [1][2][3][4][5][6][7][8] However, a suite of troublesome problems, mainly pertaining to sluggish redox kinetics and severe polysulfide (PS) shuttle, has hampered the pathway for pursuing Li-S commercialization. [9][10][11][12][13] For one thing, the conversion from PS to Li 2 S exhibits large energy barriers, which is regarded as the rate-determining step of sulfur reduction reaction (SRR) process. For another, Li 2 S is prone to accumulating at the cathode side, which is not easy to be efficiently dissociated.Recent years have witnessed a burgeoning interest in designing adsorptive and electrocatalytic mediators for effective PS management in Li-S realm, in order to essentially expedite redox kinetics and inhibit "shuttle effect." [14][15][16][17][18][19][20] Although strenuous efforts have been devoted to exploring various types of PS mediators including carbonaceous materials, [21][22][23][24][25] metal oxides/carbides/nitrides/borides/ sulfides/selenides/phosphides, [26][27][28][29][30][31][32][33][34][35][36] and heterostructures, [37][38][39][40][41][42][43][44] their unsatisfactory adsorptive and catalytic behavior caused by insufficient active sites remains a huge barrier for obtaining favorable Li-S chemistry. To circumvent this problem, adjusting the morphology of PS mediators such as reducing their size to nanoscale has been recognized as a promising method to expose more active lattice planes and edge sites. Indeed, a myriad of PS mediators possessing ultrafine nanoparticle and ultrathin nanosheet architecture has been developed to efficiently adsorb sulfur species and catalyze PS conversion. [45][46][47][48][49] Furthermore, optimizing the electronic structure of PS mediator also serves as an appealing approach to boost electrochemical activities. [50][51][52][53][54] Defect engineering, an essential strategy to tailor the atomic distribution and dictate the surface property of nanomaterials, [55][56][57][58][59][60] plays a pivotal role in optimizing the electronic structure and promoting the electrochemical performance of catalysts in various scenarios including hydrogen evolution reaction (HER), oxygen evolution reaction (OER), oxygen reduction reaction (ORR), carbon dioxide reduction reaction (CO 2 RR), and nitrogen reduction reaction (NRR). [61][62][63][64][65][66][67][68][69][70][71][72] Very recently, defect engineering has stimulated a growing attention on PS mediator design in Li-S realm. Benefiting from a collection of compelling functionalities, defective mediator showcases remarkable promise in regulating PS behavior and realizing fast redox chemistry, thereby paving an innovative way toward practical applications of Li-S batteries.Lithium-sulfur (Li-S) batteries have stimulated a burgeoning scientific and industrial interest owing to high energy density and low materials costs. The favorable reaction kinetics of sulfur species is a key prerequisite for pursuing their commercialization. Recent years have ...

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Nitrogen-Doped CoSe₂ as a Bifunctional Catalyst for High Areal Capacity and Lean Electrolyte of Li–S Battery

Cited by 234 publications

References 54 publications

Understanding Sulfur Redox Mechanisms in Different Electrolytes for Room-Temperature Na–S Batteries

Understanding Sulfur Redox Mechanisms in Different Electrolytes for Room-Temperature Na–S Batteries

In Situ Construction of Mo₂C Quantum Dots‐Decorated CNT Networks as a Multifunctional Electrocatalyst for Advanced Lithium–Sulfur Batteries

Defect Engineering for Expediting Li–S Chemistry: Strategies, Mechanisms, and Perspectives

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Nitrogen-Doped CoSe2 as a Bifunctional Catalyst for High Areal Capacity and Lean Electrolyte of Li–S Battery

Cited by 234 publications

References 54 publications

Understanding Sulfur Redox Mechanisms in Different Electrolytes for Room-Temperature Na–S Batteries

Understanding Sulfur Redox Mechanisms in Different Electrolytes for Room-Temperature Na–S Batteries

In Situ Construction of Mo2C Quantum Dots‐Decorated CNT Networks as a Multifunctional Electrocatalyst for Advanced Lithium–Sulfur Batteries

Defect Engineering for Expediting Li–S Chemistry: Strategies, Mechanisms, and Perspectives

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Nitrogen-Doped CoSe₂ as a Bifunctional Catalyst for High Areal Capacity and Lean Electrolyte of Li–S Battery

In Situ Construction of Mo₂C Quantum Dots‐Decorated CNT Networks as a Multifunctional Electrocatalyst for Advanced Lithium–Sulfur Batteries