Visualization of regulated nucleation and growth of lithium sulfides for high energy lithium sulfur batteries

Xu, Zheng; Kim, Sung Joo; Chang, Donghee; Park, Kyu‐Young; Dae, Kyun Seong; Dao, Khoi Phuong; Yuk, Jong Min; Kang, Kisuk

doi:10.1039/c9ee01338e

Cited by 108 publications

(86 citation statements)

References 53 publications

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“…Typical synthetic routes mainly rely on template-assisted selective etching fabrication, 7,8,11,12,14,17,[23][24][25][26][27] or sometimes with a post loading (Scheme S1). [28][29][30] Despite their applicability, they are restricted by tedious multistep procedures and high cost.…”

Section: Progress and Potentialmentioning

confidence: 99%

“…The pursuit of ultrafine MNPs could achieve more exposed active sites for boosting their catalytic, electronic, and kinetic properties in many applications. As far as electrochemical energy storage is concerned, conductive hollow shell and small MNPs enable rapid charge transfer and fast kinetics, and the cavity serves as nanospace for confinement and buffers destructive volume expansion to mitigate capacity fading; 8,[10][11][12][13][14][15][16] the small MNPs also function as an active site for guiding electrochemical processes, such as catalytic conversion of polysulfide in sulfur-based cathode [17][18][19] and selective nucleation for dendrite-free metal anode. 7,18,[20][21][22] Driven by the potential breakthroughs, continuous effort has been dedicated to the exploration of suitable synthetic protocols for well-defined HHSs.…”

Section: Introductionmentioning

confidence: 99%

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Generalized Domino-Driven Synthesis of Hollow Hybrid Carbon Spheres with Ultrafine Metal Nitrides/Oxides

Ding

Qiu

et al. 2020

Matter

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We have demonstrated an ingenious one-pot aqueous domino-driven synthesis toward hollow hybrid spheres with ultrafine metal nitrides/oxides in hollow carbon cavity. The micelle-interfacial copolymerization is applied for shell formation, while the copolymerization-generated H + spontaneously triggers oxometallate condensation for encapsulation. By regulating the synthetic conditions, the encapsulated metal species can be well tailored with different sizes/contents (nanocluster to several nanometers) and compositions (VN, VO, MoN, WN, bimetal-based nitrides). The ultrafine VN confined in hollow carbon exhibits excellent potassium storage performance.

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Section: Progress and Potentialmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Generalized Domino-Driven Synthesis of Hollow Hybrid Carbon Spheres with Ultrafine Metal Nitrides/Oxides

Ding

Qiu

et al. 2020

Matter

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“…As shown in Fig. 2A, the CV pro le of the Zn(OAc) 2 •DEA based cathode at a scan rate of 0.1 mV s -1 showed the typical two pairs of cathodic/anodic peaks, corresponding to the two-step reversible redox reaction between elemental sulfur (S 8 ) and Li 2 S 29,30 . The PVDF based cathode also showed two pairs of redox peaks; however, both reduction and oxidation peaks, particularly the second reduction and oxidation peaks, are much delayed.…”

Section: Introductionmentioning

confidence: 95%

Zinc Complex Based Multifunctional Reactive Lithium Polysulfide Trapper Approaching Its Theoretical Efficiency

Zuo

2020

Preprint

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The “shuttle effect” of soluble lithium polysulfides (LPS), which causes rapid capacity fading, remains a lingering issue for lithium-sulfur batteries (LSBs). Herein, we report a new type of reactive molecule-based (or molecular) LPS trapper, zinc acetate-diethanolamine (Zn(OAc)2·DEA), which demonstrated a molecular efficiency of 1.8 for LPS trapping, approaching its theoretical limit of 2. This is the highest trapping capability among all reported LPS trappers. During discharge the trapped polysulfides are much more thermodynamically favored for reduction compared to the non-trapped ones, while during charge the complex Zn(SLi)2·DEA formed in the previous discharging process can be more easily oxidized due to its lower energy barrier in comparison to Li2S, indicating the catalytic effects of Zn2+·DEA on the redox of sulfur species. Zn(OAc)2·DEA is also an excellent binder owing to its multiple intermolecular hydrogen bonds. LSBs using Zn(OAc)2·DEA as a LPS trapper, a binder, and a redox catalyst exhibited excellent long-term cycling stability (with a capacity retention of 85% after 1000 cycles at a rate of 0.5 C) and enhanced rate performance. The work demonstrated the potential of this novel type of multifunctional metal complex-based reactive molecular LPS trappers for high capacity and stable LSBs.

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“…Elemental sulfur is one of the most significant byproducts of the large petroleum industry; moreover, sulfur is benign from an environmental perspective [ 6 ]. From a chemical point of view, sulfur, as an active material, causes a multistep redox reaction in charge and discharge mechanisms [ 7 ]. Each sulfur atom provides two electrons; thus, LSBs retain their high specific capacity and energy density, where the active material of LIBs generates a single electron [ 8 , 9 ].…”

Section: Introductionmentioning

confidence: 99%

“…It is incredible to note that the defective nature of amorphous carbon provides a substantial effect on electrochemical performance. Polysulfides prefer to bond on defective sites (vacant monosite: adsorption energy of Li 2 S 4 : −0.62 eV; Li 2 S: −3.35 eV) where the polysulfides are trapped, boosted, and reduced into lithium sulfide [ 7 ]. A functionalized carbon nanotube (CNT) was coated with a uniform ZnS nanoparticle working as a sulfur host by chemical adsorption, which mitigated the shuttle effect [ 23 ].…”

Section: Introductionmentioning

confidence: 99%

Microporous Carbon Nanoparticles for Lithium–Sulfur Batteries

et al. 2020

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Rechargeable lithium–sulfur batteries (LSBs) are emerging as some of the most promising next-generation battery alternatives to state-of-the-art lithium-ion batteries (LIBs) due to their high gravimetric energy density, being inexpensive, and having an abundance of elemental sulfur (S8). However, one main, well-known drawback of LSBs is the so-called polysulfide shuttling, where the polysulfide dissolves into organic electrolytes from sulfur host materials. Numerous studies have shown the ability of porous carbon as a sulfur host material. Porous carbon can significantly impede polysulfide shuttling and mitigate the insulating passivation layers, such as Li2S, owing to its intrinsic high electrical conductivity. This work suggests a scalable and straightforward one-step synthesis method to prepare a unique interconnected microporous and mesoporous carbon framework via salt templating with a eutectic mixture of LiI and KI at 800 °C in an inert atmosphere. The synthesis step used environmentally friendly water as a washing solvent to remove salt from the carbon–salt mixture. When employed as a sulfur host material, the electrode exhibited an excellent capacity of 780 mAh g−1 at 500 mA g−1 and a sulfur loading mass of 2 mg cm−2 with a minor capacity loss of 0.36% per cycle for 100 cycles. This synthesis method of a unique porous carbon structure could provide a new avenue for the development of an electrode with a high retention capacity and high accommodated sulfur for electrochemical energy storage applications.

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Visualization of regulated nucleation and growth of lithium sulfides for high energy lithium sulfur batteries

Abstract: The nucleation and growth of lithium sulfides are directly observed by liquid in situ transmission electron microscopy.

Cited by 108 publications

References 53 publications

Generalized Domino-Driven Synthesis of Hollow Hybrid Carbon Spheres with Ultrafine Metal Nitrides/Oxides

Generalized Domino-Driven Synthesis of Hollow Hybrid Carbon Spheres with Ultrafine Metal Nitrides/Oxides

Zinc Complex Based Multifunctional Reactive Lithium Polysulfide Trapper Approaching Its Theoretical Efficiency

Microporous Carbon Nanoparticles for Lithium–Sulfur Batteries

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