Fast conversion and controlled deposition of lithium (poly)sulfides in lithium-sulfur batteries using high-loading cobalt single atoms

Li, Yuan‐Jian; Wu, Jiabin; Bao, Zhenan; Wang, Wenyu; Zhang, Guoqun; Seh, Zhi Wei; Zhang, Nian; Sun, Jie; Huang, Liang; Jian-jun, Jiang; Zhou, Jun; Sun, Yongming

doi:10.1016/j.ensm.2020.05.022

Cited by 310 publications

(245 citation statements)

References 66 publications

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“…Thus, a suitable substrate, which can offer strong metal‐support interactions, is essential for the synthesis of high metal loading SACs. Besides, smart strategies are required to prepare high metal loading SACs [27,94–97] . Usually, atoms like nitrogen (N) [98] and sulfur (S) [99] that contain lone pairs of electrons, have robust coordination ability with metal atoms, serving as coordination sites to stabilize single metal atoms.…”

Section: Synthesis Strategies Of High Metal Loading Sacsmentioning

confidence: 99%

“…Besides, smart strategies are required to prepare high metal loading SACs. [27,[94][95][96][97] Usually, atoms like nitrogen (N) [98] and sulfur (S) [99] that contain lone pairs of electrons, have robust coordination ability with metal atoms, serving as coordination sites to stabilize single metal atoms. Therefore, constructing coordination atoms, as anchoring sites, is an effective approach to synthesizing high metal loading SACs.…”

Section: Synthesis Strategies Of High Metal Loading Sacsmentioning

confidence: 99%

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Synthesis of High Metal Loading Single Atom Catalysts and Exploration of the Active Center Structure

Wang

Liu

2020

ChemCatChem

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Single‐atom catalysts (SACs) have been rising recently as a new frontier in the catalysis field. Due to maximum atom utilization efficiency and tunable electronic structures, SACs exhibit highly distinctive catalytic performance from bulk counterparts. SACs with high metal loading will facilitate practical applications. To that end, this Review focuses on recent strategies to maximize metal loading. An appropriate substrate, mainly heteroatom‐doped carbon materials, is the key to avoiding aggregation or sintering during synthetic procedures. The coordination site construction and spatial confinement strategies are adopted to prepare SACs with high metal loading. Advanced characterization techniques with atomic resolution are indispensable for identification of the exact structure of SACs. This is true, especially for the applications and challenges in developing in situ/operando characterization techniques at the atomic level, which are discussed in this Review. Moreover, it is fundamentally necessary to investigate the active center structure, which facilitates any design of efficient SACs that can maximize single‐atom catalytic activity. Furthermore, this Review highlights challenges and prospects for development of SACs.

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Section: Synthesis Strategies Of High Metal Loading Sacsmentioning

confidence: 99%

Section: Synthesis Strategies Of High Metal Loading Sacsmentioning

confidence: 99%

Synthesis of High Metal Loading Single Atom Catalysts and Exploration of the Active Center Structure

Wang

Liu

2020

ChemCatChem

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“…[ 19,20 ] On the other hand, single‐atom catalysts (SACs) based on atomically dispersed metal atoms have demonstrated outstanding catalytic performances in several reactions, including Li–S redox reactions. [ 21–25 ] Besides maximizing the metal dispersion, the main advantage of SACs is their high surface energy, which allows decreasing the energy barrier of several catalytic processes.…”

Section: Introductionmentioning

confidence: 99%

Atomically dispersed Fe in a C₂N Based Catalyst as a Sulfur Host for Efficient Lithium–Sulfur Batteries

Liang

Yang

Tang

et al. 2020

Advanced Energy Materials

128

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Lithium–sulfur batteries (LSBs) are considered to be one of the most promising next generation energy storage systems due to their high energy density and low material cost. However, there are still some challenges for the commercialization of LSBs, such as the sluggish redox reaction kinetics and the shuttle effect of lithium polysulfides (LiPS). Here a 2D layered organic material, C2N, loaded with atomically dispersed iron as an effective sulfur host in LSBs is reported. X‐ray absorption fine spectroscopy and density functional theory calculations prove the structure of the atomically dispersed Fe/C2N catalyst. As a result, Fe/C2N‐based cathodes demonstrate significantly improved rate performance and long‐term cycling stability. Fe/C2N‐based cathodes display initial capacities up to 1540 mAh g−1 at 0.1 C and 678.7 mAh g−1 at 5 C, while retaining 496.5 mAh g−1 after 2600 cycles at 3 C with a decay rate as low as 0.013% per cycle. Even at a high sulfur loading of 3 mg cm−2, they deliver remarkable specific capacity retention of 587 mAh g−1 after 500 cycles at 1 C. This work provides a rational structural design strategy for the development of high‐performance cathodes based on atomically dispersed catalysts for LSBs.

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“…[9] Physical confinement restricts the dispersion of PSs at the anode by selective building blocks such as Nafion, [10] graphene oxide, [11] and MOF, [12] which can efficiently suppresses the shuttle of PS intermediates. [13] However,the activity of PSs cannot be instantly mediated, where kinetic challenges remain in aw orking battery.C hemical adsorptive/catalytic materials such as metal carbides, [14] nitrides, [15] chalcogenides, [16] single atom sites, [17] and their carbon composites [18] effectively work in mediating the PS activity on electrochemical active interfaces.H owever, such modification on the electrode-electrolyte interfaces is unable to completely address the dissolved PSs away from the cathode chamber. [19] To this end, homogeneous regulation in liquid phase,s uch as the use of redox mediator (RM), is reported to mediate the dissolved PSs by providing alternative chemical routes for the sulfur redox reactions.…”

Section: Introductionmentioning

confidence: 99%

Direct Intermediate Regulation Enabled by Sulfur Containers in Working Lithium–Sulfur Batteries

Xie

Song

et al. 2020

Angew Chem Int Ed

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Polysulfide intermediates (PSs), the liquid-phase species of active materials in lithium-sulfur (Li-S) batteries, connect the electrochemical reactions between insulative solid sulfur and lithium sulfide and are key to full exertion of the high-energy-density Li-S system. Herein, the concept of sulfur container additives is proposed for the direct modification on the PSs species.Byreversible storage and release of the sulfur species,t he container molecule converts small PSs into large organosulfur species.The prototype di(tri)sulfide-polyethylene glycol sulfur container is highly efficient in the reversible PS transformation to multiply affect electrochemical behaviors of sulfur cathodes in terms of liquid-species clustering,r eaction kinetics,and solid deposition. The stability and capacity of Li-S cells was therebyenhanced. The sulfur container is astrategy to directly modify PSs,enlightening the precise regulation on Li-S batteries and multi-phase electrochemical systems.

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Fast conversion and controlled deposition of lithium (poly)sulfides in lithium-sulfur batteries using high-loading cobalt single atoms

Cited by 310 publications

References 66 publications

Synthesis of High Metal Loading Single Atom Catalysts and Exploration of the Active Center Structure

Synthesis of High Metal Loading Single Atom Catalysts and Exploration of the Active Center Structure

Atomically dispersed Fe in a C₂N Based Catalyst as a Sulfur Host for Efficient Lithium–Sulfur Batteries

Direct Intermediate Regulation Enabled by Sulfur Containers in Working Lithium–Sulfur Batteries

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Fast conversion and controlled deposition of lithium (poly)sulfides in lithium-sulfur batteries using high-loading cobalt single atoms

Cited by 310 publications

References 66 publications

Synthesis of High Metal Loading Single Atom Catalysts and Exploration of the Active Center Structure

Synthesis of High Metal Loading Single Atom Catalysts and Exploration of the Active Center Structure

Atomically dispersed Fe in a C2N Based Catalyst as a Sulfur Host for Efficient Lithium–Sulfur Batteries

Direct Intermediate Regulation Enabled by Sulfur Containers in Working Lithium–Sulfur Batteries

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Atomically dispersed Fe in a C₂N Based Catalyst as a Sulfur Host for Efficient Lithium–Sulfur Batteries