Lithium–Sulfur Batteries: Dual‐Functional Atomic Zinc Decorated Hollow Carbon Nanoreactors for Kinetically Accelerated Polysulfides Conversion and Dendrite Free Lithium Sulfur Batteries (Adv. Energy Mater. 39/2020)

Ren, Xiaomin; Lü, Jianmin; Dong, Chengyan; Liu, Jian; Yang, Qihua; Chen, Jian

doi:10.1002/aenm.202070162

Cited by 36 publications

(48 citation statements)

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“…The measurements were performed using symmetrical cells with identical working and counter electrodes. [ 25,26 ] When Li 2 S 6 was added to the electrolyte, the CV curve of the cell constructed using SA‐Fe/Fe 2 N@NG exhibits four distinct redox peaks, and the corresponding current responses exhibit a highly linear relationship at scan rates of 5–20 mV s –1 (Figure S10, Supporting Information). The peak “a” in the cathodic scan originates from the reduction of Li 2 S 6 on the working electrode, while peak “b” in the anodic scan represents the reconstitution of Li 2 S 6 via the oxidation of Li 2 S 2 /Li 2 S (Figure 4c).…”

Section: Resultsmentioning

confidence: 99%

Engineering Fe–N Coordination Structures for Fast Redox Conversion in Lithium–Sulfur Batteries

et al. 2021

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Despite these advantages, the large-scale applications of Li-S batteries are hindered by some major challenges originating from the multielectron and multiphase S electrochemistry. [3] The electronic/ionic insulating nature of bulk S and Li sulfides (Li 2 S 2 /Li 2 S) results in sluggish reaction kinetics and low utilization of the active material. [4] Moreover, dissolved Li polysulfide intermediates (Li 2 S n , n = 4-8) undergo reduction at the Li anode and diffuse back to the cathode. This induces the detrimental "shuttle effect" that results in low Coulombic efficiency, continuous electrode degradation, and rapid capacity decay. [5] To address the aforementioned issues, significant efforts have been devoted to the development of various conducting/ polar host materials that can encapsulate sulfur. [6] However, these "inside" modification strategies for the cathode cannot prevent pronounced diffusion of Li 2 S n through the separator to the Li anode over time. This is attributed to the inevitable Li 2 S n dissolution and escape from the S carriers. It is necessary to develop an effective cathode "outside" design strategy to block the shuttle pathway. [7] Extensive research has been conducted, based on this concept, on the modification of separator with various derived carbonbased materials. The objective of the research is to localize the soluble Li 2 S n on the cathode side and enable the reutilization of the trapped active S. [8] 2D porous carbon nanosheets exhibit a high surface area and close-packing laminar structure. Critical drawbacks, including sluggish redox kinetics and undesirable shuttling of polysulfides (Li2 S n , n = 4-8), seriously deteriorate the electrochemical performance of high-energy-density lithium-sulfur (Li-S) batteries. Herein, these challenges are addressed by constructing an integrated catalyst with dual active sites, where single-atom (SA)-Fe and polar Fe 2 N are co-embedded in nitrogen-doped graphene (SA-Fe/Fe 2 N@NG). The SA-Fe, with plane-symmetric Fe-4N coordination, and Fe 2 N, with triangular pyramidal Fe-3N coordination, in this well-designed configuration exhibit synergistic adsorption of polysulfides and catalytic selectivity for Li 2 S n lithiation and Li 2 S delithiation, respectively. These characteristics endow the SA-Fe/Fe 2 N@NG-modified separator with an optimal polysulfides confinement-catalysis ability, thus accelerating the bidirectional liquid-solid conversion (Li 2 S n ↔Li 2 S) and suppressing the shuttle effect. Consequently, a Li-S battery based on the SA-Fe/Fe 2 N@NG separator achieves a high capacity retention of 84.1% over 500 cycles at 1 C (pure S cathode, S content: 70 wt%) and a high areal capacity of 5.02 mAh cm −2 at 0.1 C (SA-Fe/Fe 2 N@NG-supported S cathode, S loading = 5 mg cm −2 ). It is expected that the outcomes of the present study will facilitate the design of high-efficiency catalysts for long-lasting Li-S batteries.

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Section: Resultsmentioning

confidence: 99%

Engineering Fe–N Coordination Structures for Fast Redox Conversion in Lithium–Sulfur Batteries

et al. 2021

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“…The sulfur composite was prepared via the classical melt‐diffusion method. [ 48 ] The sample powder (Nb 2 O 5 , Nb 4 N 5 , and Nb 4 N 5 –Nb 2 O 5 ) was thoroughly grinded with sulfur (1:4 by mass, 99%, Alfa Aesar). Then, the obtained powder was annealed at 155 °C for 12 h under Ar atmosphere.…”

Section: Methodsmentioning

confidence: 99%

Interfacial Engineering of Bifunctional Niobium (V)‐Based Heterostructure Nanosheet Toward High Efficiency Lean‐Electrolyte Lithium–Sulfur Full Batteries

Shi

Qin

et al. 2021

Adv Funct Materials

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High‐efficiency lithium–sulfur (Li–S) batteries depend on an advanced electrode structure that can attain high sulfur utilization at lean‐electrolyte conditions and minimum amount of lithium. Herein, a twinborn holey Nb4N5–Nb2O5 heterostructure is designed as a dual‐functional host for both redox–kinetics–accelerated sulfur cathode and dendrite‐inhibited lithium anode simultaneously for long‐cycling and lean‐electrolyte Li–S full batteries. Benefiting from the accelerative polysulfides anchoring–diffusion–converting efficiency of Nb4N5–Nb2O5, polysulfide‐shutting is significantly alleviated. Meanwhile, the lithiophilic nature of holey Nb4N5–Nb2O5 is applied as an ion‐redistributor for homogeneous Li‐ion deposition. Taking advantage of these merits, the Li–S full batteries present excellent electrochemical properties, including a minimum capacity decay rate of 0.025% per cycle, and a high areal capacity of 5.0 mAh cm−2 at sulfur loading of 6.9 mg cm−2, corresponding to negative to positive capacity ratio of 2.4:1 and electrolyte to sulfur ratio of 5.1 µL mg−1. Therefore, this work paves a new avenue for boosting high‐performances Li–S batteries toward practical applications.

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“…The efficient catalysis of SAV enabled the LSBs to provide a superior long‐term cyclic performance (a capacity decay of 0.073% after 400 cycle at 0.5 C. Wu and co‐workers prepared single atomic Zn modified hollow carbon sphere (Zn 1 –HNC) as both S (Zn 1 –HNC–S) and Li (Zn 1 –HNC–Li) dual‐functional hosts for achieving highly stable, fast kinetic and long‐life Li–S full battery (Zn 1 –HNC–S|| Zn 1 –HNC–Li). [ 135 ] Thanks to its excellent conductivity, high surface area (370 m 2 g −1 ), efficient active sites and protective carbon shell, the as‐prepared Zn 1 –HNC nanoreactors contributed to strong physical confinement, chemical anchoring and excellent electrocatalysis toward polysulfides. At the same time, the uniform and dendrite‐free lithium deposition was achieved in the nanoreactor with excellent lithiophilic property.…”

Section: Emerging Metal‐based Catalytic Materials For Li–s Batteriesmentioning

confidence: 99%

Emerging Catalysts to Promote Kinetics of Lithium–Sulfur Batteries

Wang

Huang

et al. 2021

Advanced Energy Materials

247

209

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Lithium–sulfur batteries (LSBs) with a high theoretical capacity of 1675 mAh g−1 hold promise in the realm of high‐energy‐density Li–metal batteries. To cope with the shuttle effect and sluggish transformation of soluble lithium polysulfides (LiPSs), varieties of traditional metal‐based materials (such as metal, metal oxides, metal sulfides, metal nitrides, and metal carbides) with unique catalytic activity for accelerating LiPSs redox have been exploited to fundamentally inhibit the shuttle effect and improve the performance of LSBs. Concurrently, some budding catalytic materials also possess enormous potential for facilitating LiPSs redox reaction in LSBs, including metal borides, metal phosphides, metal selenides, single atoms, and defect‐engineered materials. Here, recent advances in these emerging catalytic candidates as well as the evaluation methods and parameters for catalytic materials are comprehensively summarized for the first time. New insights are also given to aid in the design of high‐performance LSBs and satisfy the high expectation in the future, including the exposure of the active sites and adsorption‐catalysis synergy strategies. Finally, the current challenges and prospects for designing highly efficient catalytic materials are highlighted, aiming at providing guidance for configuring catalytic materials to make sure high‐energy and long‐life LSBs.

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Lithium–Sulfur Batteries: Dual‐Functional Atomic Zinc Decorated Hollow Carbon Nanoreactors for Kinetically Accelerated Polysulfides Conversion and Dendrite Free Lithium Sulfur Batteries (Adv. Energy Mater. 39/2020)

Cited by 36 publications

References 0 publications

Engineering Fe–N Coordination Structures for Fast Redox Conversion in Lithium–Sulfur Batteries

Engineering Fe–N Coordination Structures for Fast Redox Conversion in Lithium–Sulfur Batteries

Interfacial Engineering of Bifunctional Niobium (V)‐Based Heterostructure Nanosheet Toward High Efficiency Lean‐Electrolyte Lithium–Sulfur Full Batteries

Emerging Catalysts to Promote Kinetics of Lithium–Sulfur Batteries

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