Desolvation Synergy of Multiple H/Li‐Bonds on an Iron‐Dextran‐Based Catalyst Stimulates Lithium–Sulfur Cascade Catalysis

Li, Tingting; Cai, Dong; Yang, Shuo; Dong, Yangyang; Yu, Shuang; Zhou, Xuemei; Ge, Yifei; Xiao, Kaijun; Nie, Huagui; Yang, Zhi

doi:10.1002/adma.202207074

Cited by 24 publications

(17 citation statements)

References 65 publications

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“…The specific capacities of Li–S batteries using the MB-VN coating layer under 4.6 and 6.0 mg cm –2 sulfur are 970 and 936 mAh g –1 at 0.1 C, respectively, and they decrease to 727 and 615 mAh g –1 at 0.5 C, respectively. Notably, the above results are among the best as compared to those of recently published works (Figure i), − implying the great potential of using MB-VN-modified separators for practical applications.…”

Section: Resultssupporting

confidence: 61%

Wide-Temperature Operation of Lithium–Sulfur Batteries Enabled by Multi-Branched Vanadium Nitride Electrocatalyst

Wang

et al. 2023

ACS Nano

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High-performance lithium−sulfur (Li−S) batteries that can work normally under harsh conditions have attracted tremendous attention; however, the sluggish reaction kinetics of polysulfide conversions at low temperatures as well as the notorious polysulfide shuttling at high temperatures remain to be resolved. Herein, a multibranched vanadium nitride (MB-VN) electrocatalyst has been designed and deployed for Li−S batteries. Both experimental (time-of-flight secondary ion mass spectroscopy and adsorption tests) and theoretical results verify the strong chemical adsorption capability and high electrocatalytic activity of MB-VN with respect to polysulfides. Moreover, in situ Raman characterization manifests the effective inhibition of polysulfide shuttling by the MB-VN electrocatalyst. Using MB-VN-modified separators, the Li−S batteries deliver an excellent rate capability (707 mAh g −1 at 3.0 C) and great cyclic stability (678 mAh g −1 after 400 cycles at 1.0 C) at room temperature. With 6.0 mg cm −2 of sulfur and a lean electrolyte volume of ∼6 μL mg s −1 , Li−S batteries exhibit a high areal capacity of 5.47 mAh cm −2 . Even over a wide temperature range (−20 to +60 °C), the Li−S batteries still maintain stable cyclic performance at high current rates. This work demonstrates that metal nitride based electrocatalysts can realize low-/high-temperature-tolerant Li−S batteries.

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Section: Resultssupporting

confidence: 61%

Wide-Temperature Operation of Lithium–Sulfur Batteries Enabled by Multi-Branched Vanadium Nitride Electrocatalyst

Wang

et al. 2023

ACS Nano

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“…Moreover, the opposite peak shift trend was observed in the sulfur oxidation process and both Ni–P and Ni 2+ recovered to their initial chemical states, demonstrating a good electrochemical reversibility of Ni 2 P–Co@CNTs . As shown in Figure S29, the S 2p results show characteristic S T (∼162.7 eV, 2p 3/2 ) and S B (∼164.2 eV, 2p 3/2 ) peaks, which can be roughly assigned to long-chain polysulfides and Li 2 S 2 /Li 2 S, respectively . With the depth of sulfur reduction, the S B signal of Ni 2 P–Co@CNTs eventually disappears at 1.7 V (According to the peak area, an atomic content ratio of S T to S B is 69).…”

Section: Resultsmentioning

confidence: 93%

“…50 As shown in Figure S29, the S 2p results show characteristic S T (∼162.7 eV, 2p 3/2 ) and S B (∼164.2 eV, 2p 3/2 ) peaks, which can be roughly assigned to long-chain polysulfides and Li 2 S 2 /Li 2 S, respectively. 51 With the depth of sulfur reduction, the S B signal of Ni 2 P−Co@CNTs eventually disappears at 1.7 V (According to the peak area, an atomic content ratio of S T to S B is 69). This means an almost complete depletion of polysulfides, and it is finally catalyzed to Li 2 S 2 /Li 2 S.•In the sulfur oxidation process, both S T and S B signals are recovered to their initial chemical states, showing a good electrochemically catalytic reversibility of Ni 2 P−Co@CNTs.…”

Section: Resultsmentioning

confidence: 99%

Synthesis of the Ni₂P–Co Mott–Schottky Junction as an Electrocatalyst to Boost Sulfur Conversion Kinetics and Application in Separator Modification in Li-S Batteries

Zhang

Qiao

et al. 2023

ACS Appl. Mater. Interfaces

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To overcome the shuttling effect and sluggish conversion kinetics of polysulfides, a large number of catalysts have been designed for lithium−sulfur (Li−S) batteries. Herein, a Mott−Schottky junction catalyst composed of Co nanoparticles and Ni 2 P was designed to improve polysulfide kinetics. Our investigations reveal the rearrangement of charges at the Schottky junction interface and the construction of the built-in electric field are crucial for lowering the activation energy of the dissolved Li 2 S n reduction and Li 2 S nucleation reaction. Furthermore, a series of experimental and electrochemical tests were performed to demonstrate that the Schottky catalytic effect enhanced the synergistic catalytic effect. With a Ni 2 P−Co@CNT catalyst, the battery exhibits an initial specific capacity of 874 mAh g −1 at a rate of 4.0 C, and the decay rate per cycle is 0.049% in 700 cycles. Meanwhile, the battery shows 0.118% decay rate per cycle at 0.5 C in 100 cycles at a high sulfur loading of 10 mg cm −2 . The Schottky heterojunction structure proposed here has been shown to have a good catalytic effect on the reduction of Li 2 S n and nucleation of Li 2 S, which provides a profound guidance for efficient and rational catalyst design.

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“…In the high‐resolution S 2p spectrum ( Figure a), the peaks at 164.1 and 162.9 eV can be attributed to terminal sulfur (S T −1 ) and bridging sulfur (S B 0 ), while the peaks between 165–171 eV are due to the presence of thiosulfate and sulfate species. [ 32,33 ] The existence of S 2p species demonstrates the successful adsorption of LiPSs on the Fe@C‐CNT. The high‐resolution Li 1s spectrum is shown in Figure 4b.…”

Section: Resultsmentioning

confidence: 99%

Enhancing Electron Conductivity and Electron Density of Single Atom Based Core–Shell Nanoboxes for High Redox Activity in Lithium Sulfur Batteries

Guo

Jiang

Wang

et al. 2023

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Herein, an integrated structure of single Fe atom doped core‐shell carbon nanoboxes wrapped by self‐growing carbon nanotubes (CNTs) is designed. Within the nanoboxes, the single Fe atom doped hollow cores are bonded to the shells via the carbon needles, which act as the highways for the electron transport between cores and shells. Moreover, the single Fe atom doped nanobox shells is further wrapped and connected by self‐growing carbon nanotubes. Simultaneously, the needles and carbon nanotubes act as the highways for electron transport, which can improve the overall electron conductivity and electron density within the nanoboxes. Finite element analysis verifies the unique structure including both internal and external connections realize the integration of active sites in nano scale, and results in significant increase in electron transfer and the catalytic performance of Fe‐N4 sites in both Li2Sn lithiation and Li2S delithiation. The Li–S batteries with the double‐shelled single atom catalyst delivered the specific capacity of 702.2 mAh g−1 after 550 cycles at 1.0 C. The regional structure design and evaluation method provide a new strategy for the further development of single atom catalysts for more electrochemical processes.

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Desolvation Synergy of Multiple H/Li‐Bonds on an Iron‐Dextran‐Based Catalyst Stimulates Lithium–Sulfur Cascade Catalysis

Abstract: Scheme 1. Schematic illustration of the inspiration for this VC@INFeD molecular catalyst design from pharmaceutical chemistry to LiS chemistry.

Cited by 24 publications

References 65 publications

Wide-Temperature Operation of Lithium–Sulfur Batteries Enabled by Multi-Branched Vanadium Nitride Electrocatalyst

Wide-Temperature Operation of Lithium–Sulfur Batteries Enabled by Multi-Branched Vanadium Nitride Electrocatalyst

Synthesis of the Ni₂P–Co Mott–Schottky Junction as an Electrocatalyst to Boost Sulfur Conversion Kinetics and Application in Separator Modification in Li-S Batteries

Enhancing Electron Conductivity and Electron Density of Single Atom Based Core–Shell Nanoboxes for High Redox Activity in Lithium Sulfur Batteries

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Desolvation Synergy of Multiple H/Li‐Bonds on an Iron‐Dextran‐Based Catalyst Stimulates Lithium–Sulfur Cascade Catalysis

Abstract: Scheme 1. Schematic illustration of the inspiration for this VC@INFeD molecular catalyst design from pharmaceutical chemistry to LiS chemistry.

Cited by 24 publications

References 65 publications

Wide-Temperature Operation of Lithium–Sulfur Batteries Enabled by Multi-Branched Vanadium Nitride Electrocatalyst

Wide-Temperature Operation of Lithium–Sulfur Batteries Enabled by Multi-Branched Vanadium Nitride Electrocatalyst

Synthesis of the Ni2P–Co Mott–Schottky Junction as an Electrocatalyst to Boost Sulfur Conversion Kinetics and Application in Separator Modification in Li-S Batteries

Enhancing Electron Conductivity and Electron Density of Single Atom Based Core–Shell Nanoboxes for High Redox Activity in Lithium Sulfur Batteries

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Synthesis of the Ni₂P–Co Mott–Schottky Junction as an Electrocatalyst to Boost Sulfur Conversion Kinetics and Application in Separator Modification in Li-S Batteries