Position difference between Mo clusters and N sites induced highly synergistic electrocatalysis in integrated electrode-separator membranes with crosslinked hierarchically porous interface

Jiang, Haipeng; Gu, Shenghan; Guo, Jiao; Dai, Yan; Zheng, Wenji; Jing, Xiaobin; Wu, Xuemei; Xiao, Wu; He, Gaohong; Li, Xiangcun

doi:10.1016/j.ensm.2021.12.006

Cited by 24 publications

(8 citation statements)

References 38 publications

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“…48−50 The S 2p spectra after cycling in Figure 2b can be divided into eight peaks at 162.65/163.03 (terminal S, S T , and S T −Fe), 164.03/165.06 (bridging S, S B , and S B −Fe), 167.52/168.7 (thiosulfate), and 169.69/170.6 eV (polythionate complexes). 51 As the Fe atoms bond with S B and S T , the electron density appears to positively chemically shift, confirming the strong adsorption ability of Fe 2 O 3 toward LiPSs. The F 1s spectrum in Figure 2c reveals the chemical instances of the F atom after cycling.…”

Section: Resultsmentioning

confidence: 75%

“…Fe 2p in Figure a demonstrates four peaks at 710.0, 716.1, 719.2, and 734.5 eV, the binding energies of which correspond to Fe 2p 3/2 and Fe 2p 1/2 and their satellite peaks. Additionally, there are two more peaks at 708.0 and 714.0 eV near the Fe 2p 3/2 and Fe 2p 1/2 peaks which were indexed to the Fe–S bond after cycling. − The S 2p spectra after cycling in Figure b can be divided into eight peaks at 162.65/163.03 (terminal S, S T , and S T –Fe), 164.03/165.06 (bridging S, S B , and S B –Fe), 167.52/168.7 (thiosulfate), and 169.69/170.6 eV (polythionate complexes) . As the Fe atoms bond with S B and S T , the electron density appears to positively chemically shift, confirming the strong adsorption ability of Fe 2 O 3 toward LiPSs.…”

Section: Resultsmentioning

confidence: 99%

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Flexible and Conductive Membrane with Ultrahigh Porosity and Polysulfide-Conversion Catalytic Activity for Large-Scale Preparation of Li–S Batteries

Jiang

et al. 2022

ACS Appl. Energy Mater.

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Li−S batteries still have various problems, including volume expansion, low S conductivity, and shuttling effect of polysulfides (LiPSs), requiring resolution. Herein, polyvinylidene fluoride (PVDF) is combined with carbon nanotubes (CNTs) and Fe 2 O 3 through a one-step phase-inversion process to form a highly flexible and conductive membrane as a functional Li−S battery interlayer. The CNT skeleton is tightly entangled and crosslinked by PVDF to form a hierarchically porous framework, which is suitable for fast Li + and electron transport and volumetric expansion of S and facilitated electrolyte diffusion. Additionally, the strongly negative F atoms can accelerate Li + transport, promoting the fast redox reaction between S species and Li + . Furthermore, the uniformly doped Fe 2 O 3 nanoparticles provide abundant active sites and broad reaction interfaces for highly efficient LiPS anchoring and catalytic conversion. Li−S batteries with the membrane as the interlayer exhibit an excellent cycle performance and reversible capacity of 631.2 mAh g −1 after 400 cycles at 1 C. Furthermore, in situ Raman spectroscopy shows that long-chain Li 2 S 8 decreases, indicating that the interlayer can alleviate the shuttle of soluble LiPSs. This proposed strategy advances the practical application of Li−S batteries due to the facile and scalable production of the flexible membrane.

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Section: Resultsmentioning

confidence: 75%

Section: Resultsmentioning

confidence: 99%

Flexible and Conductive Membrane with Ultrahigh Porosity and Polysulfide-Conversion Catalytic Activity for Large-Scale Preparation of Li–S Batteries

Jiang

et al. 2022

ACS Appl. Energy Mater.

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“…X-ray photoelectron spectroscopy (XPS) was employed to further examine the chemical interaction between the Mo/MoO 2 and LiPSs, and the results are shown in Figure b,c. According to the Mo 3d spectra, the Mo/MoO 2 consists of the characteristic peaks of the Mo–Mo bond for metallic Mo (Mo 0 ) at 228.2 eV and the Mo–O bond for MoO 2 (Mo 4+ ) at 229.5 eV, respectively, confirming the coexistence of Mo and MoO 2 . , The signals at 231.1 and 232.2 eV should be ascribed to the Mo 5+ and Mo 6+ , respectively. The high valence states were originated from the unavoidable oxidation of Mo and MoO 2 when exposed to the air.…”

Section: Resultsmentioning

confidence: 84%

Built-In Electric Field on the Mott–Schottky Heterointerface-Enabled Fast Kinetics Lithium–Sulfur Batteries

Cai

Gao

Wang

et al. 2022

ACS Appl. Mater. Interfaces

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Lithium−sulfur (Li−S) batteries (LSBs) have been considered one of the most potential candidates to substitute traditional Li-ion batteries (LIBs), owing to their high theoretical energy density and low cost. Nevertheless, the shuttle effect and the sluggish redox kinetics of lithium polysulfides (LiPSs) have long been obstacles to realizing stable LSBs with high reversible capacity. In this study, we proposed a metal−semiconductor (Mo and MoO 2 ) heterostructure with the hollow microsphere morphology as an effective Mott−Schottky electrocatalyst to boost sulfur electrochemistry. The hollow structure can physically inhibit the shuttling of LiPSs and accommodate the volume fluctuation during cycling. More importantly, the built-in electric field at the heterointerfacial sites can effectively accelerate the reduction of LiPSs and oxidation of Li 2 S, thereby reaching a high sulfur utilization. With the assistance of the Mo/MoO 2 catalyst, the cell exhibited prominent rate capability and stable long-term cycling performance, showing a high capacity of 630 mA h•g −1 at 4 C and a low decay of 0.073% at 1 C after 500 cycles. Even with high areal sulfur loading of 10.0 mg•cm −2 , high capacity and good cycle stability were achieved at 0.2 C under lean electrolyte conditions (E/S ratio of 6 μL•mg −1 ).

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“…Besides, Li et al induced the Mo clusters in the N‐doped carbon shells, and used them as the electrode‐separator membranes for Li–S batteries. [ 99 ] The DFT calculation revealed the job‐synergistic catalytic mechanism of the Mo clusters and N atoms to promote the deposition and decomposition of Li 2 S during the electrochemical process. As shown in Figure 12d, the Li 2 S dissociation barrier energies are 1.58, 1.05, and 0.19 eV for NC, Mo 13 @NC‐a (Mo clusters dispersed on the NC), and Mo 13 @NC‐b (some clusters occupy the N sites and the defection), respectively, revealing that the Li 2 S dissociation on Mo 13 @NC‐b surface is more thermodynamically favorable.…”

Section: Molybdenum‐based Catalyst Materials For Advanced Li–s Batteriesmentioning

confidence: 99%

Molybdenum‐Based Catalytic Materials for Li–S Batteries: Strategies, Mechanisms, and Prospects

Liu

Lin

Bettels

et al. 2022

Adv Energy and Sustain Res

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Position difference between Mo clusters and N sites induced highly synergistic electrocatalysis in integrated electrode-separator membranes with crosslinked hierarchically porous interface

Cited by 24 publications

References 38 publications

Flexible and Conductive Membrane with Ultrahigh Porosity and Polysulfide-Conversion Catalytic Activity for Large-Scale Preparation of Li–S Batteries

Flexible and Conductive Membrane with Ultrahigh Porosity and Polysulfide-Conversion Catalytic Activity for Large-Scale Preparation of Li–S Batteries

Built-In Electric Field on the Mott–Schottky Heterointerface-Enabled Fast Kinetics Lithium–Sulfur Batteries

Molybdenum‐Based Catalytic Materials for Li–S Batteries: Strategies, Mechanisms, and Prospects

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