Phosphorus modulated porous CeO2 nanocrystallines for accelerated polysulfide catalysis in advanced Li-S batteries

doi:10.1016/j.jmst.2022.06.004

Abstract

Abstract:

The insulating nature of sulfur species, sluggish reaction kinetics, and uncontrolled dissolution of lithium polysulfide (LiPS) intermediates during the complex and multiphase sulfur redox process, have severely inhibited the applications of Li-S batteries. In this study, we report a rational strategy to accelerate the polysulfide catalysis via constructing phosphorus modulated porous CeO₂ (P-CeO₂) for advanced Li-S batteries. The morphology and surface analysis demonstrate that the P-CeO₂ consists of abundant P-modulated porous CeO₂ nanocrystallines. The battery performance reveals that the introduction of P will lead to an improved initial capacity of 1027 mA h g⁻¹ than that of bare CeO₂ (895.7 mA h g⁻¹) at 0.2 C. In addition, the P-CeO₂ cathode can maintain a low capacity decay ratio of 0.10% per cycle after 500 cycles at 1.0 C. The coin battery tests suggest that the P-CeO₂ cathode presents faster oxidation-reduction kinetics of LiPS and quick diffusion of Li⁺ ions. Meanwhile, the studies of redox processes and chemical interactions of LiPS have demonstrated the P-CeO₂ cathode displays stronger adsorption of Li₂S₆, higher redox peak current, and earlier precipitation of Li₂S than the bare CeO₂. This study demonstrates for the first time that the P-modulation of metal oxide surface can simultaneously promote the catalytic reaction kinetics and chemical interaction of LiPS. We anticipate that this P-modulation method can be extended to many other nanostructured metal catalytic sites for developing affordable advanced Li-S batteries.

Key words: Metal oxides, P-modulated porous CeO₂, Polysulfide catalytic materials, Shuttle effects, Lithium-sulfur batteries

Xuefeng Tao, Zhao Yang, Menghao Cheng, Rui Yan, Fan Chen, Sujiao Cao, Shuang Li, Tian Ma, Chong Cheng, Wei Yang. Phosphorus modulated porous CeO₂ nanocrystallines for accelerated polysulfide catalysis in advanced Li-S batteries[J]. J. Mater. Sci. Technol., 2022, 131: 212-220.

Figures/Tables 6

Fig. 1. (a) Schematic illustration of the synthetic route to P-CeO2. (b) SEM image of Ce-MOFs. (c, d) TEM images of P-CeO2. (e, f) HR-TEM images of P-CeO2. (g) SAED pattern of P-CeO2. (h) HAADF-STEM image and EDX elemental mapping images of P-CeO2.

Fig. 2. (a) The XRD patterns of CeO2 and P-CeO2. (b) The N2 adsorption-desorption isotherm of CeO2 and P-CeO2. (c) The TGA curves of the sulfur loading of CeO2 and P-CeO2. (d) The atomic element contents of CeO2 and P-CeO2. (e) High-resolution XPS spectra of P 2p of P-CeO2. (f) High-resolution XPS spectra of Ce 3d of CeO2 and P-CeO2. (g) High-resolution XPS spectra of O 1 s of P-CeO2. (h) The Raman spectra of CeO2 and P-CeO2.

Fig. 3. (a) Galvanostatic charge?discharge curves of two cathodes at 0.1 C (ΔE, Q1, Q2). (b) ΔE and Q2/Q1 values calculated from the corresponding charge?discharge curves in (a). (c) The fitting EIS spectra of two cathodes before the cycle and the equivalent circuit diagram. (d) Galvanostatic charge?discharge profiles of P-CeO2 cathode at different current densities. (e) Polarization voltage of two cathodes between the discharge and charge plateaus at different current densities. (f) The energy efficiency and (g) rate capabilities of two cathodes at different current densities.

Fig. 4. (a) The discharge?charge profiles of P-CeO2. (b) Ex-situ EIS of P-CeO2 electrode at the different status of discharge and charge. Cycling performances and corresponding coulombic efficiency of two cathodes at a high current rate of 0.2 C (c), 0.5 C (d), and 1.0 C (e). (f) Comparison of the decay rate per cycle with other Li-S anode materials at 1.0-2.0 C in the literature.

Fig. 5. (a) The CV curves of the asymmetric cells at 0.1 mV s?1. (b) Tafel plots of the oxidation process of polysulfide for CeO2 and P-CeO2 cathodes. Tafel plots of the two reduction process of polysulfide for CeO2 and P-CeO2 cathodes (c, d). (e) CV curves of P-CeO2 cathode at different scan rates. Plots of the oxidization (f) and reduction (g, h) peak currents versus square root of scan rates. (i) Schematic of the redox conversion kinetics of LiPS in the P-CeO2 cathode.

Fig. 6. (a) The UV-vis adsorption spectra of P-CeO2 and CeO2 with Li2S6 solution. (b) High-resolution XPS spectra of S 2p of Li2S6. (c) High-resolution XPS spectra of P 2p of P-CeO2 and P-CeO2 with Li2S6. (d) Schematic illustration of symmetric batteries. (e) The CV curves of symmetric batteries CeO2 and P-CeO2 with Li2S6 and blank group (without Li2S6). (f) EIS plots of symmetric batteries of CeO2 and P-CeO2 with Li2S6. Potentiostatic discharge curves of Li2S8 tetraglyme solution on CeO2 (g) and P-CeO2 (h). (i) Charge voltage profiles of CeO2 and P-CeO2 cathodes in the first cycle.

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Phosphorus modulated porous CeO₂ nanocrystallines for accelerated polysulfide catalysis in advanced Li-S batteries

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