Engineering Triple-Phase Interfaces Enabled by Layered Double Perovskite Oxide for Boosting Polysulfide Redox Conversion

Zhe Bai; Zhenhua Wang; Ruilong Li; Zeyu Wu; Pingli Feng; Lina Zhao; Tan Wang; Wenshuo Hou; Yu Bai; Guoxiu Wang; Kening Sun

doi:10.1021/acs.nanolett.3c00566

Engineering Triple-Phase Interfaces Enabled by Layered Double Perovskite Oxide for Boosting Polysulfide Redox Conversion

Zhe Bai, Zhenhua Wang^*, Ruilong Li, Zeyu Wu, Pingli Feng, Lina Zhao, Tan Wang, Wenshuo Hou, Yu Bai, Guoxiu Wang^*, Kening Sun^*

^*Corresponding author for this work

School of Chemistry and Chemical Engineering

Research output: Contribution to journal › Article › peer-review

11 Citations (Scopus)

Abstract

The electrocatalytic conversion of polysulfides is crucial to lithium-sulfur batteries and mainly occurs at triple-phase interfaces (TPIs). However, the poor electrical conductivity of conventional transition metal oxides results in limited TPIs and inferior electrocatalytic performance. Herein, a TPI engineering approach comprising superior electrically conductive layered double perovskite PrBaCo2O5+δ (PBCO) is proposed as an electrocatalyst to boost the conversion of polysulfides. PBCO has superior electrical conductivity and enriched oxygen vacancies, effectively expanding the TPI to its entire surface. DFT calculation and in situ Raman spectroscopy manifest the electrocatalytic effect of PBCO, proving the critical role of enhanced electrical conductivity of this electrocatalyst. PBCO-based Li-S batteries exhibit an impressive reversible capacity of 612 mAh g-1 after 500 cycles at 1.0 C with a capacity fading rate of 0.067% per cycle. This work reveals the mechanism of the enriched TPI approach and provides novel insight into designing new catalysts for high-performance Li-S batteries.

Original language	English
Pages (from-to)	4908-4915
Number of pages	8
Journal	Nano Letters
Volume	23
Issue number	11
DOIs	https://doi.org/10.1021/acs.nanolett.3c00566
Publication status	Published - 14 Jun 2023

Keywords

layered double perovskite oxide
lithium-sulfur batteries
oxygen vacancies
redox kinetics
triple-phase interface

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10.1021/acs.nanolett.3c00566

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title = "Engineering Triple-Phase Interfaces Enabled by Layered Double Perovskite Oxide for Boosting Polysulfide Redox Conversion",

abstract = "The electrocatalytic conversion of polysulfides is crucial to lithium-sulfur batteries and mainly occurs at triple-phase interfaces (TPIs). However, the poor electrical conductivity of conventional transition metal oxides results in limited TPIs and inferior electrocatalytic performance. Herein, a TPI engineering approach comprising superior electrically conductive layered double perovskite PrBaCo2O5+δ (PBCO) is proposed as an electrocatalyst to boost the conversion of polysulfides. PBCO has superior electrical conductivity and enriched oxygen vacancies, effectively expanding the TPI to its entire surface. DFT calculation and in situ Raman spectroscopy manifest the electrocatalytic effect of PBCO, proving the critical role of enhanced electrical conductivity of this electrocatalyst. PBCO-based Li-S batteries exhibit an impressive reversible capacity of 612 mAh g-1 after 500 cycles at 1.0 C with a capacity fading rate of 0.067% per cycle. This work reveals the mechanism of the enriched TPI approach and provides novel insight into designing new catalysts for high-performance Li-S batteries.",

keywords = "layered double perovskite oxide, lithium-sulfur batteries, oxygen vacancies, redox kinetics, triple-phase interface",

author = "Zhe Bai and Zhenhua Wang and Ruilong Li and Zeyu Wu and Pingli Feng and Lina Zhao and Tan Wang and Wenshuo Hou and Yu Bai and Guoxiu Wang and Kening Sun",

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AU - Bai, Zhe

AU - Wang, Zhenhua

AU - Li, Ruilong

AU - Wu, Zeyu

AU - Feng, Pingli

AU - Zhao, Lina

AU - Wang, Tan

AU - Hou, Wenshuo

AU - Bai, Yu

AU - Wang, Guoxiu

AU - Sun, Kening

PY - 2023/6/14

Y1 - 2023/6/14

N2 - The electrocatalytic conversion of polysulfides is crucial to lithium-sulfur batteries and mainly occurs at triple-phase interfaces (TPIs). However, the poor electrical conductivity of conventional transition metal oxides results in limited TPIs and inferior electrocatalytic performance. Herein, a TPI engineering approach comprising superior electrically conductive layered double perovskite PrBaCo2O5+δ (PBCO) is proposed as an electrocatalyst to boost the conversion of polysulfides. PBCO has superior electrical conductivity and enriched oxygen vacancies, effectively expanding the TPI to its entire surface. DFT calculation and in situ Raman spectroscopy manifest the electrocatalytic effect of PBCO, proving the critical role of enhanced electrical conductivity of this electrocatalyst. PBCO-based Li-S batteries exhibit an impressive reversible capacity of 612 mAh g-1 after 500 cycles at 1.0 C with a capacity fading rate of 0.067% per cycle. This work reveals the mechanism of the enriched TPI approach and provides novel insight into designing new catalysts for high-performance Li-S batteries.

AB - The electrocatalytic conversion of polysulfides is crucial to lithium-sulfur batteries and mainly occurs at triple-phase interfaces (TPIs). However, the poor electrical conductivity of conventional transition metal oxides results in limited TPIs and inferior electrocatalytic performance. Herein, a TPI engineering approach comprising superior electrically conductive layered double perovskite PrBaCo2O5+δ (PBCO) is proposed as an electrocatalyst to boost the conversion of polysulfides. PBCO has superior electrical conductivity and enriched oxygen vacancies, effectively expanding the TPI to its entire surface. DFT calculation and in situ Raman spectroscopy manifest the electrocatalytic effect of PBCO, proving the critical role of enhanced electrical conductivity of this electrocatalyst. PBCO-based Li-S batteries exhibit an impressive reversible capacity of 612 mAh g-1 after 500 cycles at 1.0 C with a capacity fading rate of 0.067% per cycle. This work reveals the mechanism of the enriched TPI approach and provides novel insight into designing new catalysts for high-performance Li-S batteries.

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KW - lithium-sulfur batteries

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KW - redox kinetics

KW - triple-phase interface

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Engineering Triple-Phase Interfaces Enabled by Layered Double Perovskite Oxide for Boosting Polysulfide Redox Conversion

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