首页|Tuning the crystalline and electronic structure of ZrO2 via oxygen vacancies and nano-structuring for polysulfides conversion in lithium-sulfur batteries

Tuning the crystalline and electronic structure of ZrO2 via oxygen vacancies and nano-structuring for polysulfides conversion in lithium-sulfur batteries

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The recent emergence of tetragonal phases zirconium dioxide(ZrO2)with vacancies has generated signif-icant interest as a highly efficient and stable electrocatalyst with potential applications in trapping poly-sulfides and facilitating rapid conversion in lithium-sulfur batteries(LSBs).However,the reduction of ZrO2 is challenging,even under strong reducing atmospheres at high temperatures and pressures.Consequently,the limited presence of oxygen vacancies results in insufficient active sites and reaction interfaces,thereby hindering practical implementation.Herein,we successfully introduced abundant oxygen vacancies into ZrO2 at the nanoscale with the help of carbon nanotubes(CNTs-OH)through hydrogen-etching at lower temperatures and pressures.The introduced oxygen vacancies on ZrO2-x/CNTs-OH can effectively rearrange charge distribution,enhance sulfiphilicity and increase active sites,contributing to high ionic and electronic transfer kinetics,strong binding energy and low redox barriers between polysulfides and ZrO2-x.These findings have been experimentally validated and supported by theory calculations.As a result,LSBs assembled with the ZrO2-x/CNTs-OH modified separators demon-strate excellent rate performance,superior cycling stability,and ultra-high sulfur utilization.Especially,at high sulfur loading of 6 mg cm-2,the area capacity is still up to 6.3 mA h cm-2.This work provides valuable insights into the structural and functional optimization of electrocatalysts for batteries.

Lithium-sulfur batteriesOxygen vacanciesZirconium dioxide/carbon nanotubes with-OHImproved redox kineticsSuperior cycling stability

Shengnan Fu、Chaowei Hu、Jing Li、Hongtao Cui、Yuanyuan Liu、Kaihua Liu、Yanzhao Yang、Meiri Wang

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Shandong Key Laboratory for Chemical Engineering and Processing,School of Chemistry & Chemical Engineering,Yantai University,Yantai 264000,Shandong,China

Key Laboratory for Special Functional Aggregate Materials of Education Ministry,School of Chemistry and Chemical Engineering Shandong University,Jinan 250100,Shandong,China

Natural Science Foundation of Shandong ProvinceNatural Science Foundation of Shandong ProvinceNatural Science Foundation of Shandong ProvinceNatural Science Foundation of Shandong Province

ZR2021MB101ZR2021ME113ZR2021ME177ZR2021QE096

2024

10.1016/j.jechem.2023.09.003

能源化学
中国科学院大连化学物理研究所 中国科学院成都有机化学研究所

能源化学

CSTPCDEI
影响因子：0.654
ISSN：2095-4956
年,卷(期)：2024.88(1)
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