Enhancing Bidirectional Sulfur Conversion Through p–dOrbital Hybridization via Vacancy Engineering

Kód výsledku v IS VaVaI

<a href="https://www.isvavai.cz/riv?ss=detail&h=RIV%2F60461373%3A22310%2F25%3A43933717" target="_blank" >RIV/60461373:22310/25:43933717 - isvavai.cz</a>

Výsledek na webu

<a href="https://onlinelibrary.wiley.com/doi/full/10.1002/EXP.20240362" target="_blank" >https://onlinelibrary.wiley.com/doi/full/10.1002/EXP.20240362</a>

DOI - Digital Object Identifier

<a href="http://dx.doi.org/10.1002/EXP.20240362" target="_blank" >10.1002/EXP.20240362</a>

Jazyk výsledku

angličtina

Název v původním jazyce

Enhancing Bidirectional Sulfur Conversion Through p–dOrbital Hybridization via Vacancy Engineering

Popis výsledku v původním jazyce

Lithium–sulfur batteries (LSBs) have garnered significant concern as materials with high energy density for energy storage. Nevertheless, their severe shuttle effect and delayed redox kinetics limit their practical application. Herein, a strategy based on the regulation of oxygen vacancy concentration in CoWO4 has been proposed to accelerate polysulfide kinetics. Experiments and density functional theory calculations reveal that catalytic materials with the appropriate number of oxygen vacancies (CWO-M) have moderate adsorption energy and optimal catalytic capacity for polysulfides due to strong p–d orbital hybridization. More importantly, CWO-M not only accelerates the reduction of sulfur during discharge but also significantly accelerates the oxidation of Li2S during charging, showing a favorable bidirectional catalytic effect. Benefiting from these unique advantages, the CWO-M/S-based battery exhibits an excellent rate performance of 768 mAh g−1 at 2 C and a capacity retention of 91.1% after 100 cycles at 0.2 C. Stable cycling performance with a high capacity of nearly 4 mAh cm−2 was achieved even after 100 cycles at a high sulfur loading of 8.02 mg cm−2 and a low electrolyte/sulfur (E/S) ratio of 8 µL mg S−1. This work provides significant insights into bidirectional catalysts by modulating the oxygen vacancy concentration for application in LSBs.

Název v anglickém jazyce

Enhancing Bidirectional Sulfur Conversion Through p–dOrbital Hybridization via Vacancy Engineering

Popis výsledku anglicky

Lithium–sulfur batteries (LSBs) have garnered significant concern as materials with high energy density for energy storage. Nevertheless, their severe shuttle effect and delayed redox kinetics limit their practical application. Herein, a strategy based on the regulation of oxygen vacancy concentration in CoWO4 has been proposed to accelerate polysulfide kinetics. Experiments and density functional theory calculations reveal that catalytic materials with the appropriate number of oxygen vacancies (CWO-M) have moderate adsorption energy and optimal catalytic capacity for polysulfides due to strong p–d orbital hybridization. More importantly, CWO-M not only accelerates the reduction of sulfur during discharge but also significantly accelerates the oxidation of Li2S during charging, showing a favorable bidirectional catalytic effect. Benefiting from these unique advantages, the CWO-M/S-based battery exhibits an excellent rate performance of 768 mAh g−1 at 2 C and a capacity retention of 91.1% after 100 cycles at 0.2 C. Stable cycling performance with a high capacity of nearly 4 mAh cm−2 was achieved even after 100 cycles at a high sulfur loading of 8.02 mg cm−2 and a low electrolyte/sulfur (E/S) ratio of 8 µL mg S−1. This work provides significant insights into bidirectional catalysts by modulating the oxygen vacancy concentration for application in LSBs.

Druh

J_SC - Článek v periodiku v databázi SCOPUS

CEP obor

—

OECD FORD obor

10700 - Other natural sciences

Projekt

—

Návaznosti

I - Institucionalni podpora na dlouhodoby koncepcni rozvoj vyzkumne organizace

Rok uplatnění

2025

Kód důvěrnosti údajů

S - Úplné a pravdivé údaje o projektu nepodléhají ochraně podle zvláštních právních předpisů

Název periodika

Exploration

ISSN

2766-8509

e-ISSN

2766-2098

Svazek periodika

5

Číslo periodika v rámci svazku

6

Stát vydavatele periodika

CN - Čínská lidová republika

Počet stran výsledku

11

Strana od-do

20240362

Kód UT WoS článku

—

EID výsledku v databázi Scopus

2-s2.0-105014122418