Revealing the Selective Bifunctional Electrocatalytic Sites via In Situ Irradiated X‐Ray Photoelectron Spectroscopy for Lithium–Sulfur Battery

Abstract The electrocatalysts are widely applied in lithium–sulfur (Li–S) batteries to selectively accelerate the redox kinetics behavior of Li2S, in which bifunctional active sites are established, thereby improving the electrochemical performance of the battery. Considering that the Li–S battery i...

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Main Authors: Pengpeng Zhang, Yige Zhao, Yukun Li, Neng Li, S. Ravi P. Silva, Guosheng Shao, Peng Zhang
Format: Article
Language:English
Published: Wiley 2023-03-01
Series:Advanced Science
Subjects:
Online Access:https://doi.org/10.1002/advs.202206786
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author Pengpeng Zhang
Yige Zhao
Yukun Li
Neng Li
S. Ravi P. Silva
Guosheng Shao
Peng Zhang
author_facet Pengpeng Zhang
Yige Zhao
Yukun Li
Neng Li
S. Ravi P. Silva
Guosheng Shao
Peng Zhang
author_sort Pengpeng Zhang
collection DOAJ
description Abstract The electrocatalysts are widely applied in lithium–sulfur (Li–S) batteries to selectively accelerate the redox kinetics behavior of Li2S, in which bifunctional active sites are established, thereby improving the electrochemical performance of the battery. Considering that the Li–S battery is a complex closed “black box” system, the internal redox reaction routes and active sites cannot be directly observed and monitored especially due to the distribution of potential active‐site structures and their dynamic reconstruction. Empirical evidence demonstrates that traditional electrochemical test methods and theoretical calculations only probe the net result of multi‐factors on an average and whole scale. Herein, based on the amorphous TiO2‐x@Ni selective bifunctional model catalyst, these limitations are overcome by developing a system that couples the light field and in situ irradiated X‐ray photoelectron spectroscopy to synergistically convert the “black box” battery into a “see‐through” battery for direct observation of the charge transportation, thus revealing that amorphous TiO2‐x and Ni nanoparticle as the oxidation and reduction sites selectively promote the decomposition and nucleation of Li2S, respectively. This work provides a universal method to achieve a deeper mechanistic understanding of bidirectional sulfur electrochemistry.
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spelling doaj.art-994cbb243cd248049bf72a88ad16c4dc2023-03-15T13:19:15ZengWileyAdvanced Science2198-38442023-03-01108n/an/a10.1002/advs.202206786Revealing the Selective Bifunctional Electrocatalytic Sites via In Situ Irradiated X‐Ray Photoelectron Spectroscopy for Lithium–Sulfur BatteryPengpeng Zhang0Yige Zhao1Yukun Li2Neng Li3S. Ravi P. Silva4Guosheng Shao5Peng Zhang6State Centre for International Cooperation on Designer Low‐Carbon and Environmental Materials (CDLCEM) Zhengzhou University 100 Kexue Avenue Zhengzhou 450001 ChinaState Centre for International Cooperation on Designer Low‐Carbon and Environmental Materials (CDLCEM) Zhengzhou University 100 Kexue Avenue Zhengzhou 450001 ChinaState Centre for International Cooperation on Designer Low‐Carbon and Environmental Materials (CDLCEM) Zhengzhou University 100 Kexue Avenue Zhengzhou 450001 ChinaState Key Laboratory of Silicate Materials for Architecture Wuhan University of Technology Wuhan 430000 ChinaState Centre for International Cooperation on Designer Low‐Carbon and Environmental Materials (CDLCEM) Zhengzhou University 100 Kexue Avenue Zhengzhou 450001 ChinaState Centre for International Cooperation on Designer Low‐Carbon and Environmental Materials (CDLCEM) Zhengzhou University 100 Kexue Avenue Zhengzhou 450001 ChinaState Centre for International Cooperation on Designer Low‐Carbon and Environmental Materials (CDLCEM) Zhengzhou University 100 Kexue Avenue Zhengzhou 450001 ChinaAbstract The electrocatalysts are widely applied in lithium–sulfur (Li–S) batteries to selectively accelerate the redox kinetics behavior of Li2S, in which bifunctional active sites are established, thereby improving the electrochemical performance of the battery. Considering that the Li–S battery is a complex closed “black box” system, the internal redox reaction routes and active sites cannot be directly observed and monitored especially due to the distribution of potential active‐site structures and their dynamic reconstruction. Empirical evidence demonstrates that traditional electrochemical test methods and theoretical calculations only probe the net result of multi‐factors on an average and whole scale. Herein, based on the amorphous TiO2‐x@Ni selective bifunctional model catalyst, these limitations are overcome by developing a system that couples the light field and in situ irradiated X‐ray photoelectron spectroscopy to synergistically convert the “black box” battery into a “see‐through” battery for direct observation of the charge transportation, thus revealing that amorphous TiO2‐x and Ni nanoparticle as the oxidation and reduction sites selectively promote the decomposition and nucleation of Li2S, respectively. This work provides a universal method to achieve a deeper mechanistic understanding of bidirectional sulfur electrochemistry.https://doi.org/10.1002/advs.202206786directly observationelectrocatalytic sitesin situ irradiation X‐ray photoelectron spectroscopylight fieldselective bifunctional electrocatalyst
spellingShingle Pengpeng Zhang
Yige Zhao
Yukun Li
Neng Li
S. Ravi P. Silva
Guosheng Shao
Peng Zhang
Revealing the Selective Bifunctional Electrocatalytic Sites via In Situ Irradiated X‐Ray Photoelectron Spectroscopy for Lithium–Sulfur Battery
Advanced Science
directly observation
electrocatalytic sites
in situ irradiation X‐ray photoelectron spectroscopy
light field
selective bifunctional electrocatalyst
title Revealing the Selective Bifunctional Electrocatalytic Sites via In Situ Irradiated X‐Ray Photoelectron Spectroscopy for Lithium–Sulfur Battery
title_full Revealing the Selective Bifunctional Electrocatalytic Sites via In Situ Irradiated X‐Ray Photoelectron Spectroscopy for Lithium–Sulfur Battery
title_fullStr Revealing the Selective Bifunctional Electrocatalytic Sites via In Situ Irradiated X‐Ray Photoelectron Spectroscopy for Lithium–Sulfur Battery
title_full_unstemmed Revealing the Selective Bifunctional Electrocatalytic Sites via In Situ Irradiated X‐Ray Photoelectron Spectroscopy for Lithium–Sulfur Battery
title_short Revealing the Selective Bifunctional Electrocatalytic Sites via In Situ Irradiated X‐Ray Photoelectron Spectroscopy for Lithium–Sulfur Battery
title_sort revealing the selective bifunctional electrocatalytic sites via in situ irradiated x ray photoelectron spectroscopy for lithium sulfur battery
topic directly observation
electrocatalytic sites
in situ irradiation X‐ray photoelectron spectroscopy
light field
selective bifunctional electrocatalyst
url https://doi.org/10.1002/advs.202206786
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