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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Wiley
2023-03-01
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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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