Isolated Metalloid Tellurium Atomic Cluster on Nitrogen‐Doped Carbon Nanosheet for High‐Capacity Rechargeable Lithium‐CO2 Battery

Abstract Rechargeable Li‐CO2 battery represents a sustainable technology by virtue of CO2 recyclability and energy storage capability. Unfortunately, the sluggish mass transport and electron transfer in bulky high‐crystalline discharge product of Li2CO3, severely hinder its practical capacity and re...

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Main Authors: Ke Wang, Dongyu Liu, Limin Liu, Xinyang Li, Hu Wu, Zongjie Sun, Mingtao Li, Andrey S. Vasenko, Shujiang Ding, Fengmei Wang, Chunhui Xiao
Format: Article
Language:English
Published: Wiley 2023-03-01
Series:Advanced Science
Subjects:
Online Access:https://doi.org/10.1002/advs.202205959
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author Ke Wang
Dongyu Liu
Limin Liu
Xinyang Li
Hu Wu
Zongjie Sun
Mingtao Li
Andrey S. Vasenko
Shujiang Ding
Fengmei Wang
Chunhui Xiao
author_facet Ke Wang
Dongyu Liu
Limin Liu
Xinyang Li
Hu Wu
Zongjie Sun
Mingtao Li
Andrey S. Vasenko
Shujiang Ding
Fengmei Wang
Chunhui Xiao
author_sort Ke Wang
collection DOAJ
description Abstract Rechargeable Li‐CO2 battery represents a sustainable technology by virtue of CO2 recyclability and energy storage capability. Unfortunately, the sluggish mass transport and electron transfer in bulky high‐crystalline discharge product of Li2CO3, severely hinder its practical capacity and rechargeability. Herein, a heterostructure of isolated metalloid Te atomic cluster anchored on N‐doped carbon nanosheets is designed (TeAC@NCNS) as a metal‐free cathode for Li‐CO2 battery. X‐ray absorption spectroscopy analysis demonstrates that the abundant and dispersed Te active centers can be stabilized by C atoms in form of the covalent bond. The fabricated battery shows an unprecedented full‐discharge capacity of 28.35 mAh cm−2 at 0.05 mA cm−2 and long‐term cycle life of up to 1000 h even at a high cut‐off capacity of 1 mAh cm−2. A series of ex situ characterizations combined with theoretical calculations demonstrate that the abundant Te atomic clusters acting as active centers can drive the electron redistribution of carbonate via forming TeO bonds, giving rise to poor‐crystalline Li2CO3 film during the discharge process. Moreover, the efficient electron transfer between the Te centers and intermediate species is energetically beneficial for nucleation and accelerates the decomposition of Li2CO3 on the TeAC@NCNS during the discharge/charge process.
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spelling doaj.art-e179a55ac0e44cf293981a00777738732023-03-03T08:59:14ZengWileyAdvanced Science2198-38442023-03-01107n/an/a10.1002/advs.202205959Isolated Metalloid Tellurium Atomic Cluster on Nitrogen‐Doped Carbon Nanosheet for High‐Capacity Rechargeable Lithium‐CO2 BatteryKe Wang0Dongyu Liu1Limin Liu2Xinyang Li3Hu Wu4Zongjie Sun5Mingtao Li6Andrey S. Vasenko7Shujiang Ding8Fengmei Wang9Chunhui Xiao10Xi'an Key Laboratory of Sustainable Energy Materials Chemistry School of Chemistry Energy Storage Materials and Chemistry of Shaanxi University Engineering Research Center Xi'an Jiaotong University 28 Xianning West Road Xi'an Shaanxi 710049 ChinaNational Research University Higher School of Economics (HSE University) 20 Myasnitskaya Str.  Moscow 101000 RussiaXi'an Key Laboratory of Sustainable Energy Materials Chemistry School of Chemistry Energy Storage Materials and Chemistry of Shaanxi University Engineering Research Center Xi'an Jiaotong University 28 Xianning West Road Xi'an Shaanxi 710049 ChinaXi'an Key Laboratory of Sustainable Energy Materials Chemistry School of Chemistry Energy Storage Materials and Chemistry of Shaanxi University Engineering Research Center Xi'an Jiaotong University 28 Xianning West Road Xi'an Shaanxi 710049 ChinaXi'an Key Laboratory of Sustainable Energy Materials Chemistry School of Chemistry Energy Storage Materials and Chemistry of Shaanxi University Engineering Research Center Xi'an Jiaotong University 28 Xianning West Road Xi'an Shaanxi 710049 ChinaXi'an Key Laboratory of Sustainable Energy Materials Chemistry School of Chemistry Energy Storage Materials and Chemistry of Shaanxi University Engineering Research Center Xi'an Jiaotong University 28 Xianning West Road Xi'an Shaanxi 710049 ChinaInternational Research Center for Renewable Energy (IRCRE) State Key Laboratory of Multiphase Flow in Power Engineering (MFPE) Xi'an Jiaotong University 28 Xianning West Road Xi'an Shaanxi 710049 ChinaNational Research University Higher School of Economics (HSE University) 20 Myasnitskaya Str.  Moscow 101000 RussiaXi'an Key Laboratory of Sustainable Energy Materials Chemistry School of Chemistry Energy Storage Materials and Chemistry of Shaanxi University Engineering Research Center Xi'an Jiaotong University 28 Xianning West Road Xi'an Shaanxi 710049 ChinaState Key Laboratory of Chemical Resource Engineering Beijing Advanced Innovation Center for Soft Matter Science and Engineering Beijing University of Chemical Technology Beijing 100029 ChinaXi'an Key Laboratory of Sustainable Energy Materials Chemistry School of Chemistry Energy Storage Materials and Chemistry of Shaanxi University Engineering Research Center Xi'an Jiaotong University 28 Xianning West Road Xi'an Shaanxi 710049 ChinaAbstract Rechargeable Li‐CO2 battery represents a sustainable technology by virtue of CO2 recyclability and energy storage capability. Unfortunately, the sluggish mass transport and electron transfer in bulky high‐crystalline discharge product of Li2CO3, severely hinder its practical capacity and rechargeability. Herein, a heterostructure of isolated metalloid Te atomic cluster anchored on N‐doped carbon nanosheets is designed (TeAC@NCNS) as a metal‐free cathode for Li‐CO2 battery. X‐ray absorption spectroscopy analysis demonstrates that the abundant and dispersed Te active centers can be stabilized by C atoms in form of the covalent bond. The fabricated battery shows an unprecedented full‐discharge capacity of 28.35 mAh cm−2 at 0.05 mA cm−2 and long‐term cycle life of up to 1000 h even at a high cut‐off capacity of 1 mAh cm−2. A series of ex situ characterizations combined with theoretical calculations demonstrate that the abundant Te atomic clusters acting as active centers can drive the electron redistribution of carbonate via forming TeO bonds, giving rise to poor‐crystalline Li2CO3 film during the discharge process. Moreover, the efficient electron transfer between the Te centers and intermediate species is energetically beneficial for nucleation and accelerates the decomposition of Li2CO3 on the TeAC@NCNS during the discharge/charge process.https://doi.org/10.1002/advs.202205959amorphous discharge productfree‐standing electrodemetal‐free catalystmetalloid catalystrechargeable Li‐CO2 battery
spellingShingle Ke Wang
Dongyu Liu
Limin Liu
Xinyang Li
Hu Wu
Zongjie Sun
Mingtao Li
Andrey S. Vasenko
Shujiang Ding
Fengmei Wang
Chunhui Xiao
Isolated Metalloid Tellurium Atomic Cluster on Nitrogen‐Doped Carbon Nanosheet for High‐Capacity Rechargeable Lithium‐CO2 Battery
Advanced Science
amorphous discharge product
free‐standing electrode
metal‐free catalyst
metalloid catalyst
rechargeable Li‐CO2 battery
title Isolated Metalloid Tellurium Atomic Cluster on Nitrogen‐Doped Carbon Nanosheet for High‐Capacity Rechargeable Lithium‐CO2 Battery
title_full Isolated Metalloid Tellurium Atomic Cluster on Nitrogen‐Doped Carbon Nanosheet for High‐Capacity Rechargeable Lithium‐CO2 Battery
title_fullStr Isolated Metalloid Tellurium Atomic Cluster on Nitrogen‐Doped Carbon Nanosheet for High‐Capacity Rechargeable Lithium‐CO2 Battery
title_full_unstemmed Isolated Metalloid Tellurium Atomic Cluster on Nitrogen‐Doped Carbon Nanosheet for High‐Capacity Rechargeable Lithium‐CO2 Battery
title_short Isolated Metalloid Tellurium Atomic Cluster on Nitrogen‐Doped Carbon Nanosheet for High‐Capacity Rechargeable Lithium‐CO2 Battery
title_sort isolated metalloid tellurium atomic cluster on nitrogen doped carbon nanosheet for high capacity rechargeable lithium co2 battery
topic amorphous discharge product
free‐standing electrode
metal‐free catalyst
metalloid catalyst
rechargeable Li‐CO2 battery
url https://doi.org/10.1002/advs.202205959
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