Revealing an Extended Adsorption/Insertion‐Filling Sodium Storage Mechanism in Petroleum Coke‐Derived Amorphous Carbon

Abstract Amorphous carbon holds great promise as anode material for sodium‐ion batteries due to its cost‐effectiveness and good performance. However, its sodium storage mechanism, particularly the insertion process and origin of plateau capacity, remains controversial. Here, an extended adsorption/i...

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Main Authors: Jia‐He Lv, Jing‐Song Wang, Bin He, Tao Wu, An‐Hui Lu, Wenrui Zhang, Juping Xu, Wen Yin, Guang‐Ping Hao, Wen‐Cui Li
Format: Article
Language:English
Published: Wiley 2024-11-01
Series:Advanced Science
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Online Access:https://doi.org/10.1002/advs.202407538
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author Jia‐He Lv
Jing‐Song Wang
Bin He
Tao Wu
An‐Hui Lu
Wenrui Zhang
Juping Xu
Wen Yin
Guang‐Ping Hao
Wen‐Cui Li
author_facet Jia‐He Lv
Jing‐Song Wang
Bin He
Tao Wu
An‐Hui Lu
Wenrui Zhang
Juping Xu
Wen Yin
Guang‐Ping Hao
Wen‐Cui Li
author_sort Jia‐He Lv
collection DOAJ
description Abstract Amorphous carbon holds great promise as anode material for sodium‐ion batteries due to its cost‐effectiveness and good performance. However, its sodium storage mechanism, particularly the insertion process and origin of plateau capacity, remains controversial. Here, an extended adsorption/insertion‐filling sodium storage mechanism is proposed using petroleum coke‐derived amorphous carbon as a multi‐microcrystalline model. Combining in situ X‐ray diffraction, in situ Raman, theoretical calculations, and neutron scattering, the effective storage form and location of sodium ions in amorphous carbon are revealed. The sodium adsorption at defect sites leads to a high‐potential sloping capacity. The sodium insertion process occurs in both the pseudo‐graphite phase (d002 > 0.370 nm) and graphite‐like phase (0.345 ≤ d002 < 0.370 nm) rather than the graphite phase, contributing to low‐potential sloping capacity. The sodium filling into accessible closed pores forms quasi‐metallic sodium clusters, contributing to plateau capacity. The threshold of the effective interlayer spacing for sodium insertion is extended to 0.345 nm, breaking the consensus of insertion interlayer threshold and enhancing understanding of closed pore filling. The extended adsorption/insertion‐filling mechanism explains the sodium storage behavior of amorphous carbon with different microstructures, providing theoretical guidance for the rational design of high‐performance amorphous carbon anodes.
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spelling doaj-art-ee2eac1ced0547a4b80dd46fb9e7625f2025-08-20T02:15:32ZengWileyAdvanced Science2198-38442024-11-011142n/an/a10.1002/advs.202407538Revealing an Extended Adsorption/Insertion‐Filling Sodium Storage Mechanism in Petroleum Coke‐Derived Amorphous CarbonJia‐He Lv0Jing‐Song Wang1Bin He2Tao Wu3An‐Hui Lu4Wenrui Zhang5Juping Xu6Wen Yin7Guang‐Ping Hao8Wen‐Cui Li9State Key Laboratory of Fine Chemicals School of Chemical Engineering Dalian University of Technology Dalian 116024 P. R. ChinaState Key Laboratory of Fine Chemicals School of Chemical Engineering Dalian University of Technology Dalian 116024 P. R. ChinaState Key Laboratory of Fine Chemicals School of Chemical Engineering Dalian University of Technology Dalian 116024 P. R. ChinaState Key Laboratory of Fine Chemicals School of Chemical Engineering Dalian University of Technology Dalian 116024 P. R. ChinaState Key Laboratory of Fine Chemicals School of Chemical Engineering Dalian University of Technology Dalian 116024 P. R. ChinaState Key Laboratory of Fine Chemicals School of Chemical Engineering Dalian University of Technology Dalian 116024 P. R. ChinaSpallation Neutron Source Science Center Dongguan 523803 P. R. ChinaSpallation Neutron Source Science Center Dongguan 523803 P. R. ChinaState Key Laboratory of Fine Chemicals School of Chemical Engineering Dalian University of Technology Dalian 116024 P. R. ChinaState Key Laboratory of Fine Chemicals School of Chemical Engineering Dalian University of Technology Dalian 116024 P. R. ChinaAbstract Amorphous carbon holds great promise as anode material for sodium‐ion batteries due to its cost‐effectiveness and good performance. However, its sodium storage mechanism, particularly the insertion process and origin of plateau capacity, remains controversial. Here, an extended adsorption/insertion‐filling sodium storage mechanism is proposed using petroleum coke‐derived amorphous carbon as a multi‐microcrystalline model. Combining in situ X‐ray diffraction, in situ Raman, theoretical calculations, and neutron scattering, the effective storage form and location of sodium ions in amorphous carbon are revealed. The sodium adsorption at defect sites leads to a high‐potential sloping capacity. The sodium insertion process occurs in both the pseudo‐graphite phase (d002 > 0.370 nm) and graphite‐like phase (0.345 ≤ d002 < 0.370 nm) rather than the graphite phase, contributing to low‐potential sloping capacity. The sodium filling into accessible closed pores forms quasi‐metallic sodium clusters, contributing to plateau capacity. The threshold of the effective interlayer spacing for sodium insertion is extended to 0.345 nm, breaking the consensus of insertion interlayer threshold and enhancing understanding of closed pore filling. The extended adsorption/insertion‐filling mechanism explains the sodium storage behavior of amorphous carbon with different microstructures, providing theoretical guidance for the rational design of high‐performance amorphous carbon anodes.https://doi.org/10.1002/advs.202407538closed pore fillinginterlayer insertionpetroleum cokesodium storage mechanismsodium‐ion batteries
spellingShingle Jia‐He Lv
Jing‐Song Wang
Bin He
Tao Wu
An‐Hui Lu
Wenrui Zhang
Juping Xu
Wen Yin
Guang‐Ping Hao
Wen‐Cui Li
Revealing an Extended Adsorption/Insertion‐Filling Sodium Storage Mechanism in Petroleum Coke‐Derived Amorphous Carbon
Advanced Science
closed pore filling
interlayer insertion
petroleum coke
sodium storage mechanism
sodium‐ion batteries
title Revealing an Extended Adsorption/Insertion‐Filling Sodium Storage Mechanism in Petroleum Coke‐Derived Amorphous Carbon
title_full Revealing an Extended Adsorption/Insertion‐Filling Sodium Storage Mechanism in Petroleum Coke‐Derived Amorphous Carbon
title_fullStr Revealing an Extended Adsorption/Insertion‐Filling Sodium Storage Mechanism in Petroleum Coke‐Derived Amorphous Carbon
title_full_unstemmed Revealing an Extended Adsorption/Insertion‐Filling Sodium Storage Mechanism in Petroleum Coke‐Derived Amorphous Carbon
title_short Revealing an Extended Adsorption/Insertion‐Filling Sodium Storage Mechanism in Petroleum Coke‐Derived Amorphous Carbon
title_sort revealing an extended adsorption insertion filling sodium storage mechanism in petroleum coke derived amorphous carbon
topic closed pore filling
interlayer insertion
petroleum coke
sodium storage mechanism
sodium‐ion batteries
url https://doi.org/10.1002/advs.202407538
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