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High Crystallinity 2D π–d Conjugated Conductive Metal–Organic Framework for Boosting Polysulfide Conversion in Lithium–Sulfur Batteries

The catalytic performance of metal–organic frameworks (MOFs) in Li‐S batteries is significantly hindered by unsuitable pore size, low conductivity, and large steric contact hindrance between the catalytic site and lithium polysulfide (LPSs). Herein, the smallest π‐conjugated hexaaminobenzene (HAB) a...

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Autores principales: Guo, Tong, Ding, Yichen, Xu, Chang, Bai, Wuxin, Pan, Shencheng, Liu, Mingliang, Bi, Min, Sun, Jingwen, Ouyang, Xiaoping, Wang, Xin, Fu, Yongsheng, Zhu, Junwu
Formato: Online Artículo Texto
Lenguaje:English
Publicado: John Wiley and Sons Inc. 2023
Materias:
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10520645/
https://www.ncbi.nlm.nih.gov/pubmed/37505447
http://dx.doi.org/10.1002/advs.202302518
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author Guo, Tong
Ding, Yichen
Xu, Chang
Bai, Wuxin
Pan, Shencheng
Liu, Mingliang
Bi, Min
Sun, Jingwen
Ouyang, Xiaoping
Wang, Xin
Fu, Yongsheng
Zhu, Junwu
author_facet Guo, Tong
Ding, Yichen
Xu, Chang
Bai, Wuxin
Pan, Shencheng
Liu, Mingliang
Bi, Min
Sun, Jingwen
Ouyang, Xiaoping
Wang, Xin
Fu, Yongsheng
Zhu, Junwu
author_sort Guo, Tong
collection PubMed
description The catalytic performance of metal–organic frameworks (MOFs) in Li‐S batteries is significantly hindered by unsuitable pore size, low conductivity, and large steric contact hindrance between the catalytic site and lithium polysulfide (LPSs). Herein, the smallest π‐conjugated hexaaminobenzene (HAB) as linker and Ni(II) ions as skeletal node are in situ assembled into high crystallinity Ni‐HAB 2D conductive MOFs with dense Ni‐N(4) units via dsp(2) hybridization on the surface of carbon nanotube (CNT), fabricating Ni‐HAB@CNT as separator modified layer in Li‐S batteries. As‐obtained unique π‐d conjugated Ni‐HAB nanostructure features ordered micropores with suitable pore size (≈8 Å) induced by HAB ligands, which can cooperate with dense Ni‐N(4) chemisorption sites to effectively suppress the shuttle effect. Meanwhile, the conversion kinetics of LPSs is significantly accelerated owing to the small steric contact hindrance and increased delocalized electron density endued by the planar tetracoordinate structure. Consequently, the Li‐S battery with Ni‐HAB@CNT modified separator achieves an areal capacity of 6.29 mAh cm(−2) at high sulfur loading of 6.5 mg cm(−2) under electrolyte/sulfur ratio of 5 µL mg(−1). Moreover, Li‐S single‐electrode pouch cells with modified separators deliver a high reversible capacity of 791 mAh g(−1) after 50 cycles at 0.1 C with electrolyte/sulfur ratio of 6 µL mg(−1).
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spelling pubmed-105206452023-09-27 High Crystallinity 2D π–d Conjugated Conductive Metal–Organic Framework for Boosting Polysulfide Conversion in Lithium–Sulfur Batteries Guo, Tong Ding, Yichen Xu, Chang Bai, Wuxin Pan, Shencheng Liu, Mingliang Bi, Min Sun, Jingwen Ouyang, Xiaoping Wang, Xin Fu, Yongsheng Zhu, Junwu Adv Sci (Weinh) Research Articles The catalytic performance of metal–organic frameworks (MOFs) in Li‐S batteries is significantly hindered by unsuitable pore size, low conductivity, and large steric contact hindrance between the catalytic site and lithium polysulfide (LPSs). Herein, the smallest π‐conjugated hexaaminobenzene (HAB) as linker and Ni(II) ions as skeletal node are in situ assembled into high crystallinity Ni‐HAB 2D conductive MOFs with dense Ni‐N(4) units via dsp(2) hybridization on the surface of carbon nanotube (CNT), fabricating Ni‐HAB@CNT as separator modified layer in Li‐S batteries. As‐obtained unique π‐d conjugated Ni‐HAB nanostructure features ordered micropores with suitable pore size (≈8 Å) induced by HAB ligands, which can cooperate with dense Ni‐N(4) chemisorption sites to effectively suppress the shuttle effect. Meanwhile, the conversion kinetics of LPSs is significantly accelerated owing to the small steric contact hindrance and increased delocalized electron density endued by the planar tetracoordinate structure. Consequently, the Li‐S battery with Ni‐HAB@CNT modified separator achieves an areal capacity of 6.29 mAh cm(−2) at high sulfur loading of 6.5 mg cm(−2) under electrolyte/sulfur ratio of 5 µL mg(−1). Moreover, Li‐S single‐electrode pouch cells with modified separators deliver a high reversible capacity of 791 mAh g(−1) after 50 cycles at 0.1 C with electrolyte/sulfur ratio of 6 µL mg(−1). John Wiley and Sons Inc. 2023-07-28 /pmc/articles/PMC10520645/ /pubmed/37505447 http://dx.doi.org/10.1002/advs.202302518 Text en © 2023 The Authors. Advanced Science published by Wiley‐VCH GmbH https://creativecommons.org/licenses/by/4.0/This is an open access article under the terms of the http://creativecommons.org/licenses/by/4.0/ (https://creativecommons.org/licenses/by/4.0/) License, which permits use, distribution and reproduction in any medium, provided the original work is properly cited.
spellingShingle Research Articles
Guo, Tong
Ding, Yichen
Xu, Chang
Bai, Wuxin
Pan, Shencheng
Liu, Mingliang
Bi, Min
Sun, Jingwen
Ouyang, Xiaoping
Wang, Xin
Fu, Yongsheng
Zhu, Junwu
High Crystallinity 2D π–d Conjugated Conductive Metal–Organic Framework for Boosting Polysulfide Conversion in Lithium–Sulfur Batteries
title High Crystallinity 2D π–d Conjugated Conductive Metal–Organic Framework for Boosting Polysulfide Conversion in Lithium–Sulfur Batteries
title_full High Crystallinity 2D π–d Conjugated Conductive Metal–Organic Framework for Boosting Polysulfide Conversion in Lithium–Sulfur Batteries
title_fullStr High Crystallinity 2D π–d Conjugated Conductive Metal–Organic Framework for Boosting Polysulfide Conversion in Lithium–Sulfur Batteries
title_full_unstemmed High Crystallinity 2D π–d Conjugated Conductive Metal–Organic Framework for Boosting Polysulfide Conversion in Lithium–Sulfur Batteries
title_short High Crystallinity 2D π–d Conjugated Conductive Metal–Organic Framework for Boosting Polysulfide Conversion in Lithium–Sulfur Batteries
title_sort high crystallinity 2d π–d conjugated conductive metal–organic framework for boosting polysulfide conversion in lithium–sulfur batteries
topic Research Articles
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10520645/
https://www.ncbi.nlm.nih.gov/pubmed/37505447
http://dx.doi.org/10.1002/advs.202302518
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