Cofactor‐Assisted Artificial Enzyme with Multiple Li‐Bond Networks for Sustainable Polysulfide Conversion in Lithium–Sulfur Batteries
Abstract Lithium–sulfur batteries possess high theoretical energy density but suffer from rapid capacity fade due to the shuttling and sluggish conversion of polysulfides. Aiming at these problems, a biomimetic design of cofactor‐assisted artificial enzyme catalyst, melamine (MM) crosslinked hemin o...
| Main Authors: | , , , , , , , |
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| Format: | Article |
| Language: | English |
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Wiley
2022-01-01
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| Series: | Advanced Science |
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| Online Access: | https://doi.org/10.1002/advs.202104205 |
| _version_ | 1818952542456905728 |
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| author | Suya Zhou Shuo Yang Dong Cai Ce Liang Shuang Yu Yue Hu Huagui Nie Zhi Yang |
| author_facet | Suya Zhou Shuo Yang Dong Cai Ce Liang Shuang Yu Yue Hu Huagui Nie Zhi Yang |
| author_sort | Suya Zhou |
| collection | DOAJ |
| description | Abstract Lithium–sulfur batteries possess high theoretical energy density but suffer from rapid capacity fade due to the shuttling and sluggish conversion of polysulfides. Aiming at these problems, a biomimetic design of cofactor‐assisted artificial enzyme catalyst, melamine (MM) crosslinked hemin on carboxylated carbon nanotubes (CNTs) (i.e., [CNTs–MM–hemin]), is presented to efficiently convert polysulfides. The MM cofactors bind with the hemin artificial enzymes and CNT conductive substrates through FeN5 coordination and/or covalent amide bonds to provide high and durable catalytic activity for polysulfide conversions, while π–π conjugations between hemin and CNTs and multiple Li‐bond networks offered by MM endow the cathode with good electronic/Li+ transmission ability. This synergistic mechanism enables rapid sulfur reaction kinetics, alleviated polysulfide shuttling, and an ultralow (<1.3%) loss of hemin active sites in electrolyte, which is ≈60 times lower than those of noncovalent crosslinked samples. As a result, the Li–S battery using [CNTs–MM–hemin] cathode retains a capacity of 571 mAh g−1 after 900 cycles at 1C with an ultralow capacity decay rate of 0.046% per cycle. Even under raising sulfur loadings up to 7.5 mg cm−2, the cathode still can steadily run 110 cycles with a capacity retention of 83%. |
| first_indexed | 2024-12-20T09:52:02Z |
| format | Article |
| id | doaj.art-7487fd71f1984871aec50430d9f0e6a5 |
| institution | Directory Open Access Journal |
| issn | 2198-3844 |
| language | English |
| last_indexed | 2024-12-20T09:52:02Z |
| publishDate | 2022-01-01 |
| publisher | Wiley |
| record_format | Article |
| series | Advanced Science |
| spelling | doaj.art-7487fd71f1984871aec50430d9f0e6a52022-12-21T19:44:34ZengWileyAdvanced Science2198-38442022-01-0193n/an/a10.1002/advs.202104205Cofactor‐Assisted Artificial Enzyme with Multiple Li‐Bond Networks for Sustainable Polysulfide Conversion in Lithium–Sulfur BatteriesSuya Zhou0Shuo Yang1Dong Cai2Ce Liang3Shuang Yu4Yue Hu5Huagui Nie6Zhi Yang7Key Laboratory of Carbon Materials of Zhejiang Province Wenzhou University Wenzhou 325035 ChinaKey Laboratory of Carbon Materials of Zhejiang Province Wenzhou University Wenzhou 325035 ChinaKey Laboratory of Carbon Materials of Zhejiang Province Wenzhou University Wenzhou 325035 ChinaKey Laboratory of Carbon Materials of Zhejiang Province Wenzhou University Wenzhou 325035 ChinaKey Laboratory of Carbon Materials of Zhejiang Province Wenzhou University Wenzhou 325035 ChinaKey Laboratory of Carbon Materials of Zhejiang Province Wenzhou University Wenzhou 325035 ChinaKey Laboratory of Carbon Materials of Zhejiang Province Wenzhou University Wenzhou 325035 ChinaKey Laboratory of Carbon Materials of Zhejiang Province Wenzhou University Wenzhou 325035 ChinaAbstract Lithium–sulfur batteries possess high theoretical energy density but suffer from rapid capacity fade due to the shuttling and sluggish conversion of polysulfides. Aiming at these problems, a biomimetic design of cofactor‐assisted artificial enzyme catalyst, melamine (MM) crosslinked hemin on carboxylated carbon nanotubes (CNTs) (i.e., [CNTs–MM–hemin]), is presented to efficiently convert polysulfides. The MM cofactors bind with the hemin artificial enzymes and CNT conductive substrates through FeN5 coordination and/or covalent amide bonds to provide high and durable catalytic activity for polysulfide conversions, while π–π conjugations between hemin and CNTs and multiple Li‐bond networks offered by MM endow the cathode with good electronic/Li+ transmission ability. This synergistic mechanism enables rapid sulfur reaction kinetics, alleviated polysulfide shuttling, and an ultralow (<1.3%) loss of hemin active sites in electrolyte, which is ≈60 times lower than those of noncovalent crosslinked samples. As a result, the Li–S battery using [CNTs–MM–hemin] cathode retains a capacity of 571 mAh g−1 after 900 cycles at 1C with an ultralow capacity decay rate of 0.046% per cycle. Even under raising sulfur loadings up to 7.5 mg cm−2, the cathode still can steadily run 110 cycles with a capacity retention of 83%.https://doi.org/10.1002/advs.202104205biomimetic catalystscovalent amide bondsFeN5 coordination structureslithium–sulfur batteriesmultiple Li‐bond networks |
| spellingShingle | Suya Zhou Shuo Yang Dong Cai Ce Liang Shuang Yu Yue Hu Huagui Nie Zhi Yang Cofactor‐Assisted Artificial Enzyme with Multiple Li‐Bond Networks for Sustainable Polysulfide Conversion in Lithium–Sulfur Batteries Advanced Science biomimetic catalysts covalent amide bonds FeN5 coordination structures lithium–sulfur batteries multiple Li‐bond networks |
| title | Cofactor‐Assisted Artificial Enzyme with Multiple Li‐Bond Networks for Sustainable Polysulfide Conversion in Lithium–Sulfur Batteries |
| title_full | Cofactor‐Assisted Artificial Enzyme with Multiple Li‐Bond Networks for Sustainable Polysulfide Conversion in Lithium–Sulfur Batteries |
| title_fullStr | Cofactor‐Assisted Artificial Enzyme with Multiple Li‐Bond Networks for Sustainable Polysulfide Conversion in Lithium–Sulfur Batteries |
| title_full_unstemmed | Cofactor‐Assisted Artificial Enzyme with Multiple Li‐Bond Networks for Sustainable Polysulfide Conversion in Lithium–Sulfur Batteries |
| title_short | Cofactor‐Assisted Artificial Enzyme with Multiple Li‐Bond Networks for Sustainable Polysulfide Conversion in Lithium–Sulfur Batteries |
| title_sort | cofactor assisted artificial enzyme with multiple li bond networks for sustainable polysulfide conversion in lithium sulfur batteries |
| topic | biomimetic catalysts covalent amide bonds FeN5 coordination structures lithium–sulfur batteries multiple Li‐bond networks |
| url | https://doi.org/10.1002/advs.202104205 |
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