Unlocking Modulation Rule of Heterointerface Engineering Induced D‐Band Center on Polysulfides Conversion in Lithium–Sulfur Batteries
Abstract MOF‐derived heterostructures have been widely utilized as S hosts to address the three issues faced by the sulfur (S) cathode in lithium–sulfur batteries. Precisely pinpointing the active center in the heterostructure and unlocking the modulation rule of heterostructure on polysulfides (LiP...
Saved in:
| Main Authors: | , , , , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
Wiley
2025-05-01
|
| Series: | Advanced Science |
| Subjects: | |
| Online Access: | https://doi.org/10.1002/advs.202501940 |
| Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
| _version_ | 1849324086260400128 |
|---|---|
| author | Wenbin Li Ni Wang Jingjie Pei Dongyan Li Guiqiang Cao Ruixian Duan Jingjing Wang Xifei Li |
| author_facet | Wenbin Li Ni Wang Jingjie Pei Dongyan Li Guiqiang Cao Ruixian Duan Jingjing Wang Xifei Li |
| author_sort | Wenbin Li |
| collection | DOAJ |
| description | Abstract MOF‐derived heterostructures have been widely utilized as S hosts to address the three issues faced by the sulfur (S) cathode in lithium–sulfur batteries. Precisely pinpointing the active center in the heterostructure and unlocking the modulation rule of heterostructure on polysulfides (LiPSs) conversion are particularly important. Herein, the two homologous hetero‐hosts of ZIF‐67‐derived CoSe2@CoSe0.25S1.75/NC and CoSe2@CoS2/NC nanoparticles anchored in the nitrogen‐doped carbon (NC) matrix are successfully constructed, and confirm that Co at the heterointerface is the primary active center, rather than Co within the individual phases. It is revealed that the ɛd (d‐band center) of Co in the heterostructure can be a significant descriptor for the adsorption ability and conversion ability to LiPSs, and the discharge‐specific capacities, which describe a volcano curve as a function of εd. It is also found that the best Li+ storage property appears at CoSe2@CoSe0.25S1.75 heterointerface among the five structures (CoSe2@CoSe0.25S1.75, CoSe2@CoS2, CoSe0.25S1.75, CoSe2, CoS2). The capacity is up to 600 mAh g−1 with a large retention rate of 73.3% at 0.2 C after 100 cycles, and the capacity decay rate is only 0.083% per cycle at 1 C during 300 long‐cycling process. |
| format | Article |
| id | doaj-art-d36c106f0d714958bef24b478974daa0 |
| institution | Kabale University |
| issn | 2198-3844 |
| language | English |
| publishDate | 2025-05-01 |
| publisher | Wiley |
| record_format | Article |
| series | Advanced Science |
| spelling | doaj-art-d36c106f0d714958bef24b478974daa02025-08-20T03:48:47ZengWileyAdvanced Science2198-38442025-05-011217n/an/a10.1002/advs.202501940Unlocking Modulation Rule of Heterointerface Engineering Induced D‐Band Center on Polysulfides Conversion in Lithium–Sulfur BatteriesWenbin Li0Ni Wang1Jingjie Pei2Dongyan Li3Guiqiang Cao4Ruixian Duan5Jingjing Wang6Xifei Li7Institute of Advanced Electrochemical Energy and School of Materials Science and EngineeringXi'an University of TechnologyXi'an 710048 ChinaInstitute of Advanced Electrochemical Energy and School of Materials Science and EngineeringXi'an University of TechnologyXi'an 710048 ChinaInstitute of Advanced Electrochemical Energy and School of Materials Science and EngineeringXi'an University of TechnologyXi'an 710048 ChinaInstitute of Advanced Electrochemical Energy and School of Materials Science and EngineeringXi'an University of TechnologyXi'an 710048 ChinaInstitute of Advanced Electrochemical Energy and School of Materials Science and EngineeringXi'an University of TechnologyXi'an 710048 ChinaInstitute of Advanced Electrochemical Energy and School of Materials Science and EngineeringXi'an University of TechnologyXi'an 710048 ChinaInstitute of Advanced Electrochemical Energy and School of Materials Science and EngineeringXi'an University of TechnologyXi'an 710048 ChinaInstitute of Advanced Electrochemical Energy and School of Materials Science and EngineeringXi'an University of TechnologyXi'an 710048 ChinaAbstract MOF‐derived heterostructures have been widely utilized as S hosts to address the three issues faced by the sulfur (S) cathode in lithium–sulfur batteries. Precisely pinpointing the active center in the heterostructure and unlocking the modulation rule of heterostructure on polysulfides (LiPSs) conversion are particularly important. Herein, the two homologous hetero‐hosts of ZIF‐67‐derived CoSe2@CoSe0.25S1.75/NC and CoSe2@CoS2/NC nanoparticles anchored in the nitrogen‐doped carbon (NC) matrix are successfully constructed, and confirm that Co at the heterointerface is the primary active center, rather than Co within the individual phases. It is revealed that the ɛd (d‐band center) of Co in the heterostructure can be a significant descriptor for the adsorption ability and conversion ability to LiPSs, and the discharge‐specific capacities, which describe a volcano curve as a function of εd. It is also found that the best Li+ storage property appears at CoSe2@CoSe0.25S1.75 heterointerface among the five structures (CoSe2@CoSe0.25S1.75, CoSe2@CoS2, CoSe0.25S1.75, CoSe2, CoS2). The capacity is up to 600 mAh g−1 with a large retention rate of 73.3% at 0.2 C after 100 cycles, and the capacity decay rate is only 0.083% per cycle at 1 C during 300 long‐cycling process.https://doi.org/10.1002/advs.202501940d‐band centerheterointerface engineeringlithium–sulfur batteriespolysulfides conversionsulfur cathode host |
| spellingShingle | Wenbin Li Ni Wang Jingjie Pei Dongyan Li Guiqiang Cao Ruixian Duan Jingjing Wang Xifei Li Unlocking Modulation Rule of Heterointerface Engineering Induced D‐Band Center on Polysulfides Conversion in Lithium–Sulfur Batteries Advanced Science d‐band center heterointerface engineering lithium–sulfur batteries polysulfides conversion sulfur cathode host |
| title | Unlocking Modulation Rule of Heterointerface Engineering Induced D‐Band Center on Polysulfides Conversion in Lithium–Sulfur Batteries |
| title_full | Unlocking Modulation Rule of Heterointerface Engineering Induced D‐Band Center on Polysulfides Conversion in Lithium–Sulfur Batteries |
| title_fullStr | Unlocking Modulation Rule of Heterointerface Engineering Induced D‐Band Center on Polysulfides Conversion in Lithium–Sulfur Batteries |
| title_full_unstemmed | Unlocking Modulation Rule of Heterointerface Engineering Induced D‐Band Center on Polysulfides Conversion in Lithium–Sulfur Batteries |
| title_short | Unlocking Modulation Rule of Heterointerface Engineering Induced D‐Band Center on Polysulfides Conversion in Lithium–Sulfur Batteries |
| title_sort | unlocking modulation rule of heterointerface engineering induced d band center on polysulfides conversion in lithium sulfur batteries |
| topic | d‐band center heterointerface engineering lithium–sulfur batteries polysulfides conversion sulfur cathode host |
| url | https://doi.org/10.1002/advs.202501940 |
| work_keys_str_mv | AT wenbinli unlockingmodulationruleofheterointerfaceengineeringinduceddbandcenteronpolysulfidesconversioninlithiumsulfurbatteries AT niwang unlockingmodulationruleofheterointerfaceengineeringinduceddbandcenteronpolysulfidesconversioninlithiumsulfurbatteries AT jingjiepei unlockingmodulationruleofheterointerfaceengineeringinduceddbandcenteronpolysulfidesconversioninlithiumsulfurbatteries AT dongyanli unlockingmodulationruleofheterointerfaceengineeringinduceddbandcenteronpolysulfidesconversioninlithiumsulfurbatteries AT guiqiangcao unlockingmodulationruleofheterointerfaceengineeringinduceddbandcenteronpolysulfidesconversioninlithiumsulfurbatteries AT ruixianduan unlockingmodulationruleofheterointerfaceengineeringinduceddbandcenteronpolysulfidesconversioninlithiumsulfurbatteries AT jingjingwang unlockingmodulationruleofheterointerfaceengineeringinduceddbandcenteronpolysulfidesconversioninlithiumsulfurbatteries AT xifeili unlockingmodulationruleofheterointerfaceengineeringinduceddbandcenteronpolysulfidesconversioninlithiumsulfurbatteries |