Optimizing Reversible Phase‐Transformation of FeS2 Anode via Atomic‐Interface Engineering Toward Fast‐Charging Sodium Storage: Theoretical Predication and Experimental Validation
Abstract Sodium‐storage performance of pyrite FeS2 is greatly improved by constructing various FeS2‐based nanostructures to optimize its ion‐transport kinetics and structural stability. However, less attention has been paid to rapid capacity degradation and electrode failure caused by the irreversib...
Saved in:
| Main Authors: | , , , , , , , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
Wiley
2025-01-01
|
| Series: | Advanced Science |
| Subjects: | |
| Online Access: | https://doi.org/10.1002/advs.202411884 |
| Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
| _version_ | 1841543156398555136 |
|---|---|
| author | Wenxi Zhao Yanbing Zhou Hao Zhou Xinqin Wang Shengjun Sun Xun He Yongsong Luo Binwu Ying Yongchao Yao Xiaoqing Ma Xuping Sun |
| author_facet | Wenxi Zhao Yanbing Zhou Hao Zhou Xinqin Wang Shengjun Sun Xun He Yongsong Luo Binwu Ying Yongchao Yao Xiaoqing Ma Xuping Sun |
| author_sort | Wenxi Zhao |
| collection | DOAJ |
| description | Abstract Sodium‐storage performance of pyrite FeS2 is greatly improved by constructing various FeS2‐based nanostructures to optimize its ion‐transport kinetics and structural stability. However, less attention has been paid to rapid capacity degradation and electrode failure caused by the irreversible phase‐transition of intermediate NaxFeS2 to FeS2 and polysulfides dissolution upon cycling. Under the guidance of theoretical calculations, coupling FeS2 nanoparticles with honeycomb‐like nitrogen‐doped carbon (NC) nanosheet supported single‐atom manganese (SAs Mn) catalyst (FeS2/SAs Mn@NC) via atomic‐interface engineering is proposed to address above challenge. Systematic electrochemical analyses and theoretical results unveil that the functional integration of such two type components can significantly enhance ionic conductivity, accelerate charge transfer efficiency, and improve Na+‐adsorption capability. Particularly, SAs Mn@NC with Mn‐Nx coordination center can reduce the decomposition barrier of Na2S and NaxFeS2 to further accelerate reversible phase transformation of Fe/Na2S→NaFeS2→FeS2 and polysulfides decomposition. As predicted, such FeS2/SAs Mn@NC showcases outstanding rate capability and fascinating cyclic durability. A sequence of kinetic studies and ex situ characterizations provide the comprehensive understanding for ion‐transport kinetics and phase‐transformation process. Its practical use is further demonstrated in sodium‐ion full cell and capacitor with impressive electrochemical capability and excellent energy‐density output. |
| format | Article |
| id | doaj-art-8d30da46e90e49ea8130baca95d0e7a1 |
| institution | Kabale University |
| issn | 2198-3844 |
| language | English |
| publishDate | 2025-01-01 |
| publisher | Wiley |
| record_format | Article |
| series | Advanced Science |
| spelling | doaj-art-8d30da46e90e49ea8130baca95d0e7a12025-01-13T15:29:43ZengWileyAdvanced Science2198-38442025-01-01122n/an/a10.1002/advs.202411884Optimizing Reversible Phase‐Transformation of FeS2 Anode via Atomic‐Interface Engineering Toward Fast‐Charging Sodium Storage: Theoretical Predication and Experimental ValidationWenxi Zhao0Yanbing Zhou1Hao Zhou2Xinqin Wang3Shengjun Sun4Xun He5Yongsong Luo6Binwu Ying7Yongchao Yao8Xiaoqing Ma9Xuping Sun10School of Electronic Information Engineering Yangtze Normal University Fuling Chongqing 408100 ChinaDepartment of Laboratory Medicine West China Hospital Sichuan University Chengdu Sichuan 610041 ChinaSchool of Electronic Information Engineering Yangtze Normal University Fuling Chongqing 408100 ChinaSchool of Electronic Engineering Lanzhou City University Lanzhou Gansu 730070 ChinaCollege of Chemistry, Chemical Engineering and Materials Science Shandong Normal University Jinan Shandong 250014 ChinaInstitute of Fundamental and Frontier Sciences University of Electronic Science and Technology of China Chengdu Sichuan 610054 ChinaCenter for High Altitude Medicine West China Hospital Sichuan University Chengdu Sichuan 610041 ChinaDepartment of Laboratory Medicine West China Hospital Sichuan University Chengdu Sichuan 610041 ChinaCenter for High Altitude Medicine West China Hospital Sichuan University Chengdu Sichuan 610041 ChinaSchool of Electronic Information Engineering Yangtze Normal University Fuling Chongqing 408100 ChinaCollege of Chemistry, Chemical Engineering and Materials Science Shandong Normal University Jinan Shandong 250014 ChinaAbstract Sodium‐storage performance of pyrite FeS2 is greatly improved by constructing various FeS2‐based nanostructures to optimize its ion‐transport kinetics and structural stability. However, less attention has been paid to rapid capacity degradation and electrode failure caused by the irreversible phase‐transition of intermediate NaxFeS2 to FeS2 and polysulfides dissolution upon cycling. Under the guidance of theoretical calculations, coupling FeS2 nanoparticles with honeycomb‐like nitrogen‐doped carbon (NC) nanosheet supported single‐atom manganese (SAs Mn) catalyst (FeS2/SAs Mn@NC) via atomic‐interface engineering is proposed to address above challenge. Systematic electrochemical analyses and theoretical results unveil that the functional integration of such two type components can significantly enhance ionic conductivity, accelerate charge transfer efficiency, and improve Na+‐adsorption capability. Particularly, SAs Mn@NC with Mn‐Nx coordination center can reduce the decomposition barrier of Na2S and NaxFeS2 to further accelerate reversible phase transformation of Fe/Na2S→NaFeS2→FeS2 and polysulfides decomposition. As predicted, such FeS2/SAs Mn@NC showcases outstanding rate capability and fascinating cyclic durability. A sequence of kinetic studies and ex situ characterizations provide the comprehensive understanding for ion‐transport kinetics and phase‐transformation process. Its practical use is further demonstrated in sodium‐ion full cell and capacitor with impressive electrochemical capability and excellent energy‐density output.https://doi.org/10.1002/advs.202411884anodehoneycomb‐like FeS2/SAs Mn@NCreversible phase transformationsingle‐atom catalystsodium‐ion batteries |
| spellingShingle | Wenxi Zhao Yanbing Zhou Hao Zhou Xinqin Wang Shengjun Sun Xun He Yongsong Luo Binwu Ying Yongchao Yao Xiaoqing Ma Xuping Sun Optimizing Reversible Phase‐Transformation of FeS2 Anode via Atomic‐Interface Engineering Toward Fast‐Charging Sodium Storage: Theoretical Predication and Experimental Validation Advanced Science anode honeycomb‐like FeS2/SAs Mn@NC reversible phase transformation single‐atom catalyst sodium‐ion batteries |
| title | Optimizing Reversible Phase‐Transformation of FeS2 Anode via Atomic‐Interface Engineering Toward Fast‐Charging Sodium Storage: Theoretical Predication and Experimental Validation |
| title_full | Optimizing Reversible Phase‐Transformation of FeS2 Anode via Atomic‐Interface Engineering Toward Fast‐Charging Sodium Storage: Theoretical Predication and Experimental Validation |
| title_fullStr | Optimizing Reversible Phase‐Transformation of FeS2 Anode via Atomic‐Interface Engineering Toward Fast‐Charging Sodium Storage: Theoretical Predication and Experimental Validation |
| title_full_unstemmed | Optimizing Reversible Phase‐Transformation of FeS2 Anode via Atomic‐Interface Engineering Toward Fast‐Charging Sodium Storage: Theoretical Predication and Experimental Validation |
| title_short | Optimizing Reversible Phase‐Transformation of FeS2 Anode via Atomic‐Interface Engineering Toward Fast‐Charging Sodium Storage: Theoretical Predication and Experimental Validation |
| title_sort | optimizing reversible phase transformation of fes2 anode via atomic interface engineering toward fast charging sodium storage theoretical predication and experimental validation |
| topic | anode honeycomb‐like FeS2/SAs Mn@NC reversible phase transformation single‐atom catalyst sodium‐ion batteries |
| url | https://doi.org/10.1002/advs.202411884 |
| work_keys_str_mv | AT wenxizhao optimizingreversiblephasetransformationoffes2anodeviaatomicinterfaceengineeringtowardfastchargingsodiumstoragetheoreticalpredicationandexperimentalvalidation AT yanbingzhou optimizingreversiblephasetransformationoffes2anodeviaatomicinterfaceengineeringtowardfastchargingsodiumstoragetheoreticalpredicationandexperimentalvalidation AT haozhou optimizingreversiblephasetransformationoffes2anodeviaatomicinterfaceengineeringtowardfastchargingsodiumstoragetheoreticalpredicationandexperimentalvalidation AT xinqinwang optimizingreversiblephasetransformationoffes2anodeviaatomicinterfaceengineeringtowardfastchargingsodiumstoragetheoreticalpredicationandexperimentalvalidation AT shengjunsun optimizingreversiblephasetransformationoffes2anodeviaatomicinterfaceengineeringtowardfastchargingsodiumstoragetheoreticalpredicationandexperimentalvalidation AT xunhe optimizingreversiblephasetransformationoffes2anodeviaatomicinterfaceengineeringtowardfastchargingsodiumstoragetheoreticalpredicationandexperimentalvalidation AT yongsongluo optimizingreversiblephasetransformationoffes2anodeviaatomicinterfaceengineeringtowardfastchargingsodiumstoragetheoreticalpredicationandexperimentalvalidation AT binwuying optimizingreversiblephasetransformationoffes2anodeviaatomicinterfaceengineeringtowardfastchargingsodiumstoragetheoreticalpredicationandexperimentalvalidation AT yongchaoyao optimizingreversiblephasetransformationoffes2anodeviaatomicinterfaceengineeringtowardfastchargingsodiumstoragetheoreticalpredicationandexperimentalvalidation AT xiaoqingma optimizingreversiblephasetransformationoffes2anodeviaatomicinterfaceengineeringtowardfastchargingsodiumstoragetheoreticalpredicationandexperimentalvalidation AT xupingsun optimizingreversiblephasetransformationoffes2anodeviaatomicinterfaceengineeringtowardfastchargingsodiumstoragetheoreticalpredicationandexperimentalvalidation |