Screening Ammonium‐Based Cationic Additives to Regulate Interfacial Chemistry for Aqueous Ultra‐Stable Zn Metal Anode
Abstract The interfacial dynamics and chemistry at the electrolyte/metal interface, particularly the formation of an adsorption interphase, is paramount in dictating the reversibility of Zn metal deposition and dissolution processes in battery systems. Herein, a series of different cationic ammonium...
Saved in:
| Main Authors: | , , , , , , , , , , |
|---|---|
| Format: | Article |
| Language: | English |
| Published: |
Wiley
2024-11-01
|
| Series: | Advanced Science |
| Subjects: | |
| Online Access: | https://doi.org/10.1002/advs.202407102 |
| Tags: |
Add Tag
No Tags, Be the first to tag this record!
|
| _version_ | 1846161995009622016 |
|---|---|
| author | Leilei Zheng Huihua Li Mingbo Gao Keer Huang Jian Wang Long Su Lei Li Hongzhen Lin Xinpei Gao Zhengqing Liu Huang Zhang |
| author_facet | Leilei Zheng Huihua Li Mingbo Gao Keer Huang Jian Wang Long Su Lei Li Hongzhen Lin Xinpei Gao Zhengqing Liu Huang Zhang |
| author_sort | Leilei Zheng |
| collection | DOAJ |
| description | Abstract The interfacial dynamics and chemistry at the electrolyte/metal interface, particularly the formation of an adsorption interphase, is paramount in dictating the reversibility of Zn metal deposition and dissolution processes in battery systems. Herein, a series of different cationic ammonium‐based electrolyte additives are screened that effectively modulate the interfacial chemistry of zinc anodes in aqueous electrolytes, significantly improving the reversibility of Zn metal plating/stripping processes. As initially comprehensive investigation by combining theoretical calculation and molecular dynamic simulation, the tetramethylammonium cation, with its specific molecular structure and charge distribution, is identified as pivotal in mediating the Zn(H2O)62+ solvation shell structure at the electrode/electrolyte interface and shows the strong resistance against electrolyte corrosion as revealed by X‐ray and optical measurements. As a result, the Zn||Zn symmetric cell with optimal electrolyte lasts for over 4400 h of stable plating/stripping behaviors, and the Zn||Cu asymmetric cell stabilizes for 2100 cycles with an average Coulombic efficiency of 99.8%, which is much better than the‐state‐of‐art progress. Consequently, full‐cells coupled with various cathodes showcase improved electrochemical performance, displaying high capacity‐retention and low self‐discharge behaviors. These findings offer essential insights of cationic additives in ameliorating zinc anode performance. |
| format | Article |
| id | doaj-art-c88f9a1cf8b94bb38d4c5b67e33f84be |
| institution | Kabale University |
| issn | 2198-3844 |
| language | English |
| publishDate | 2024-11-01 |
| publisher | Wiley |
| record_format | Article |
| series | Advanced Science |
| spelling | doaj-art-c88f9a1cf8b94bb38d4c5b67e33f84be2024-11-20T19:25:40ZengWileyAdvanced Science2198-38442024-11-011143n/an/a10.1002/advs.202407102Screening Ammonium‐Based Cationic Additives to Regulate Interfacial Chemistry for Aqueous Ultra‐Stable Zn Metal AnodeLeilei Zheng0Huihua Li1Mingbo Gao2Keer Huang3Jian Wang4Long Su5Lei Li6Hongzhen Lin7Xinpei Gao8Zhengqing Liu9Huang Zhang10Key Laboratory of Engineering Dielectric and Applications (Ministry of Education), School of Electrical and Electronic Engineering Harbin University of Science and Technology Harbin 150080 P. R. ChinaKey Laboratory of Engineering Dielectric and Applications (Ministry of Education), School of Electrical and Electronic Engineering Harbin University of Science and Technology Harbin 150080 P. R. ChinaKey Laboratory of Engineering Dielectric and Applications (Ministry of Education), School of Electrical and Electronic Engineering Harbin University of Science and Technology Harbin 150080 P. R. ChinaInstitute of Flexible Electronics Northwestern Polytechnical University Xi'an 710072 P. R. Chinai‐lab & CAS Key Laboratory of Nanophotonic Materials and Devices, Suzhou Institute of Nano‐Tech and Nano‐Bionics Chinese Academy of Sciences Suzhou 215123 P. R. ChinaKey Laboratory of Colloid and Interface Chemistry (Ministry of Education) Shandong University Jinan 250100 P. R. ChinaInstitute of Flexible Electronics Northwestern Polytechnical University Xi'an 710072 P. R. Chinai‐lab & CAS Key Laboratory of Nanophotonic Materials and Devices, Suzhou Institute of Nano‐Tech and Nano‐Bionics Chinese Academy of Sciences Suzhou 215123 P. R. ChinaKey Laboratory of Advanced Materials in Tropical Island Resources (Ministry of Education), School of Chemistry and Chemical Engineering Hainan University Haikou 570228 P. R. ChinaInstitute of Flexible Electronics Northwestern Polytechnical University Xi'an 710072 P. R. ChinaKey Laboratory of Engineering Dielectric and Applications (Ministry of Education), School of Electrical and Electronic Engineering Harbin University of Science and Technology Harbin 150080 P. R. ChinaAbstract The interfacial dynamics and chemistry at the electrolyte/metal interface, particularly the formation of an adsorption interphase, is paramount in dictating the reversibility of Zn metal deposition and dissolution processes in battery systems. Herein, a series of different cationic ammonium‐based electrolyte additives are screened that effectively modulate the interfacial chemistry of zinc anodes in aqueous electrolytes, significantly improving the reversibility of Zn metal plating/stripping processes. As initially comprehensive investigation by combining theoretical calculation and molecular dynamic simulation, the tetramethylammonium cation, with its specific molecular structure and charge distribution, is identified as pivotal in mediating the Zn(H2O)62+ solvation shell structure at the electrode/electrolyte interface and shows the strong resistance against electrolyte corrosion as revealed by X‐ray and optical measurements. As a result, the Zn||Zn symmetric cell with optimal electrolyte lasts for over 4400 h of stable plating/stripping behaviors, and the Zn||Cu asymmetric cell stabilizes for 2100 cycles with an average Coulombic efficiency of 99.8%, which is much better than the‐state‐of‐art progress. Consequently, full‐cells coupled with various cathodes showcase improved electrochemical performance, displaying high capacity‐retention and low self‐discharge behaviors. These findings offer essential insights of cationic additives in ameliorating zinc anode performance.https://doi.org/10.1002/advs.202407102cationic electrolyte additivesinterfacial chemistrysolvation shell structuretheoretical simulationzinc metal anodes |
| spellingShingle | Leilei Zheng Huihua Li Mingbo Gao Keer Huang Jian Wang Long Su Lei Li Hongzhen Lin Xinpei Gao Zhengqing Liu Huang Zhang Screening Ammonium‐Based Cationic Additives to Regulate Interfacial Chemistry for Aqueous Ultra‐Stable Zn Metal Anode Advanced Science cationic electrolyte additives interfacial chemistry solvation shell structure theoretical simulation zinc metal anodes |
| title | Screening Ammonium‐Based Cationic Additives to Regulate Interfacial Chemistry for Aqueous Ultra‐Stable Zn Metal Anode |
| title_full | Screening Ammonium‐Based Cationic Additives to Regulate Interfacial Chemistry for Aqueous Ultra‐Stable Zn Metal Anode |
| title_fullStr | Screening Ammonium‐Based Cationic Additives to Regulate Interfacial Chemistry for Aqueous Ultra‐Stable Zn Metal Anode |
| title_full_unstemmed | Screening Ammonium‐Based Cationic Additives to Regulate Interfacial Chemistry for Aqueous Ultra‐Stable Zn Metal Anode |
| title_short | Screening Ammonium‐Based Cationic Additives to Regulate Interfacial Chemistry for Aqueous Ultra‐Stable Zn Metal Anode |
| title_sort | screening ammonium based cationic additives to regulate interfacial chemistry for aqueous ultra stable zn metal anode |
| topic | cationic electrolyte additives interfacial chemistry solvation shell structure theoretical simulation zinc metal anodes |
| url | https://doi.org/10.1002/advs.202407102 |
| work_keys_str_mv | AT leileizheng screeningammoniumbasedcationicadditivestoregulateinterfacialchemistryforaqueousultrastableznmetalanode AT huihuali screeningammoniumbasedcationicadditivestoregulateinterfacialchemistryforaqueousultrastableznmetalanode AT mingbogao screeningammoniumbasedcationicadditivestoregulateinterfacialchemistryforaqueousultrastableznmetalanode AT keerhuang screeningammoniumbasedcationicadditivestoregulateinterfacialchemistryforaqueousultrastableznmetalanode AT jianwang screeningammoniumbasedcationicadditivestoregulateinterfacialchemistryforaqueousultrastableznmetalanode AT longsu screeningammoniumbasedcationicadditivestoregulateinterfacialchemistryforaqueousultrastableznmetalanode AT leili screeningammoniumbasedcationicadditivestoregulateinterfacialchemistryforaqueousultrastableznmetalanode AT hongzhenlin screeningammoniumbasedcationicadditivestoregulateinterfacialchemistryforaqueousultrastableznmetalanode AT xinpeigao screeningammoniumbasedcationicadditivestoregulateinterfacialchemistryforaqueousultrastableznmetalanode AT zhengqingliu screeningammoniumbasedcationicadditivestoregulateinterfacialchemistryforaqueousultrastableznmetalanode AT huangzhang screeningammoniumbasedcationicadditivestoregulateinterfacialchemistryforaqueousultrastableznmetalanode |