Mitigating Polysulfide Shuttles with Upcycled Alkali Metal Terephthalate Decorated Separators
High energy density lithium–sulfur batteries (LSBs) are a potential replacement for lithium-ion batteries (LIBs). However, practical lifetimes are inhibited by lithium polysulfide (LiPS) shuttling. Concurrently, plastic waste accumulation worldwide threatens our ecosystems. Herein, a fast and facile...
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MDPI AG
2022-11-01
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| Online Access: | https://www.mdpi.com/2313-0105/8/12/253 |
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| author | Daniel A. Gribble Zih-Yu Lin Sourav Ghosh Brett M. Savoie Vilas G. Pol |
| author_facet | Daniel A. Gribble Zih-Yu Lin Sourav Ghosh Brett M. Savoie Vilas G. Pol |
| author_sort | Daniel A. Gribble |
| collection | DOAJ |
| description | High energy density lithium–sulfur batteries (LSBs) are a potential replacement for lithium-ion batteries (LIBs). However, practical lifetimes are inhibited by lithium polysulfide (LiPS) shuttling. Concurrently, plastic waste accumulation worldwide threatens our ecosystems. Herein, a fast and facile strategy to upcycle polyethylene terephthalate (PET) waste into useful materials is investigated. Dilithium terephthalate (Li<sub>2</sub>TP) and dipotassium terephthalate (K<sub>2</sub>TP) salts were synthesized from waste soda bottles via microwave depolymerization and solution coated onto glass fiber paper (GFP) separators. Salt-functionalized separators with Li<sub>2</sub>TP@GFP and K<sub>2</sub>TP@GFP mitigated LiPS shuttling and improved electrochemical performance in cells. Pore analysis and density functional theory (DFT) calculations indicate the action mechanism is synergistic physical blocking of bulky LiPS anions in nanopores and diffusion inhibition via electrostatic interactions with abundant carboxylate groups. LSBs with K<sub>2</sub>TP@GFP separator showing highest LiPS affinity and smallest pore size demonstrated enhanced initial capacity as compared to non-modified GFP by 5.4% to 648 mAh g<sup>−1</sup>, and increased cycle 100 capacity by 23% to 551 mAh g<sup>−1</sup>. Overall, K<sub>2</sub>TP@GFP retained 85% of initial capacity after 100 cycles with an average capacity fading of 0.15% per cycle. By comparison, GFP retained only 73% of initial capacity after 100 cycles with 0.27% average capacity loss, demonstrating effective LiPS retention. |
| first_indexed | 2024-03-09T17:19:49Z |
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| language | English |
| last_indexed | 2024-03-09T17:19:49Z |
| publishDate | 2022-11-01 |
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| series | Batteries |
| spelling | doaj.art-12f99c926e0f4723b3387657949e9ab32023-11-24T13:16:34ZengMDPI AGBatteries2313-01052022-11-0181225310.3390/batteries8120253Mitigating Polysulfide Shuttles with Upcycled Alkali Metal Terephthalate Decorated SeparatorsDaniel A. Gribble0Zih-Yu Lin1Sourav Ghosh2Brett M. Savoie3Vilas G. Pol4Davidson School of Chemical Engineering, Purdue University, West Lafayette, IN 47907, USADavidson School of Chemical Engineering, Purdue University, West Lafayette, IN 47907, USADavidson School of Chemical Engineering, Purdue University, West Lafayette, IN 47907, USADavidson School of Chemical Engineering, Purdue University, West Lafayette, IN 47907, USADavidson School of Chemical Engineering, Purdue University, West Lafayette, IN 47907, USAHigh energy density lithium–sulfur batteries (LSBs) are a potential replacement for lithium-ion batteries (LIBs). However, practical lifetimes are inhibited by lithium polysulfide (LiPS) shuttling. Concurrently, plastic waste accumulation worldwide threatens our ecosystems. Herein, a fast and facile strategy to upcycle polyethylene terephthalate (PET) waste into useful materials is investigated. Dilithium terephthalate (Li<sub>2</sub>TP) and dipotassium terephthalate (K<sub>2</sub>TP) salts were synthesized from waste soda bottles via microwave depolymerization and solution coated onto glass fiber paper (GFP) separators. Salt-functionalized separators with Li<sub>2</sub>TP@GFP and K<sub>2</sub>TP@GFP mitigated LiPS shuttling and improved electrochemical performance in cells. Pore analysis and density functional theory (DFT) calculations indicate the action mechanism is synergistic physical blocking of bulky LiPS anions in nanopores and diffusion inhibition via electrostatic interactions with abundant carboxylate groups. LSBs with K<sub>2</sub>TP@GFP separator showing highest LiPS affinity and smallest pore size demonstrated enhanced initial capacity as compared to non-modified GFP by 5.4% to 648 mAh g<sup>−1</sup>, and increased cycle 100 capacity by 23% to 551 mAh g<sup>−1</sup>. Overall, K<sub>2</sub>TP@GFP retained 85% of initial capacity after 100 cycles with an average capacity fading of 0.15% per cycle. By comparison, GFP retained only 73% of initial capacity after 100 cycles with 0.27% average capacity loss, demonstrating effective LiPS retention.https://www.mdpi.com/2313-0105/8/12/253waste PETdilithium terephthalatedipotassium terephthalatemicrowave synthesislithium sulfur batterymodified separator |
| spellingShingle | Daniel A. Gribble Zih-Yu Lin Sourav Ghosh Brett M. Savoie Vilas G. Pol Mitigating Polysulfide Shuttles with Upcycled Alkali Metal Terephthalate Decorated Separators Batteries waste PET dilithium terephthalate dipotassium terephthalate microwave synthesis lithium sulfur battery modified separator |
| title | Mitigating Polysulfide Shuttles with Upcycled Alkali Metal Terephthalate Decorated Separators |
| title_full | Mitigating Polysulfide Shuttles with Upcycled Alkali Metal Terephthalate Decorated Separators |
| title_fullStr | Mitigating Polysulfide Shuttles with Upcycled Alkali Metal Terephthalate Decorated Separators |
| title_full_unstemmed | Mitigating Polysulfide Shuttles with Upcycled Alkali Metal Terephthalate Decorated Separators |
| title_short | Mitigating Polysulfide Shuttles with Upcycled Alkali Metal Terephthalate Decorated Separators |
| title_sort | mitigating polysulfide shuttles with upcycled alkali metal terephthalate decorated separators |
| topic | waste PET dilithium terephthalate dipotassium terephthalate microwave synthesis lithium sulfur battery modified separator |
| url | https://www.mdpi.com/2313-0105/8/12/253 |
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