Evaluation of the Removal of PVDF Using ToF-SIMS: Comparing Dihydrolevoglucosenone and Pyrolysis as Pretreatments for Cathode Materials of Lithium-Ion Batteries
Effective and environmentally benign removal of polyvinylidene fluoride (PVDF) binders from spent battery electrodes remains a critical hurdle in sustainable recycling, primarily due to issues related to the mitigation of fluorinated compound emissions. This work evaluates PVDF binder removal from c...
| Main Authors: | , , , , , , , , , |
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| Format: | Journal Article |
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MDPI
2025
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| Online Access: | http://purl.org/au-research/grants/arc/LE190100053 http://hdl.handle.net/20.500.11937/97421 |
| _version_ | 1848766261762195456 |
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| author | Henderson, Marc Simon Salces, Aliza Marie Rickard, William DA Fougerouse, Denis Medina, Álvaro José Rodríguez Oraby, Elsayed A Beh, Jane Rudolph, Martin Vanderbruggen, Anna Eksteen, Jacques |
| author_facet | Henderson, Marc Simon Salces, Aliza Marie Rickard, William DA Fougerouse, Denis Medina, Álvaro José Rodríguez Oraby, Elsayed A Beh, Jane Rudolph, Martin Vanderbruggen, Anna Eksteen, Jacques |
| author_sort | Henderson, Marc Simon |
| building | Curtin Institutional Repository |
| collection | Online Access |
| description | Effective and environmentally benign removal of polyvinylidene fluoride (PVDF) binders from spent battery electrodes remains a critical hurdle in sustainable recycling, primarily due to issues related to the mitigation of fluorinated compound emissions. This work evaluates PVDF binder removal from cathode active material using either a green solvent-based dissolution process or pyrolysis, analyzed by time-of-flight secondary ion mass spectrometry (ToF-SIMS). The solvent pretreatment involved mixing dihydrolevoglucosenone (Cyrene™) with PVDF-coated NMC811 at 100 °C, followed by hot filtration to separate the Cyrene-PVDF solution. Pyrolysis was conducted at 800 °C under an argon atmosphere. Positive ToF-SIMS spectra for Cyrene showed characteristic peaks at ketene (42 m/z) and 1,3-dioxole (86 m/z), along with intense C2H3O+, C3H3O+, C4H7+, and C3H5O+ peaks. The characteristic peaks used to identify PVDF were C3H2F5+ (133 m/z), C3H2F3+ (95 m/z), and C3HF4+ (113 m/z). Both processes resulted in PVDF removal, with pyrolysis demonstrating higher effectiveness. Particle agglomeration was observed in both pretreated NMC811 samples, however agglomeration was more pronounced with Cyrene pretreatment due to PVDF redeposition. Following pyrolysis, PVDF was transformed into a defluorinated carbonaceous material. |
| first_indexed | 2025-11-14T11:48:20Z |
| format | Journal Article |
| id | curtin-20.500.11937-97421 |
| institution | Curtin University Malaysia |
| institution_category | Local University |
| last_indexed | 2025-11-14T11:48:20Z |
| publishDate | 2025 |
| publisher | MDPI |
| recordtype | eprints |
| repository_type | Digital Repository |
| spelling | curtin-20.500.11937-974212025-05-23T05:17:11Z Evaluation of the Removal of PVDF Using ToF-SIMS: Comparing Dihydrolevoglucosenone and Pyrolysis as Pretreatments for Cathode Materials of Lithium-Ion Batteries Henderson, Marc Simon Salces, Aliza Marie Rickard, William DA Fougerouse, Denis Medina, Álvaro José Rodríguez Oraby, Elsayed A Beh, Jane Rudolph, Martin Vanderbruggen, Anna Eksteen, Jacques Effective and environmentally benign removal of polyvinylidene fluoride (PVDF) binders from spent battery electrodes remains a critical hurdle in sustainable recycling, primarily due to issues related to the mitigation of fluorinated compound emissions. This work evaluates PVDF binder removal from cathode active material using either a green solvent-based dissolution process or pyrolysis, analyzed by time-of-flight secondary ion mass spectrometry (ToF-SIMS). The solvent pretreatment involved mixing dihydrolevoglucosenone (Cyrene™) with PVDF-coated NMC811 at 100 °C, followed by hot filtration to separate the Cyrene-PVDF solution. Pyrolysis was conducted at 800 °C under an argon atmosphere. Positive ToF-SIMS spectra for Cyrene showed characteristic peaks at ketene (42 m/z) and 1,3-dioxole (86 m/z), along with intense C2H3O+, C3H3O+, C4H7+, and C3H5O+ peaks. The characteristic peaks used to identify PVDF were C3H2F5+ (133 m/z), C3H2F3+ (95 m/z), and C3HF4+ (113 m/z). Both processes resulted in PVDF removal, with pyrolysis demonstrating higher effectiveness. Particle agglomeration was observed in both pretreated NMC811 samples, however agglomeration was more pronounced with Cyrene pretreatment due to PVDF redeposition. Following pyrolysis, PVDF was transformed into a defluorinated carbonaceous material. 2025 Journal Article http://hdl.handle.net/20.500.11937/97421 10.3390/recycling10020056 http://purl.org/au-research/grants/arc/LE190100053 MDPI fulltext |
| spellingShingle | Henderson, Marc Simon Salces, Aliza Marie Rickard, William DA Fougerouse, Denis Medina, Álvaro José Rodríguez Oraby, Elsayed A Beh, Jane Rudolph, Martin Vanderbruggen, Anna Eksteen, Jacques Evaluation of the Removal of PVDF Using ToF-SIMS: Comparing Dihydrolevoglucosenone and Pyrolysis as Pretreatments for Cathode Materials of Lithium-Ion Batteries |
| title | Evaluation of the Removal of PVDF Using ToF-SIMS: Comparing Dihydrolevoglucosenone and Pyrolysis as Pretreatments for Cathode Materials of Lithium-Ion Batteries |
| title_full | Evaluation of the Removal of PVDF Using ToF-SIMS: Comparing Dihydrolevoglucosenone and Pyrolysis as Pretreatments for Cathode Materials of Lithium-Ion Batteries |
| title_fullStr | Evaluation of the Removal of PVDF Using ToF-SIMS: Comparing Dihydrolevoglucosenone and Pyrolysis as Pretreatments for Cathode Materials of Lithium-Ion Batteries |
| title_full_unstemmed | Evaluation of the Removal of PVDF Using ToF-SIMS: Comparing Dihydrolevoglucosenone and Pyrolysis as Pretreatments for Cathode Materials of Lithium-Ion Batteries |
| title_short | Evaluation of the Removal of PVDF Using ToF-SIMS: Comparing Dihydrolevoglucosenone and Pyrolysis as Pretreatments for Cathode Materials of Lithium-Ion Batteries |
| title_sort | evaluation of the removal of pvdf using tof-sims: comparing dihydrolevoglucosenone and pyrolysis as pretreatments for cathode materials of lithium-ion batteries |
| url | http://purl.org/au-research/grants/arc/LE190100053 http://hdl.handle.net/20.500.11937/97421 |