Hydrogenolysis of Polyethylene and Polypropylene into Propane over Cobalt-Based Catalysts
The development of technologies to recycle polyethylene (PE) and polypropylene (PP), globally the two most produced polymers, is critical to increase plastic circularity. Here, we show that 5 wt % cobalt supported on ZSM-5 zeolite catalyzes the solvent-free hydrogenolysis of PE and PP into propane w...
| Main Authors: | , , , , , , , , |
|---|---|
| 其他作者: | |
| 格式: | 文件 |
| 语言: | English |
| 出版: |
American Chemical Society (ACS)
2023
|
| 在线阅读: | https://hdl.handle.net/1721.1/146958 |
| _version_ | 1826213747617693696 |
|---|---|
| author | Zichittella, Guido Ebrahim, Amani M Zhu, Jie Brenner, Anna E Drake, Griffin Beckham, Gregg T Bare, Simon R Rorrer, Julie E Román-Leshkov, Yuriy |
| author2 | Massachusetts Institute of Technology. Department of Chemical Engineering |
| author_facet | Massachusetts Institute of Technology. Department of Chemical Engineering Zichittella, Guido Ebrahim, Amani M Zhu, Jie Brenner, Anna E Drake, Griffin Beckham, Gregg T Bare, Simon R Rorrer, Julie E Román-Leshkov, Yuriy |
| author_sort | Zichittella, Guido |
| collection | MIT |
| description | The development of technologies to recycle polyethylene (PE) and polypropylene (PP), globally the two most produced polymers, is critical to increase plastic circularity. Here, we show that 5 wt % cobalt supported on ZSM-5 zeolite catalyzes the solvent-free hydrogenolysis of PE and PP into propane with weight-based selectivity in the gas phase over 80 wt % after 20 h at 523 K and 40 bar H2. This catalyst significantly reduces the formation of undesired CH4 (≤5 wt %), a product which is favored when using bulk cobalt oxide or cobalt nanoparticles supported on other carriers (selectivity ≤95 wt %). The superior performance of Co/ZSM-5 is attributed to the stabilization of dispersed oxidic cobalt nanoparticles by the zeolite support, preventing further reduction to metallic species that appear to catalyze CH4 generation. While ZSM-5 is also active for propane formation at 523 K, the presence of Co promotes stability and selectivity. After optimizing the metal loading, it was demonstrated that 10 wt % Co/ZSM-5 can selectively catalyze the hydrogenolysis of low-density PE (LDPE), mixtures of LDPE and PP, as well as postconsumer PE, showcasing the effectiveness of this technology to upcycle realistic plastic waste. Cobalt supported on zeolites FAU, MOR, and BEA were also effective catalysts for C2-C4 hydrocarbon formation and revealed that the framework topology provides a handle to tune gas-phase selectivity. |
| first_indexed | 2024-09-23T15:54:11Z |
| format | Article |
| id | mit-1721.1/146958 |
| institution | Massachusetts Institute of Technology |
| language | English |
| last_indexed | 2024-09-23T15:54:11Z |
| publishDate | 2023 |
| publisher | American Chemical Society (ACS) |
| record_format | dspace |
| spelling | mit-1721.1/1469582023-01-05T03:04:31Z Hydrogenolysis of Polyethylene and Polypropylene into Propane over Cobalt-Based Catalysts Zichittella, Guido Ebrahim, Amani M Zhu, Jie Brenner, Anna E Drake, Griffin Beckham, Gregg T Bare, Simon R Rorrer, Julie E Román-Leshkov, Yuriy Massachusetts Institute of Technology. Department of Chemical Engineering The development of technologies to recycle polyethylene (PE) and polypropylene (PP), globally the two most produced polymers, is critical to increase plastic circularity. Here, we show that 5 wt % cobalt supported on ZSM-5 zeolite catalyzes the solvent-free hydrogenolysis of PE and PP into propane with weight-based selectivity in the gas phase over 80 wt % after 20 h at 523 K and 40 bar H2. This catalyst significantly reduces the formation of undesired CH4 (≤5 wt %), a product which is favored when using bulk cobalt oxide or cobalt nanoparticles supported on other carriers (selectivity ≤95 wt %). The superior performance of Co/ZSM-5 is attributed to the stabilization of dispersed oxidic cobalt nanoparticles by the zeolite support, preventing further reduction to metallic species that appear to catalyze CH4 generation. While ZSM-5 is also active for propane formation at 523 K, the presence of Co promotes stability and selectivity. After optimizing the metal loading, it was demonstrated that 10 wt % Co/ZSM-5 can selectively catalyze the hydrogenolysis of low-density PE (LDPE), mixtures of LDPE and PP, as well as postconsumer PE, showcasing the effectiveness of this technology to upcycle realistic plastic waste. Cobalt supported on zeolites FAU, MOR, and BEA were also effective catalysts for C2-C4 hydrocarbon formation and revealed that the framework topology provides a handle to tune gas-phase selectivity. 2023-01-04T13:57:47Z 2023-01-04T13:57:47Z 2022-10-24 2023-01-04T13:51:08Z Article http://purl.org/eprint/type/JournalArticle https://hdl.handle.net/1721.1/146958 Zichittella, Guido, Ebrahim, Amani M, Zhu, Jie, Brenner, Anna E, Drake, Griffin et al. 2022. "Hydrogenolysis of Polyethylene and Polypropylene into Propane over Cobalt-Based Catalysts." JACS Au, 2 (10). en 10.1021/jacsau.2c00402 JACS Au Creative Commons Attribution 4.0 International license https://creativecommons.org/licenses/by/4.0/ application/pdf American Chemical Society (ACS) ACS |
| spellingShingle | Zichittella, Guido Ebrahim, Amani M Zhu, Jie Brenner, Anna E Drake, Griffin Beckham, Gregg T Bare, Simon R Rorrer, Julie E Román-Leshkov, Yuriy Hydrogenolysis of Polyethylene and Polypropylene into Propane over Cobalt-Based Catalysts |
| title | Hydrogenolysis of Polyethylene and Polypropylene into Propane over Cobalt-Based Catalysts |
| title_full | Hydrogenolysis of Polyethylene and Polypropylene into Propane over Cobalt-Based Catalysts |
| title_fullStr | Hydrogenolysis of Polyethylene and Polypropylene into Propane over Cobalt-Based Catalysts |
| title_full_unstemmed | Hydrogenolysis of Polyethylene and Polypropylene into Propane over Cobalt-Based Catalysts |
| title_short | Hydrogenolysis of Polyethylene and Polypropylene into Propane over Cobalt-Based Catalysts |
| title_sort | hydrogenolysis of polyethylene and polypropylene into propane over cobalt based catalysts |
| url | https://hdl.handle.net/1721.1/146958 |
| work_keys_str_mv | AT zichittellaguido hydrogenolysisofpolyethyleneandpolypropyleneintopropaneovercobaltbasedcatalysts AT ebrahimamanim hydrogenolysisofpolyethyleneandpolypropyleneintopropaneovercobaltbasedcatalysts AT zhujie hydrogenolysisofpolyethyleneandpolypropyleneintopropaneovercobaltbasedcatalysts AT brennerannae hydrogenolysisofpolyethyleneandpolypropyleneintopropaneovercobaltbasedcatalysts AT drakegriffin hydrogenolysisofpolyethyleneandpolypropyleneintopropaneovercobaltbasedcatalysts AT beckhamgreggt hydrogenolysisofpolyethyleneandpolypropyleneintopropaneovercobaltbasedcatalysts AT baresimonr hydrogenolysisofpolyethyleneandpolypropyleneintopropaneovercobaltbasedcatalysts AT rorrerjuliee hydrogenolysisofpolyethyleneandpolypropyleneintopropaneovercobaltbasedcatalysts AT romanleshkovyuriy hydrogenolysisofpolyethyleneandpolypropyleneintopropaneovercobaltbasedcatalysts |