دورية أكاديمية
Method of H 2 Transfer Is Vital for Catalytic Hydrodefluorination of Perfluorooctanoic Acid (PFOA)
| العنوان: | Method of H 2 Transfer Is Vital for Catalytic Hydrodefluorination of Perfluorooctanoic Acid (PFOA) |
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| المؤلفون: | Min Long, Yu Chen, Thomas P. Senftle, Welman Elias, Kimberly Heck, Chen Zhou, Michael S. Wong, Bruce E. Rittmann |
| سنة النشر: | 1753 |
| مصطلحات موضوعية: | Biophysics, Biochemistry, Medicine, Cell Biology, Space Science, Biological Sciences not elsewhere classified, situ autocatalytic reduction, reactive hydrogen species, provides mechanistic insights, directly deposited onto, also significantly increased, full reductive defluorination, 2 +, 0 , elemental palladium nanoparticles, 2 , np catalyst compared, catalytic hydrodefluorination ability, defluorination rate, catalyst film, catalytic hydrogenation, catalytic hydrodefluorination, study documents, recalcitrant contaminants, persistent contaminants, perfluorooctanoic acid, lumen pressure, higher coverage, crucial role, critical role |
| الوصف: | The efficient transfer of H 2 plays a critical role in catalytic hydrogenation, particularly for the removal of recalcitrant contaminants from water. One of the most persistent contaminants, perfluorooctanoic acid (PFOA), was used to investigate how the method of H 2 transfer affected the catalytic hydrodefluorination ability of elemental palladium nanoparticles (Pd 0 NPs). Pd 0 NPs were synthesized through an in situ autocatalytic reduction of Pd 2+ driven by H 2 from the membrane. The Pd 0 nanoparticles were directly deposited onto the membrane fibers to form the catalyst film. Direct delivery of H 2 to Pd 0 NPs through the walls of nonporous gas transfer membranes enhanced the hydrodefluorination of PFOA, compared to delivering H 2 through the headspace. A higher H 2 lumen pressure (20 vs 5 psig) also significantly increased the defluorination rate, although 5 psig H 2 flux was sufficient for full reductive defluorination of PFOA. Calculations made using density functional theory (DFT) suggest that subsurface hydrogen delivered directly from the membrane increases and accelerates hydrodefluorination by creating a higher coverage of reactive hydrogen species on the Pd 0 NP catalyst compared to H 2 delivery through the headspace. This study documents the crucial role of the H 2 transfer method in the catalytic hydrogenation of PFOA and provides mechanistic insights into how membrane delivery accelerates hydrodefluorination. |
| نوع الوثيقة: | article in journal/newspaper |
| اللغة: | unknown |
| العلاقة: | https://figshare.com/articles/journal_contribution/Method_of_H_sub_2_sub_Transfer_Is_Vital_for_Catalytic_Hydrodefluorination_of_Perfluorooctanoic_Acid_PFOA_/24926721Test |
| DOI: | 10.1021/acs.est.3c07650.s001 |
| الإتاحة: | https://doi.org/10.1021/acs.est.3c07650.s001Test https://figshare.com/articles/journal_contribution/Method_of_H_sub_2_sub_Transfer_Is_Vital_for_Catalytic_Hydrodefluorination_of_Perfluorooctanoic_Acid_PFOA_/24926721Test |
| حقوق: | CC BY-NC 4.0 |
| رقم الانضمام: | edsbas.44509C11 |
| قاعدة البيانات: | BASE |
| DOI: | 10.1021/acs.est.3c07650.s001 |
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