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Electrochemical Reoxidation Enables Continuous Methane-to-Methanol Catalysis with Aqueous Pt Salts
[Image: see text] The direct conversion of methane to methanol would enable better utilization of abundant natural gas resources. In the presence of stoichiometric Pt(IV) oxidants, Pt(II) ions are capable of catalyzing this reaction in aqueous solutions at modest temperatures. Practical implementati...
Autores principales: | , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
American Chemical Society
2019
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Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6661865/ https://www.ncbi.nlm.nih.gov/pubmed/31403070 http://dx.doi.org/10.1021/acscentsci.9b00273 |
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author | Kim, R. Soyoung Surendranath, Yogesh |
author_facet | Kim, R. Soyoung Surendranath, Yogesh |
author_sort | Kim, R. Soyoung |
collection | PubMed |
description | [Image: see text] The direct conversion of methane to methanol would enable better utilization of abundant natural gas resources. In the presence of stoichiometric Pt(IV) oxidants, Pt(II) ions are capable of catalyzing this reaction in aqueous solutions at modest temperatures. Practical implementation of this chemistry requires a viable strategy for replacing or regenerating the expensive Pt(IV) oxidant. Herein, we establish an electrochemical strategy for continuous regeneration of the Pt(IV) oxidant to furnish overall electrochemical methane oxidation. We show that Cl-adsorbed Pt electrodes catalyze facile oxidation of Pt(II) to Pt(IV) at low overpotential without concomitant methanol oxidation. Exploiting this facile electrochemistry, we maintain the Pt(II/IV) ratio during Pt(II)-catalyzed methane oxidation via in situ monitoring of the solution potential coupled with dynamic modulation of the electric current. This approach leads to sustained methane oxidation catalysis with 70% selectivity for methanol. |
format | Online Article Text |
id | pubmed-6661865 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2019 |
publisher | American Chemical Society |
record_format | MEDLINE/PubMed |
spelling | pubmed-66618652019-08-09 Electrochemical Reoxidation Enables Continuous Methane-to-Methanol Catalysis with Aqueous Pt Salts Kim, R. Soyoung Surendranath, Yogesh ACS Cent Sci [Image: see text] The direct conversion of methane to methanol would enable better utilization of abundant natural gas resources. In the presence of stoichiometric Pt(IV) oxidants, Pt(II) ions are capable of catalyzing this reaction in aqueous solutions at modest temperatures. Practical implementation of this chemistry requires a viable strategy for replacing or regenerating the expensive Pt(IV) oxidant. Herein, we establish an electrochemical strategy for continuous regeneration of the Pt(IV) oxidant to furnish overall electrochemical methane oxidation. We show that Cl-adsorbed Pt electrodes catalyze facile oxidation of Pt(II) to Pt(IV) at low overpotential without concomitant methanol oxidation. Exploiting this facile electrochemistry, we maintain the Pt(II/IV) ratio during Pt(II)-catalyzed methane oxidation via in situ monitoring of the solution potential coupled with dynamic modulation of the electric current. This approach leads to sustained methane oxidation catalysis with 70% selectivity for methanol. American Chemical Society 2019-06-17 2019-07-24 /pmc/articles/PMC6661865/ /pubmed/31403070 http://dx.doi.org/10.1021/acscentsci.9b00273 Text en Copyright © 2019 American Chemical Society This is an open access article published under an ACS AuthorChoice License (http://pubs.acs.org/page/policy/authorchoice_termsofuse.html) , which permits copying and redistribution of the article or any adaptations for non-commercial purposes. |
spellingShingle | Kim, R. Soyoung Surendranath, Yogesh Electrochemical Reoxidation Enables Continuous Methane-to-Methanol Catalysis with Aqueous Pt Salts |
title | Electrochemical Reoxidation Enables Continuous Methane-to-Methanol
Catalysis with Aqueous Pt Salts |
title_full | Electrochemical Reoxidation Enables Continuous Methane-to-Methanol
Catalysis with Aqueous Pt Salts |
title_fullStr | Electrochemical Reoxidation Enables Continuous Methane-to-Methanol
Catalysis with Aqueous Pt Salts |
title_full_unstemmed | Electrochemical Reoxidation Enables Continuous Methane-to-Methanol
Catalysis with Aqueous Pt Salts |
title_short | Electrochemical Reoxidation Enables Continuous Methane-to-Methanol
Catalysis with Aqueous Pt Salts |
title_sort | electrochemical reoxidation enables continuous methane-to-methanol
catalysis with aqueous pt salts |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC6661865/ https://www.ncbi.nlm.nih.gov/pubmed/31403070 http://dx.doi.org/10.1021/acscentsci.9b00273 |
work_keys_str_mv | AT kimrsoyoung electrochemicalreoxidationenablescontinuousmethanetomethanolcatalysiswithaqueousptsalts AT surendranathyogesh electrochemicalreoxidationenablescontinuousmethanetomethanolcatalysiswithaqueousptsalts |