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Direct Catalytic Oxidation of Low-Concentration Methane to Methanol in One Step on Ni-Promoted BiOCl Catalysts

[Image: see text] The direct oxidation of low-concentration methane (CH(4)) to methanol (CH(3)OH) is often regarded as the “holy grail”. However, it still is very difficult and challenging to oxidize methane to methanol in one step. In this work, we present a new approach to directly oxidize CH(4) t...

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Autores principales: Zhu, Chen, Guo, Ge, Li, Wenzhi, Wu, Mingwei, Jiang, Yihang, Wu, Wenjian, Zhang, Hao
Formato: Online Artículo Texto
Lenguaje:English
Publicado: American Chemical Society 2023
Acceso en línea:https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10061602/
https://www.ncbi.nlm.nih.gov/pubmed/37008125
http://dx.doi.org/10.1021/acsomega.2c08039
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author Zhu, Chen
Guo, Ge
Li, Wenzhi
Wu, Mingwei
Jiang, Yihang
Wu, Wenjian
Zhang, Hao
author_facet Zhu, Chen
Guo, Ge
Li, Wenzhi
Wu, Mingwei
Jiang, Yihang
Wu, Wenjian
Zhang, Hao
author_sort Zhu, Chen
collection PubMed
description [Image: see text] The direct oxidation of low-concentration methane (CH(4)) to methanol (CH(3)OH) is often regarded as the “holy grail”. However, it still is very difficult and challenging to oxidize methane to methanol in one step. In this work, we present a new approach to directly oxidize CH(4) to generate CH(3)OH in one step by doping non-noble metal Ni sites on bismuth oxychloride (BiOCl) equipped with high oxygen vacancies. Thereinto, the conversion rate of CH(3)OH can reach 39.07 μmol/(g(cat)·h) under 420 °C and flow conditions on the basis of O(2) and H(2)O. The crystal morphology structure, physicochemical properties, metal dispersion, and surface adsorption capacity of Ni–BiOCl were explored, and the positive effect on the oxygen vacancy of the catalyst was proved, thus improving the catalytic performance. Furthermore, in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) was also performed to study the surface adsorption and reaction process of methane to methanol in one step. Results demonstrate that the key to keep good activity lies in the oxygen vacancies of unsaturated Bi atoms, which can adsorb and active CH(4) and to produce methyl groups and adsorbing hydroxyl groups in methane oxidation process. This study broadens the application of oxygen-deficient catalysts in the catalytic conversion of CH(4) to CH(3)OH in one step, which provides a new perspective on the role of oxygen vacancies in improving the catalytic performance of methane oxidation.
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spelling pubmed-100616022023-03-31 Direct Catalytic Oxidation of Low-Concentration Methane to Methanol in One Step on Ni-Promoted BiOCl Catalysts Zhu, Chen Guo, Ge Li, Wenzhi Wu, Mingwei Jiang, Yihang Wu, Wenjian Zhang, Hao ACS Omega [Image: see text] The direct oxidation of low-concentration methane (CH(4)) to methanol (CH(3)OH) is often regarded as the “holy grail”. However, it still is very difficult and challenging to oxidize methane to methanol in one step. In this work, we present a new approach to directly oxidize CH(4) to generate CH(3)OH in one step by doping non-noble metal Ni sites on bismuth oxychloride (BiOCl) equipped with high oxygen vacancies. Thereinto, the conversion rate of CH(3)OH can reach 39.07 μmol/(g(cat)·h) under 420 °C and flow conditions on the basis of O(2) and H(2)O. The crystal morphology structure, physicochemical properties, metal dispersion, and surface adsorption capacity of Ni–BiOCl were explored, and the positive effect on the oxygen vacancy of the catalyst was proved, thus improving the catalytic performance. Furthermore, in situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) was also performed to study the surface adsorption and reaction process of methane to methanol in one step. Results demonstrate that the key to keep good activity lies in the oxygen vacancies of unsaturated Bi atoms, which can adsorb and active CH(4) and to produce methyl groups and adsorbing hydroxyl groups in methane oxidation process. This study broadens the application of oxygen-deficient catalysts in the catalytic conversion of CH(4) to CH(3)OH in one step, which provides a new perspective on the role of oxygen vacancies in improving the catalytic performance of methane oxidation. American Chemical Society 2023-03-16 /pmc/articles/PMC10061602/ /pubmed/37008125 http://dx.doi.org/10.1021/acsomega.2c08039 Text en © 2023 The Authors. Published by American Chemical Society https://creativecommons.org/licenses/by-nc-nd/4.0/Permits non-commercial access and re-use, provided that author attribution and integrity are maintained; but does not permit creation of adaptations or other derivative works (https://creativecommons.org/licenses/by-nc-nd/4.0/).
spellingShingle Zhu, Chen
Guo, Ge
Li, Wenzhi
Wu, Mingwei
Jiang, Yihang
Wu, Wenjian
Zhang, Hao
Direct Catalytic Oxidation of Low-Concentration Methane to Methanol in One Step on Ni-Promoted BiOCl Catalysts
title Direct Catalytic Oxidation of Low-Concentration Methane to Methanol in One Step on Ni-Promoted BiOCl Catalysts
title_full Direct Catalytic Oxidation of Low-Concentration Methane to Methanol in One Step on Ni-Promoted BiOCl Catalysts
title_fullStr Direct Catalytic Oxidation of Low-Concentration Methane to Methanol in One Step on Ni-Promoted BiOCl Catalysts
title_full_unstemmed Direct Catalytic Oxidation of Low-Concentration Methane to Methanol in One Step on Ni-Promoted BiOCl Catalysts
title_short Direct Catalytic Oxidation of Low-Concentration Methane to Methanol in One Step on Ni-Promoted BiOCl Catalysts
title_sort direct catalytic oxidation of low-concentration methane to methanol in one step on ni-promoted biocl catalysts
url https://www.ncbi.nlm.nih.gov/pmc/articles/PMC10061602/
https://www.ncbi.nlm.nih.gov/pubmed/37008125
http://dx.doi.org/10.1021/acsomega.2c08039
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