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Inverse ZrO(2)/Cu as a highly efficient methanol synthesis catalyst from CO(2) hydrogenation
Enhancing the intrinsic activity and space time yield of Cu based heterogeneous methanol synthesis catalysts through CO(2) hydrogenation is one of the major topics in CO(2) conversion into value-added liquid fuels and chemicals. Here we report inverse ZrO(2)/Cu catalysts with a tunable Zr/Cu ratio h...
Autores principales: | , , , , , , , , , , , , , , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
Publicado: |
Nature Publishing Group UK
2020
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7666171/ https://www.ncbi.nlm.nih.gov/pubmed/33188189 http://dx.doi.org/10.1038/s41467-020-19634-8 |
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author | Wu, Congyi Lin, Lili Liu, Jinjia Zhang, Jingpeng Zhang, Feng Zhou, Tong Rui, Ning Yao, Siyu Deng, Yuchen Yang, Feng Xu, Wenqian Luo, Jun Zhao, Yue Yan, Binhang Wen, Xiao-Dong Rodriguez, José A. Ma, Ding |
author_facet | Wu, Congyi Lin, Lili Liu, Jinjia Zhang, Jingpeng Zhang, Feng Zhou, Tong Rui, Ning Yao, Siyu Deng, Yuchen Yang, Feng Xu, Wenqian Luo, Jun Zhao, Yue Yan, Binhang Wen, Xiao-Dong Rodriguez, José A. Ma, Ding |
author_sort | Wu, Congyi |
collection | PubMed |
description | Enhancing the intrinsic activity and space time yield of Cu based heterogeneous methanol synthesis catalysts through CO(2) hydrogenation is one of the major topics in CO(2) conversion into value-added liquid fuels and chemicals. Here we report inverse ZrO(2)/Cu catalysts with a tunable Zr/Cu ratio have been prepared via an oxalate co-precipitation method, showing excellent performance for CO(2) hydrogenation to methanol. Under optimal condition, the catalyst composed by 10% of ZrO(2) supported over 90% of Cu exhibits the highest mass-specific methanol formation rate of 524 g(MeOH)kg(cat)(−1)h(−1) at 220 °C, 3.3 times higher than the activity of traditional Cu/ZrO(2) catalysts (159 g(MeOH)kg(cat)(−1)h(−1)). In situ XRD-PDF, XAFS and AP-XPS structural studies reveal that the inverse ZrO(2)/Cu catalysts are composed of islands of partially reduced 1–2 nm amorphous ZrO(2) supported over metallic Cu particles. The ZrO(2) islands are highly active for the CO(2) activation. Meanwhile, an intermediate of formate adsorbed on the Cu at 1350 cm(−1) is discovered by the in situ DRIFTS. This formate intermediate exhibits fast hydrogenation conversion to methoxy. The activation of CO(2) and hydrogenation of all the surface oxygenate intermediates are significantly accelerated over the inverse ZrO(2)/Cu configuration, accounting for the excellent methanol formation activity observed. |
format | Online Article Text |
id | pubmed-7666171 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2020 |
publisher | Nature Publishing Group UK |
record_format | MEDLINE/PubMed |
spelling | pubmed-76661712020-11-17 Inverse ZrO(2)/Cu as a highly efficient methanol synthesis catalyst from CO(2) hydrogenation Wu, Congyi Lin, Lili Liu, Jinjia Zhang, Jingpeng Zhang, Feng Zhou, Tong Rui, Ning Yao, Siyu Deng, Yuchen Yang, Feng Xu, Wenqian Luo, Jun Zhao, Yue Yan, Binhang Wen, Xiao-Dong Rodriguez, José A. Ma, Ding Nat Commun Article Enhancing the intrinsic activity and space time yield of Cu based heterogeneous methanol synthesis catalysts through CO(2) hydrogenation is one of the major topics in CO(2) conversion into value-added liquid fuels and chemicals. Here we report inverse ZrO(2)/Cu catalysts with a tunable Zr/Cu ratio have been prepared via an oxalate co-precipitation method, showing excellent performance for CO(2) hydrogenation to methanol. Under optimal condition, the catalyst composed by 10% of ZrO(2) supported over 90% of Cu exhibits the highest mass-specific methanol formation rate of 524 g(MeOH)kg(cat)(−1)h(−1) at 220 °C, 3.3 times higher than the activity of traditional Cu/ZrO(2) catalysts (159 g(MeOH)kg(cat)(−1)h(−1)). In situ XRD-PDF, XAFS and AP-XPS structural studies reveal that the inverse ZrO(2)/Cu catalysts are composed of islands of partially reduced 1–2 nm amorphous ZrO(2) supported over metallic Cu particles. The ZrO(2) islands are highly active for the CO(2) activation. Meanwhile, an intermediate of formate adsorbed on the Cu at 1350 cm(−1) is discovered by the in situ DRIFTS. This formate intermediate exhibits fast hydrogenation conversion to methoxy. The activation of CO(2) and hydrogenation of all the surface oxygenate intermediates are significantly accelerated over the inverse ZrO(2)/Cu configuration, accounting for the excellent methanol formation activity observed. Nature Publishing Group UK 2020-11-13 /pmc/articles/PMC7666171/ /pubmed/33188189 http://dx.doi.org/10.1038/s41467-020-19634-8 Text en © The Author(s) 2020 Open Access This article is licensed under a Creative Commons Attribution 4.0 International License, which permits use, sharing, adaptation, distribution and reproduction in any medium or format, as long as you give appropriate credit to the original author(s) and the source, provide a link to the Creative Commons license, and indicate if changes were made. The images or other third party material in this article are included in the article’s Creative Commons license, unless indicated otherwise in a credit line to the material. If material is not included in the article’s Creative Commons license and your intended use is not permitted by statutory regulation or exceeds the permitted use, you will need to obtain permission directly from the copyright holder. To view a copy of this license, visit http://creativecommons.org/licenses/by/4.0/. |
spellingShingle | Article Wu, Congyi Lin, Lili Liu, Jinjia Zhang, Jingpeng Zhang, Feng Zhou, Tong Rui, Ning Yao, Siyu Deng, Yuchen Yang, Feng Xu, Wenqian Luo, Jun Zhao, Yue Yan, Binhang Wen, Xiao-Dong Rodriguez, José A. Ma, Ding Inverse ZrO(2)/Cu as a highly efficient methanol synthesis catalyst from CO(2) hydrogenation |
title | Inverse ZrO(2)/Cu as a highly efficient methanol synthesis catalyst from CO(2) hydrogenation |
title_full | Inverse ZrO(2)/Cu as a highly efficient methanol synthesis catalyst from CO(2) hydrogenation |
title_fullStr | Inverse ZrO(2)/Cu as a highly efficient methanol synthesis catalyst from CO(2) hydrogenation |
title_full_unstemmed | Inverse ZrO(2)/Cu as a highly efficient methanol synthesis catalyst from CO(2) hydrogenation |
title_short | Inverse ZrO(2)/Cu as a highly efficient methanol synthesis catalyst from CO(2) hydrogenation |
title_sort | inverse zro(2)/cu as a highly efficient methanol synthesis catalyst from co(2) hydrogenation |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC7666171/ https://www.ncbi.nlm.nih.gov/pubmed/33188189 http://dx.doi.org/10.1038/s41467-020-19634-8 |
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