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Uranium-Doped Zinc, Copper, and Nickel Oxides for Enhanced Catalytic Conversion of Furfural to Furfuryl Alcohol: A Relativistic DFT Study
Transition metal oxides (TMOs) and actinide ones (AnOs) have been widely applied in catalytic reactions due to their excellent physicochemical properties. However, the reaction pathway and mechanism, especially involving TM–An heterometallic centers, remain underexplored. In this respect, relativist...
Autores principales: | , , , |
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Formato: | Online Artículo Texto |
Lenguaje: | English |
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MDPI
2022
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Materias: | |
Acceso en línea: | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9502827/ https://www.ncbi.nlm.nih.gov/pubmed/36144824 http://dx.doi.org/10.3390/molecules27186094 |
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author | Li, Shuang Hou, Yu-Chang Guo, Yuan-Ru Pan, Qing-Jiang |
author_facet | Li, Shuang Hou, Yu-Chang Guo, Yuan-Ru Pan, Qing-Jiang |
author_sort | Li, Shuang |
collection | PubMed |
description | Transition metal oxides (TMOs) and actinide ones (AnOs) have been widely applied in catalytic reactions due to their excellent physicochemical properties. However, the reaction pathway and mechanism, especially involving TM–An heterometallic centers, remain underexplored. In this respect, relativistic density functional theory (DFT) was used to examine uranium-doped zinc, copper, and nickel oxides for their catalytic activity toward the conversion of furfural to furfuryl alcohol. A comparison was made with their undoped TMOs. It was found that the three TMOs were capable of catalyzing the reaction, where the free energies of adsorption, hydrogenation, and desorption fell between −33.93 and 45.00 kJ/mol. The uranium doping extremely strengthened the adsorption of CuO-U and NiO-U toward furfural, making hydrogenation or desorption much harder. Intriguingly, ZnO-U showed the best catalytic performance among all six catalyst candidates, as its three reaction energies were very small (−10.54–8.12 kJ/mol). The reaction process and mechanism were further addressed in terms of the geometrical, bonding, charge, and electronic properties. |
format | Online Article Text |
id | pubmed-9502827 |
institution | National Center for Biotechnology Information |
language | English |
publishDate | 2022 |
publisher | MDPI |
record_format | MEDLINE/PubMed |
spelling | pubmed-95028272022-09-24 Uranium-Doped Zinc, Copper, and Nickel Oxides for Enhanced Catalytic Conversion of Furfural to Furfuryl Alcohol: A Relativistic DFT Study Li, Shuang Hou, Yu-Chang Guo, Yuan-Ru Pan, Qing-Jiang Molecules Article Transition metal oxides (TMOs) and actinide ones (AnOs) have been widely applied in catalytic reactions due to their excellent physicochemical properties. However, the reaction pathway and mechanism, especially involving TM–An heterometallic centers, remain underexplored. In this respect, relativistic density functional theory (DFT) was used to examine uranium-doped zinc, copper, and nickel oxides for their catalytic activity toward the conversion of furfural to furfuryl alcohol. A comparison was made with their undoped TMOs. It was found that the three TMOs were capable of catalyzing the reaction, where the free energies of adsorption, hydrogenation, and desorption fell between −33.93 and 45.00 kJ/mol. The uranium doping extremely strengthened the adsorption of CuO-U and NiO-U toward furfural, making hydrogenation or desorption much harder. Intriguingly, ZnO-U showed the best catalytic performance among all six catalyst candidates, as its three reaction energies were very small (−10.54–8.12 kJ/mol). The reaction process and mechanism were further addressed in terms of the geometrical, bonding, charge, and electronic properties. MDPI 2022-09-18 /pmc/articles/PMC9502827/ /pubmed/36144824 http://dx.doi.org/10.3390/molecules27186094 Text en © 2022 by the authors. https://creativecommons.org/licenses/by/4.0/Licensee MDPI, Basel, Switzerland. This article is an open access article distributed under the terms and conditions of the Creative Commons Attribution (CC BY) license (https://creativecommons.org/licenses/by/4.0/). |
spellingShingle | Article Li, Shuang Hou, Yu-Chang Guo, Yuan-Ru Pan, Qing-Jiang Uranium-Doped Zinc, Copper, and Nickel Oxides for Enhanced Catalytic Conversion of Furfural to Furfuryl Alcohol: A Relativistic DFT Study |
title | Uranium-Doped Zinc, Copper, and Nickel Oxides for Enhanced Catalytic Conversion of Furfural to Furfuryl Alcohol: A Relativistic DFT Study |
title_full | Uranium-Doped Zinc, Copper, and Nickel Oxides for Enhanced Catalytic Conversion of Furfural to Furfuryl Alcohol: A Relativistic DFT Study |
title_fullStr | Uranium-Doped Zinc, Copper, and Nickel Oxides for Enhanced Catalytic Conversion of Furfural to Furfuryl Alcohol: A Relativistic DFT Study |
title_full_unstemmed | Uranium-Doped Zinc, Copper, and Nickel Oxides for Enhanced Catalytic Conversion of Furfural to Furfuryl Alcohol: A Relativistic DFT Study |
title_short | Uranium-Doped Zinc, Copper, and Nickel Oxides for Enhanced Catalytic Conversion of Furfural to Furfuryl Alcohol: A Relativistic DFT Study |
title_sort | uranium-doped zinc, copper, and nickel oxides for enhanced catalytic conversion of furfural to furfuryl alcohol: a relativistic dft study |
topic | Article |
url | https://www.ncbi.nlm.nih.gov/pmc/articles/PMC9502827/ https://www.ncbi.nlm.nih.gov/pubmed/36144824 http://dx.doi.org/10.3390/molecules27186094 |
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