Cobalt Element Effect of Ternary Mesoporous Cerium Lanthanum Solid Solution for the Catalytic Conversion of Methanol and CO<sub>2</sub> into Dimethyl Carbonate
A citric acid ligand assisted self-assembly method is used for the synthesis of ternary mesoporous cerium lanthanum solid solution doped with metal elements (Co, Zr, Mg). Their textural property was characterized by X-ray diffraction, transmission electron microscopy, N<sub>2</sub> adsor...
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MDPI AG
2022-01-01
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| Online Access: | https://www.mdpi.com/1420-3049/27/1/270 |
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| author | Xu Li Hua Shi Yunhan Gu Qingyan Cheng Yanji Wang |
| author_facet | Xu Li Hua Shi Yunhan Gu Qingyan Cheng Yanji Wang |
| author_sort | Xu Li |
| collection | DOAJ |
| description | A citric acid ligand assisted self-assembly method is used for the synthesis of ternary mesoporous cerium lanthanum solid solution doped with metal elements (Co, Zr, Mg). Their textural property was characterized by X-ray diffraction, transmission electron microscopy, N<sub>2</sub> adsorption-desorption, X-ray photoelectron spectroscopy and TPD techniques, and so on. The results of catalytic testing for synthesis of dimethyl carbonate (DMC) from CH<sub>3</sub>OH and CO<sub>2</sub> indicated that the DMC yield reached 316 mmol/g on Ce-La-Co solid solution when the reaction temperature was 413 K and the reaction pressure was 8.0 MPa. It was found that Co had synergistic effect with La and Ce, doping of Co on the mesoporous Ce-La solid solution was helpful to increase the surface area of the catalyst, promote CO<sub>2</sub> adsorption and activation, and improve the redox performance of solid solution catalyst. The conversion of Co<sup>2+</sup> to Co<sup>3+</sup> resulted in the continuous redox cycle between Ce<sup>4+</sup> and Ce<sup>3+</sup>, and the oxygen vacancy content of the catalyst was increased. Studies have shown that the catalytic performance of Ce-La-Co solid solution is positively correlated with oxygen vacancy content. On this basis, the reaction mechanism of DMC synthesis from CO<sub>2</sub> and CH<sub>3</sub>OH on the catalyst was speculated. |
| first_indexed | 2024-03-10T03:30:12Z |
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| last_indexed | 2024-03-10T03:30:12Z |
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| spelling | doaj.art-b745f67499bd4cfaa0d0c5b783a782232023-11-23T11:59:11ZengMDPI AGMolecules1420-30492022-01-0127127010.3390/molecules27010270Cobalt Element Effect of Ternary Mesoporous Cerium Lanthanum Solid Solution for the Catalytic Conversion of Methanol and CO<sub>2</sub> into Dimethyl CarbonateXu Li0Hua Shi1Yunhan Gu2Qingyan Cheng3Yanji Wang4Key Laboratory of Green Chemical Technology and High Efficient Energy Saving of Hebei Province, Tianjin Key Laboratory of Chemical Process Safety, School of Chemical Engineering, Hebei University of Technology, Tianjin 300401, ChinaChina Tianchen Engineering Corporation, Tianjin 300499, ChinaKey Laboratory of Green Chemical Technology and High Efficient Energy Saving of Hebei Province, Tianjin Key Laboratory of Chemical Process Safety, School of Chemical Engineering, Hebei University of Technology, Tianjin 300401, ChinaKey Laboratory of Green Chemical Technology and High Efficient Energy Saving of Hebei Province, Tianjin Key Laboratory of Chemical Process Safety, School of Chemical Engineering, Hebei University of Technology, Tianjin 300401, ChinaKey Laboratory of Green Chemical Technology and High Efficient Energy Saving of Hebei Province, Tianjin Key Laboratory of Chemical Process Safety, School of Chemical Engineering, Hebei University of Technology, Tianjin 300401, ChinaA citric acid ligand assisted self-assembly method is used for the synthesis of ternary mesoporous cerium lanthanum solid solution doped with metal elements (Co, Zr, Mg). Their textural property was characterized by X-ray diffraction, transmission electron microscopy, N<sub>2</sub> adsorption-desorption, X-ray photoelectron spectroscopy and TPD techniques, and so on. The results of catalytic testing for synthesis of dimethyl carbonate (DMC) from CH<sub>3</sub>OH and CO<sub>2</sub> indicated that the DMC yield reached 316 mmol/g on Ce-La-Co solid solution when the reaction temperature was 413 K and the reaction pressure was 8.0 MPa. It was found that Co had synergistic effect with La and Ce, doping of Co on the mesoporous Ce-La solid solution was helpful to increase the surface area of the catalyst, promote CO<sub>2</sub> adsorption and activation, and improve the redox performance of solid solution catalyst. The conversion of Co<sup>2+</sup> to Co<sup>3+</sup> resulted in the continuous redox cycle between Ce<sup>4+</sup> and Ce<sup>3+</sup>, and the oxygen vacancy content of the catalyst was increased. Studies have shown that the catalytic performance of Ce-La-Co solid solution is positively correlated with oxygen vacancy content. On this basis, the reaction mechanism of DMC synthesis from CO<sub>2</sub> and CH<sub>3</sub>OH on the catalyst was speculated.https://www.mdpi.com/1420-3049/27/1/270solid solutioncatalystcobaltdimethyl carbonateoxygen vacancy |
| spellingShingle | Xu Li Hua Shi Yunhan Gu Qingyan Cheng Yanji Wang Cobalt Element Effect of Ternary Mesoporous Cerium Lanthanum Solid Solution for the Catalytic Conversion of Methanol and CO<sub>2</sub> into Dimethyl Carbonate Molecules solid solution catalyst cobalt dimethyl carbonate oxygen vacancy |
| title | Cobalt Element Effect of Ternary Mesoporous Cerium Lanthanum Solid Solution for the Catalytic Conversion of Methanol and CO<sub>2</sub> into Dimethyl Carbonate |
| title_full | Cobalt Element Effect of Ternary Mesoporous Cerium Lanthanum Solid Solution for the Catalytic Conversion of Methanol and CO<sub>2</sub> into Dimethyl Carbonate |
| title_fullStr | Cobalt Element Effect of Ternary Mesoporous Cerium Lanthanum Solid Solution for the Catalytic Conversion of Methanol and CO<sub>2</sub> into Dimethyl Carbonate |
| title_full_unstemmed | Cobalt Element Effect of Ternary Mesoporous Cerium Lanthanum Solid Solution for the Catalytic Conversion of Methanol and CO<sub>2</sub> into Dimethyl Carbonate |
| title_short | Cobalt Element Effect of Ternary Mesoporous Cerium Lanthanum Solid Solution for the Catalytic Conversion of Methanol and CO<sub>2</sub> into Dimethyl Carbonate |
| title_sort | cobalt element effect of ternary mesoporous cerium lanthanum solid solution for the catalytic conversion of methanol and co sub 2 sub into dimethyl carbonate |
| topic | solid solution catalyst cobalt dimethyl carbonate oxygen vacancy |
| url | https://www.mdpi.com/1420-3049/27/1/270 |
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