Pd-modified CuO-ZnO-Al2O3 catalysts via mixed-phases-containing precursor for methanol synthesis from CO2 hydrogenation under mild conditions
A series of palladium-modified (Pd-modified) CuO-ZnO-Al2O3 (CZA) catalysts with various Pd loadings (0.3 wt% to 2.4 wt%) were prepared using the wetness impregnation method, on two CZA supports with different structures that are CZA-aged precursor composed of a mixture of zincian-malachite and hydro...
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| Format: | Article |
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KeAi Communications Co., Ltd.
2024-03-01
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| Series: | Carbon Resources Conversion |
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| Online Access: | http://www.sciencedirect.com/science/article/pii/S258891332300039X |
| _version_ | 1797422573089193984 |
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| author | Xiao Fan Kaiying Wang Xiaoqing He Shiguang Li Miao Yu Xinhua Liang |
| author_facet | Xiao Fan Kaiying Wang Xiaoqing He Shiguang Li Miao Yu Xinhua Liang |
| author_sort | Xiao Fan |
| collection | DOAJ |
| description | A series of palladium-modified (Pd-modified) CuO-ZnO-Al2O3 (CZA) catalysts with various Pd loadings (0.3 wt% to 2.4 wt%) were prepared using the wetness impregnation method, on two CZA supports with different structures that are CZA-aged precursor composed of a mixture of zincian-malachite and hydrotalcite-like phases (CZA-zH), and CuO-ZnO-Al2O3 metal oxide nanoparticles (CZA-MO). Enhancement on catalytic activity can be observed on both Pd-modified CZA catalysts in a temperature range of 180–240 °C for methanol synthesis via CO2 hydrogenation. Pd/CZA-zH catalysts exhibited a more efficient and stable production of methanol at a relatively low reaction temperature of 180 °C for 100 hrs of reaction. The improvement of activity is mainly ascribed to a higher surface area and abundant oxygen-containing functional groups (e.g., –OH) of CZA-zH support, which is beneficial for better adsorption and distribution of Pd promoter. Hydrogen temperature programmed reduction and X-ray photoelectron spectroscopy results demonstrated a better interaction between Pd and Cu on Pd/CZA-zH catalysts via enhanced reducibility of CuO, and peak shift of Cu to a lower binding energy. The difference in the efficient utilization of hydrogen spillover effect of Pd promoter over two CZA supports resulted in the different performances for methanol synthesis under mild reaction conditions. |
| first_indexed | 2024-03-09T07:34:14Z |
| format | Article |
| id | doaj.art-633a56827e1e4fc6a33872ac7c6dd9c7 |
| institution | Directory Open Access Journal |
| issn | 2588-9133 |
| language | English |
| last_indexed | 2024-03-09T07:34:14Z |
| publishDate | 2024-03-01 |
| publisher | KeAi Communications Co., Ltd. |
| record_format | Article |
| series | Carbon Resources Conversion |
| spelling | doaj.art-633a56827e1e4fc6a33872ac7c6dd9c72023-12-03T05:42:24ZengKeAi Communications Co., Ltd.Carbon Resources Conversion2588-91332024-03-0171100184Pd-modified CuO-ZnO-Al2O3 catalysts via mixed-phases-containing precursor for methanol synthesis from CO2 hydrogenation under mild conditionsXiao Fan0Kaiying Wang1Xiaoqing He2Shiguang Li3Miao Yu4Xinhua Liang5Linda and Bipin Doshi Department of Chemical and Biochemical Engineering, Missouri University of Science and Technology, Rolla, MO 65409, United StatesDepartment of Energy, Environmental and Chemical Engineering, Washington University in St. Louis, St. Louis, MO 63130, United StatesElectron Microscopy Core Facility, University of Missouri, Columbia, MO 65211, United States; Department of Mechanical and Aerospace Engineering, University of Missouri, Columbia, MO 65211, United StatesGas Technology Institute, 1700 South Mount Prospect Road, Des Plaines, IL 60018, United StatesDepartment of Chemical and Biological Engineering, University at Buffalo, Buffalo, NY 14260, United StatesLinda and Bipin Doshi Department of Chemical and Biochemical Engineering, Missouri University of Science and Technology, Rolla, MO 65409, United States; Department of Energy, Environmental and Chemical Engineering, Washington University in St. Louis, St. Louis, MO 63130, United States; Corresponding author at: Department of Energy, Environmental and Chemical Engineering, Washington University in St. Louis, St. Louis, MO 63130, United States.A series of palladium-modified (Pd-modified) CuO-ZnO-Al2O3 (CZA) catalysts with various Pd loadings (0.3 wt% to 2.4 wt%) were prepared using the wetness impregnation method, on two CZA supports with different structures that are CZA-aged precursor composed of a mixture of zincian-malachite and hydrotalcite-like phases (CZA-zH), and CuO-ZnO-Al2O3 metal oxide nanoparticles (CZA-MO). Enhancement on catalytic activity can be observed on both Pd-modified CZA catalysts in a temperature range of 180–240 °C for methanol synthesis via CO2 hydrogenation. Pd/CZA-zH catalysts exhibited a more efficient and stable production of methanol at a relatively low reaction temperature of 180 °C for 100 hrs of reaction. The improvement of activity is mainly ascribed to a higher surface area and abundant oxygen-containing functional groups (e.g., –OH) of CZA-zH support, which is beneficial for better adsorption and distribution of Pd promoter. Hydrogen temperature programmed reduction and X-ray photoelectron spectroscopy results demonstrated a better interaction between Pd and Cu on Pd/CZA-zH catalysts via enhanced reducibility of CuO, and peak shift of Cu to a lower binding energy. The difference in the efficient utilization of hydrogen spillover effect of Pd promoter over two CZA supports resulted in the different performances for methanol synthesis under mild reaction conditions.http://www.sciencedirect.com/science/article/pii/S258891332300039XCO2 hydrogenationLow-temperature methanol synthesisPd-modificationCuO-ZnO-Al2O3Hydrogen spillover |
| spellingShingle | Xiao Fan Kaiying Wang Xiaoqing He Shiguang Li Miao Yu Xinhua Liang Pd-modified CuO-ZnO-Al2O3 catalysts via mixed-phases-containing precursor for methanol synthesis from CO2 hydrogenation under mild conditions Carbon Resources Conversion CO2 hydrogenation Low-temperature methanol synthesis Pd-modification CuO-ZnO-Al2O3 Hydrogen spillover |
| title | Pd-modified CuO-ZnO-Al2O3 catalysts via mixed-phases-containing precursor for methanol synthesis from CO2 hydrogenation under mild conditions |
| title_full | Pd-modified CuO-ZnO-Al2O3 catalysts via mixed-phases-containing precursor for methanol synthesis from CO2 hydrogenation under mild conditions |
| title_fullStr | Pd-modified CuO-ZnO-Al2O3 catalysts via mixed-phases-containing precursor for methanol synthesis from CO2 hydrogenation under mild conditions |
| title_full_unstemmed | Pd-modified CuO-ZnO-Al2O3 catalysts via mixed-phases-containing precursor for methanol synthesis from CO2 hydrogenation under mild conditions |
| title_short | Pd-modified CuO-ZnO-Al2O3 catalysts via mixed-phases-containing precursor for methanol synthesis from CO2 hydrogenation under mild conditions |
| title_sort | pd modified cuo zno al2o3 catalysts via mixed phases containing precursor for methanol synthesis from co2 hydrogenation under mild conditions |
| topic | CO2 hydrogenation Low-temperature methanol synthesis Pd-modification CuO-ZnO-Al2O3 Hydrogen spillover |
| url | http://www.sciencedirect.com/science/article/pii/S258891332300039X |
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