{"title":"锰掺杂Ni-Cu/Co改性稻壳中介孔SiO2的CO2甲烷化研究","authors":"Margarita Popova, Momtchil Dimitrov, Manuela Oykova, Pavletta Shestakova, Daniela Kovacheva, Genoveva Atanasova, Ágnes Szegedi","doi":"10.1007/s11356-025-35931-5","DOIUrl":null,"url":null,"abstract":"<p><p>Mesoporous silica (SiO<sub>2</sub>) was prepared using a simple procedure from rice husks without the application of a template. Incipient wetness impregnation method was employed to prepare magnesium-doped nickel-copper- and nickel-cobalt-containing SiO<sub>2</sub> catalysts. The obtained materials were characterized by X-ray powder diffraction (XRD), N<sub>2</sub> physisorption, transmission electron microscopy (TEM), temperature-programmed reduction (TPR-TGA), and NMR and XPS spectroscopies. The study demonstrated the significant influence of Ni and Co/Cu content, as well as the sequence of Mg promotion (before or after the nickel-copper- and nickel-cobalt-modification) on the physico-chemical properties of the catalysts. The peculiar properties of the mesoporous carrier positively influenced the formation of finely dispersed nickel and/or copper/cobalt oxide species, which were readily reducible at temperatures below 600 °C. XPS analysis revealed that the surface of Mg-doped Ni-Co supported SiO<sub>2</sub> catalysts was rich in nickel. All the prepared catalysts were active in CO<sub>2</sub> hydrogenation to methane. The Mg-doped Ni-Co supported SiO<sub>2</sub> catalysts showed higher catalytic activity compared to their Mg-doped Ni-Cu counterparts. The 1.5Mg10Ni5Co/SiO<sub>2</sub> catalyst demonstrated 82% CO<sub>2</sub> conversion and 99.5% selectivity to methane. The activity and selectivity of this catalyst was maintained at 400 °C for a reaction time of 4 h.</p>","PeriodicalId":545,"journal":{"name":"Environmental Science and Pollution Research","volume":" ","pages":""},"PeriodicalIF":5.8000,"publicationDate":"2025-02-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"CO<sub>2</sub> methanation on Mg-doped Ni-Cu/Co modified mesoporous SiO<sub>2</sub> derived from rice husks.\",\"authors\":\"Margarita Popova, Momtchil Dimitrov, Manuela Oykova, Pavletta Shestakova, Daniela Kovacheva, Genoveva Atanasova, Ágnes Szegedi\",\"doi\":\"10.1007/s11356-025-35931-5\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<p><p>Mesoporous silica (SiO<sub>2</sub>) was prepared using a simple procedure from rice husks without the application of a template. Incipient wetness impregnation method was employed to prepare magnesium-doped nickel-copper- and nickel-cobalt-containing SiO<sub>2</sub> catalysts. The obtained materials were characterized by X-ray powder diffraction (XRD), N<sub>2</sub> physisorption, transmission electron microscopy (TEM), temperature-programmed reduction (TPR-TGA), and NMR and XPS spectroscopies. The study demonstrated the significant influence of Ni and Co/Cu content, as well as the sequence of Mg promotion (before or after the nickel-copper- and nickel-cobalt-modification) on the physico-chemical properties of the catalysts. The peculiar properties of the mesoporous carrier positively influenced the formation of finely dispersed nickel and/or copper/cobalt oxide species, which were readily reducible at temperatures below 600 °C. XPS analysis revealed that the surface of Mg-doped Ni-Co supported SiO<sub>2</sub> catalysts was rich in nickel. All the prepared catalysts were active in CO<sub>2</sub> hydrogenation to methane. The Mg-doped Ni-Co supported SiO<sub>2</sub> catalysts showed higher catalytic activity compared to their Mg-doped Ni-Cu counterparts. The 1.5Mg10Ni5Co/SiO<sub>2</sub> catalyst demonstrated 82% CO<sub>2</sub> conversion and 99.5% selectivity to methane. The activity and selectivity of this catalyst was maintained at 400 °C for a reaction time of 4 h.</p>\",\"PeriodicalId\":545,\"journal\":{\"name\":\"Environmental Science and Pollution Research\",\"volume\":\" \",\"pages\":\"\"},\"PeriodicalIF\":5.8000,\"publicationDate\":\"2025-02-10\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Environmental Science and Pollution Research\",\"FirstCategoryId\":\"93\",\"ListUrlMain\":\"https://doi.org/10.1007/s11356-025-35931-5\",\"RegionNum\":3,\"RegionCategory\":\"环境科学与生态学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"0\",\"JCRName\":\"ENVIRONMENTAL SCIENCES\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Environmental Science and Pollution Research","FirstCategoryId":"93","ListUrlMain":"https://doi.org/10.1007/s11356-025-35931-5","RegionNum":3,"RegionCategory":"环境科学与生态学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"0","JCRName":"ENVIRONMENTAL SCIENCES","Score":null,"Total":0}
CO2 methanation on Mg-doped Ni-Cu/Co modified mesoporous SiO2 derived from rice husks.
Mesoporous silica (SiO2) was prepared using a simple procedure from rice husks without the application of a template. Incipient wetness impregnation method was employed to prepare magnesium-doped nickel-copper- and nickel-cobalt-containing SiO2 catalysts. The obtained materials were characterized by X-ray powder diffraction (XRD), N2 physisorption, transmission electron microscopy (TEM), temperature-programmed reduction (TPR-TGA), and NMR and XPS spectroscopies. The study demonstrated the significant influence of Ni and Co/Cu content, as well as the sequence of Mg promotion (before or after the nickel-copper- and nickel-cobalt-modification) on the physico-chemical properties of the catalysts. The peculiar properties of the mesoporous carrier positively influenced the formation of finely dispersed nickel and/or copper/cobalt oxide species, which were readily reducible at temperatures below 600 °C. XPS analysis revealed that the surface of Mg-doped Ni-Co supported SiO2 catalysts was rich in nickel. All the prepared catalysts were active in CO2 hydrogenation to methane. The Mg-doped Ni-Co supported SiO2 catalysts showed higher catalytic activity compared to their Mg-doped Ni-Cu counterparts. The 1.5Mg10Ni5Co/SiO2 catalyst demonstrated 82% CO2 conversion and 99.5% selectivity to methane. The activity and selectivity of this catalyst was maintained at 400 °C for a reaction time of 4 h.
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