Bui T. Thu-Thao , Ngoc-Dung Lai , Ponnusamy Senthil Kumar , Tan Ji Siang , Thuy-Phuong T. Pham , Natarajan Rajamohan , Shams Forruque Ahmed , G. Abdulkareem-Alsultan , Aishah Abdul Jalil , Mohammad Yusuf , Dai-Viet N. Vo
{"title":"耐焦掺杂钴/介孔氧化铝催化剂在甲烷干转化过程中制氢","authors":"Bui T. Thu-Thao , Ngoc-Dung Lai , Ponnusamy Senthil Kumar , Tan Ji Siang , Thuy-Phuong T. Pham , Natarajan Rajamohan , Shams Forruque Ahmed , G. Abdulkareem-Alsultan , Aishah Abdul Jalil , Mohammad Yusuf , Dai-Viet N. Vo","doi":"10.1016/j.joei.2025.102116","DOIUrl":null,"url":null,"abstract":"<div><div>Dry reforming of methane, DRM is largely recognized as a promising route for generating H<sub>2</sub> energy to substitute fossil fuels. In this work, the promotional effect of praseodymium dopant (0-7 wt %) on the performance and coking resistance of mesoporous alumina (MA)-dispersed Co catalysts was investigated at a stoichiometric DRM feed composition and 650–750 °C. Pr promotion considerably reduced Co<sub>3</sub>O<sub>4</sub> crystal dimension from 16.8 to 7.8 nm and 5Pr10Co/MA possessed the smallest Co<sub>3</sub>O<sub>4</sub> crystallite size. The total basic site concentration was boosted with Pr addition from 66.8 to 169.7 μmol CO<sub>2</sub> <span><math><mrow><msubsup><mi>g</mi><mrow><mi>c</mi><mi>a</mi><mi>t</mi></mrow><mrow><mo>−</mo><mn>1</mn></mrow></msubsup></mrow></math></span>. Stable CH<sub>4</sub> conversion with time-on-stream was evidenced on Pr-promoted catalysts (1 %-5 %Pr) because of enhancing basic site concentration and CO<sub>2</sub> adsorption. Notably, 5Pr10Co/MA achieved the greatest CH<sub>4</sub> (90.91 %) and CO<sub>2</sub> (82.13 %) conversions at 700 °C and exhibited the highest coke resistance with the least carbon deposition percentage (0.87 %) and carbon formation rate (2.42 × 10<sup>−5</sup> <span><math><mrow><msub><mi>g</mi><mrow><mi>c</mi><mi>a</mi><mi>r</mi><mi>b</mi><mi>o</mi><mi>n</mi></mrow></msub><mspace></mspace><msubsup><mi>g</mi><mrow><mi>c</mi><mi>a</mi><mi>t</mi></mrow><mrow><mo>−</mo><mn>1</mn></mrow></msubsup></mrow></math></span> min<sup>−1</sup>) owing to the smallest Co<sub>3</sub>O<sub>4</sub> crystallite size, oxygen vacancy and redox attributes. An enhancement in H<sub>2</sub> yield from 52.52 % to 87.94 % was evidenced on 5Pr10Co/MA with rising temperature from 650 to 750 °C. The two-step mechanism for coke suppression triggered by a redox PrO<sub>2</sub>/Pr<sub>2</sub>O<sub>3</sub> pair was also elaborated in this study.</div></div>","PeriodicalId":17287,"journal":{"name":"Journal of The Energy Institute","volume":"120 ","pages":"Article 102116"},"PeriodicalIF":5.6000,"publicationDate":"2025-04-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Hydrogen production from methane dry reforming on coke-resistant Pr-doped Co/mesoporous alumina catalysts\",\"authors\":\"Bui T. Thu-Thao , Ngoc-Dung Lai , Ponnusamy Senthil Kumar , Tan Ji Siang , Thuy-Phuong T. Pham , Natarajan Rajamohan , Shams Forruque Ahmed , G. Abdulkareem-Alsultan , Aishah Abdul Jalil , Mohammad Yusuf , Dai-Viet N. Vo\",\"doi\":\"10.1016/j.joei.2025.102116\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"<div><div>Dry reforming of methane, DRM is largely recognized as a promising route for generating H<sub>2</sub> energy to substitute fossil fuels. In this work, the promotional effect of praseodymium dopant (0-7 wt %) on the performance and coking resistance of mesoporous alumina (MA)-dispersed Co catalysts was investigated at a stoichiometric DRM feed composition and 650–750 °C. Pr promotion considerably reduced Co<sub>3</sub>O<sub>4</sub> crystal dimension from 16.8 to 7.8 nm and 5Pr10Co/MA possessed the smallest Co<sub>3</sub>O<sub>4</sub> crystallite size. The total basic site concentration was boosted with Pr addition from 66.8 to 169.7 μmol CO<sub>2</sub> <span><math><mrow><msubsup><mi>g</mi><mrow><mi>c</mi><mi>a</mi><mi>t</mi></mrow><mrow><mo>−</mo><mn>1</mn></mrow></msubsup></mrow></math></span>. Stable CH<sub>4</sub> conversion with time-on-stream was evidenced on Pr-promoted catalysts (1 %-5 %Pr) because of enhancing basic site concentration and CO<sub>2</sub> adsorption. Notably, 5Pr10Co/MA achieved the greatest CH<sub>4</sub> (90.91 %) and CO<sub>2</sub> (82.13 %) conversions at 700 °C and exhibited the highest coke resistance with the least carbon deposition percentage (0.87 %) and carbon formation rate (2.42 × 10<sup>−5</sup> <span><math><mrow><msub><mi>g</mi><mrow><mi>c</mi><mi>a</mi><mi>r</mi><mi>b</mi><mi>o</mi><mi>n</mi></mrow></msub><mspace></mspace><msubsup><mi>g</mi><mrow><mi>c</mi><mi>a</mi><mi>t</mi></mrow><mrow><mo>−</mo><mn>1</mn></mrow></msubsup></mrow></math></span> min<sup>−1</sup>) owing to the smallest Co<sub>3</sub>O<sub>4</sub> crystallite size, oxygen vacancy and redox attributes. An enhancement in H<sub>2</sub> yield from 52.52 % to 87.94 % was evidenced on 5Pr10Co/MA with rising temperature from 650 to 750 °C. The two-step mechanism for coke suppression triggered by a redox PrO<sub>2</sub>/Pr<sub>2</sub>O<sub>3</sub> pair was also elaborated in this study.</div></div>\",\"PeriodicalId\":17287,\"journal\":{\"name\":\"Journal of The Energy Institute\",\"volume\":\"120 \",\"pages\":\"Article 102116\"},\"PeriodicalIF\":5.6000,\"publicationDate\":\"2025-04-19\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of The Energy Institute\",\"FirstCategoryId\":\"5\",\"ListUrlMain\":\"https://www.sciencedirect.com/science/article/pii/S1743967125001448\",\"RegionNum\":2,\"RegionCategory\":\"工程技术\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"ENERGY & FUELS\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of The Energy Institute","FirstCategoryId":"5","ListUrlMain":"https://www.sciencedirect.com/science/article/pii/S1743967125001448","RegionNum":2,"RegionCategory":"工程技术","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"ENERGY & FUELS","Score":null,"Total":0}
Hydrogen production from methane dry reforming on coke-resistant Pr-doped Co/mesoporous alumina catalysts
Dry reforming of methane, DRM is largely recognized as a promising route for generating H2 energy to substitute fossil fuels. In this work, the promotional effect of praseodymium dopant (0-7 wt %) on the performance and coking resistance of mesoporous alumina (MA)-dispersed Co catalysts was investigated at a stoichiometric DRM feed composition and 650–750 °C. Pr promotion considerably reduced Co3O4 crystal dimension from 16.8 to 7.8 nm and 5Pr10Co/MA possessed the smallest Co3O4 crystallite size. The total basic site concentration was boosted with Pr addition from 66.8 to 169.7 μmol CO2 . Stable CH4 conversion with time-on-stream was evidenced on Pr-promoted catalysts (1 %-5 %Pr) because of enhancing basic site concentration and CO2 adsorption. Notably, 5Pr10Co/MA achieved the greatest CH4 (90.91 %) and CO2 (82.13 %) conversions at 700 °C and exhibited the highest coke resistance with the least carbon deposition percentage (0.87 %) and carbon formation rate (2.42 × 10−5 min−1) owing to the smallest Co3O4 crystallite size, oxygen vacancy and redox attributes. An enhancement in H2 yield from 52.52 % to 87.94 % was evidenced on 5Pr10Co/MA with rising temperature from 650 to 750 °C. The two-step mechanism for coke suppression triggered by a redox PrO2/Pr2O3 pair was also elaborated in this study.
期刊介绍:
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