Structured hierarchical Mn-Co mixed oxides supported on silicalite-1 foam catalyst for catalytic combustion

doi:10.1016/j.cjche.2020.06.019

中国化学工程学报 ›› 2020, Vol. 28 ›› Issue (9): 2319-2327.DOI: 10.1016/j.cjche.2020.06.019

• Catalysis, Kinetics and Reaction Engineering • 上一篇下一篇

Structured hierarchical Mn-Co mixed oxides supported on silicalite-1 foam catalyst for catalytic combustion

Yanan Guan^1,2, Hengyu Shen^1,2, Xing Guo³, Boyang Mao⁴, Zhenyuan Yang^1,2, Yangtao Zhou¹, He Liang⁵, Xiaolei Fan⁶, Yilai Jiao¹, Jinsong Zhang¹

1 Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China;
2 School of Materials Science and Engineering, University of Science and Technology of China, Shenyang 110016, China;
3 Science and Technology on Vacuum Technology and Physics Laboratory, Lanzhou Institute of Physics, Lanzhou 730010, China;
4 Department of Engineering, University of Cambridge, JJ Thomson Avenue, Cambridge CB3 0FA, United Kingdom;
5 Department of Eye and Vision Science, Institute of Life Course and Medical Sciences, University of Liverpool, 6 West Derby Street, Liverpool, L7 8TX, United Kingdom;
6 Department of Chemical Engineering and Analytical Science, School of Engineering, The University of Manchester, Oxford Road, Manchester, M13 9PL, United Kingdom

收稿日期:2020-05-19 修回日期:2020-06-08 出版日期:2020-09-28 发布日期:2020-10-21
通讯作者: Xiaolei Fan, Yilai Jiao, Jinsong Zhang
基金资助:
Yilai Jiao thanks the financial support from the Key Projects of Natural Science Foundation of Liaoning Province (2018010047-301) and the Shenyang National Laboratory for Materials Science for his research (Y8L6641161). Xing Guo thanks the financial support from the National Key R&D Program of China (2016YFB0501303). This project has received funding from European Union's Horizon 2020 research and innovation programme under grant agreement No. 872102.

Structured hierarchical Mn-Co mixed oxides supported on silicalite-1 foam catalyst for catalytic combustion

Yanan Guan^1,2, Hengyu Shen^1,2, Xing Guo³, Boyang Mao⁴, Zhenyuan Yang^1,2, Yangtao Zhou¹, He Liang⁵, Xiaolei Fan⁶, Yilai Jiao¹, Jinsong Zhang¹

1 Shenyang National Laboratory for Materials Science, Institute of Metal Research, Chinese Academy of Sciences, Shenyang 110016, China;
2 School of Materials Science and Engineering, University of Science and Technology of China, Shenyang 110016, China;
3 Science and Technology on Vacuum Technology and Physics Laboratory, Lanzhou Institute of Physics, Lanzhou 730010, China;
4 Department of Engineering, University of Cambridge, JJ Thomson Avenue, Cambridge CB3 0FA, United Kingdom;
5 Department of Eye and Vision Science, Institute of Life Course and Medical Sciences, University of Liverpool, 6 West Derby Street, Liverpool, L7 8TX, United Kingdom;
6 Department of Chemical Engineering and Analytical Science, School of Engineering, The University of Manchester, Oxford Road, Manchester, M13 9PL, United Kingdom

Received:2020-05-19 Revised:2020-06-08 Online:2020-09-28 Published:2020-10-21
Contact: Xiaolei Fan, Yilai Jiao, Jinsong Zhang
Supported by:
Yilai Jiao thanks the financial support from the Key Projects of Natural Science Foundation of Liaoning Province (2018010047-301) and the Shenyang National Laboratory for Materials Science for his research (Y8L6641161). Xing Guo thanks the financial support from the National Key R&D Program of China (2016YFB0501303). This project has received funding from European Union's Horizon 2020 research and innovation programme under grant agreement No. 872102.

摘要/Abstract

摘要： Silicalite-1 (S1) foam was functionalized by supporting manganese-cobalt (Mn-Co) mixed oxides to develop the structured hierarchical catalyst (Mn-Co@S1F) for catalytic combustion for the first time. The self-supporting S1 foam with hierarchical porosity was prepared via hydrothermal synthesis with polyurethane (PU) foam as the template. Subsequently, Mn-Co oxide nano sheets were uniformly grown on the surface of S1 foams under hydrothermal conditions to prepare the structured hierarchical catalyst with specific surface area of 354 m²·g^-1, micropore volume of 0.141 cm³·g^-1 and total pore volume of 0.217 cm³·g^-1, as well as a good capacity to adsorb toluene (1.7 mmol·g^-1 at p/p₀ = 0.99). Comparative catalytic combustion of toluene of over developed structured catalyst Mn-Co@S1F was performed against the control catalysts of bulk Mn-Co@S1 (i.e., the crushed Mn-Co@S1F) and unsupported Mn-Co oxides (i.e., Mn-Co). Mn-Co@S1F exhibited comparatively the best catalytic performance, that is, complete and stable toluene conversion at 248 °C over 65 h due to the synergy between Mn-Co oxides and S1 foam, which provided a large number of oxygen vacancies, high redox capacity. In addition, the hierarchical porous structure also improved the accessibility of active sites and facilitated the global mass transfer across the catalyst bed, being beneficial to the catalysis and catalyst longevity.

关键词: Structured catalyst, Silicalite-1, Mn-Co oxides, Cellular foam, Catalytic combustion

Abstract: Silicalite-1 (S1) foam was functionalized by supporting manganese-cobalt (Mn-Co) mixed oxides to develop the structured hierarchical catalyst (Mn-Co@S1F) for catalytic combustion for the first time. The self-supporting S1 foam with hierarchical porosity was prepared via hydrothermal synthesis with polyurethane (PU) foam as the template. Subsequently, Mn-Co oxide nano sheets were uniformly grown on the surface of S1 foams under hydrothermal conditions to prepare the structured hierarchical catalyst with specific surface area of 354 m²·g^-1, micropore volume of 0.141 cm³·g^-1 and total pore volume of 0.217 cm³·g^-1, as well as a good capacity to adsorb toluene (1.7 mmol·g^-1 at p/p₀ = 0.99). Comparative catalytic combustion of toluene of over developed structured catalyst Mn-Co@S1F was performed against the control catalysts of bulk Mn-Co@S1 (i.e., the crushed Mn-Co@S1F) and unsupported Mn-Co oxides (i.e., Mn-Co). Mn-Co@S1F exhibited comparatively the best catalytic performance, that is, complete and stable toluene conversion at 248 °C over 65 h due to the synergy between Mn-Co oxides and S1 foam, which provided a large number of oxygen vacancies, high redox capacity. In addition, the hierarchical porous structure also improved the accessibility of active sites and facilitated the global mass transfer across the catalyst bed, being beneficial to the catalysis and catalyst longevity.

Key words: Structured catalyst, Silicalite-1, Mn-Co oxides, Cellular foam, Catalytic combustion

Yanan Guan, Hengyu Shen, Xing Guo, Boyang Mao, Zhenyuan Yang, Yangtao Zhou, He Liang, Xiaolei Fan, Yilai Jiao, Jinsong Zhang. Structured hierarchical Mn-Co mixed oxides supported on silicalite-1 foam catalyst for catalytic combustion[J]. 中国化学工程学报, 2020, 28(9): 2319-2327.

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Structured hierarchical Mn-Co mixed oxides supported on silicalite-1 foam catalyst for catalytic combustion

Structured hierarchical Mn-Co mixed oxides supported on silicalite-1 foam catalyst for catalytic combustion

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