Metal-carbonate interface promoted activity of Ag/MgCO₃ catalyst for aqueous-phase formaldehyde reforming into hydrogen
Aqueous-phase reforming of biomass-derived formaldehyde is one of efficient and sustainable routes to generate molecular hydrogen as clean energy resource. In this work, Ag/MgCO3 catalyst is prepared with constructed stable carbonate-modified metal-support interfaces. Under mild and neutral reaction...
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sg-ntu-dr.10356-1706662023-09-25T07:03:19Z Metal-carbonate interface promoted activity of Ag/MgCO₃ catalyst for aqueous-phase formaldehyde reforming into hydrogen Wang, Qiaojuan Wang, Jianyue Rui, Wenjuan Yang, Dan Wan, Xiaoyue Zhou, Chunmei Li, Renhong Liu, Wen Dai, Yihu Yang, Yanhui School of Chemistry, Chemical Engineering and Biotechnology Engineering::Chemical engineering Formaldehyde Reforming Hydrogen Production Aqueous-phase reforming of biomass-derived formaldehyde is one of efficient and sustainable routes to generate molecular hydrogen as clean energy resource. In this work, Ag/MgCO3 catalyst is prepared with constructed stable carbonate-modified metal-support interfaces. Under mild and neutral reaction conditions, it exhibits a near an order of magnitude higher low-temperature activity in formaldehyde reforming reaction for producing hydrogen in comparison with Ag/MgO. The catalytic and spectral observations reveal that the Ag/MgCO3-catalyzed reaction follows an O2-involved HCHO/H2O reforming reaction pathway through O2[rad]−, [rad]OOH and [rad]H radicals as highly active intermediates. Ag/MgCO3 catalyst shows high rates in isotopic H2-D2 exchange and HCHO/D2O reforming reactions and displays an apparent activation energy (Ea) as low as 7.5 kJ mol−1 within 10–50 °C, indicating facile activation of HCHO C[sbnd]H and H2O O[sbnd]H bonds. Furthermore, Ag/MgCO3 catalyst adsorbs HCHO molecule in a favorable configuration and strength, as evidenced by the HCHO desorption profile. Comprehensive positive factors benefit to the superior hydrogen production activity of carbonate-modified Ag/MgCO3 than Ag/MgO. We thank National Natural Science Foundation of China (22178161), Postdoctoral Science Foundation of China (2022 M711597), and National Key R&D Program of China (2018YFE0122600) for the financial support. 2023-09-25T07:03:19Z 2023-09-25T07:03:19Z 2023 Journal Article Wang, Q., Wang, J., Rui, W., Yang, D., Wan, X., Zhou, C., Li, R., Liu, W., Dai, Y. & Yang, Y. (2023). Metal-carbonate interface promoted activity of Ag/MgCO₃ catalyst for aqueous-phase formaldehyde reforming into hydrogen. Fuel, 337, 126897-. https://dx.doi.org/10.1016/j.fuel.2022.126897 0016-2361 https://hdl.handle.net/10356/170666 10.1016/j.fuel.2022.126897 2-s2.0-85146470004 337 126897 en Fuel © 2022 Elsevier Ltd. All rights reserved. |
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Engineering::Chemical engineering Formaldehyde Reforming Hydrogen Production Wang, Qiaojuan Wang, Jianyue Rui, Wenjuan Yang, Dan Wan, Xiaoyue Zhou, Chunmei Li, Renhong Liu, Wen Dai, Yihu Yang, Yanhui Metal-carbonate interface promoted activity of Ag/MgCO₃ catalyst for aqueous-phase formaldehyde reforming into hydrogen |
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Aqueous-phase reforming of biomass-derived formaldehyde is one of efficient and sustainable routes to generate molecular hydrogen as clean energy resource. In this work, Ag/MgCO3 catalyst is prepared with constructed stable carbonate-modified metal-support interfaces. Under mild and neutral reaction conditions, it exhibits a near an order of magnitude higher low-temperature activity in formaldehyde reforming reaction for producing hydrogen in comparison with Ag/MgO. The catalytic and spectral observations reveal that the Ag/MgCO3-catalyzed reaction follows an O2-involved HCHO/H2O reforming reaction pathway through O2[rad]−, [rad]OOH and [rad]H radicals as highly active intermediates. Ag/MgCO3 catalyst shows high rates in isotopic H2-D2 exchange and HCHO/D2O reforming reactions and displays an apparent activation energy (Ea) as low as 7.5 kJ mol−1 within 10–50 °C, indicating facile activation of HCHO C[sbnd]H and H2O O[sbnd]H bonds. Furthermore, Ag/MgCO3 catalyst adsorbs HCHO molecule in a favorable configuration and strength, as evidenced by the HCHO desorption profile. Comprehensive positive factors benefit to the superior hydrogen production activity of carbonate-modified Ag/MgCO3 than Ag/MgO. |
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School of Chemistry, Chemical Engineering and Biotechnology |
author_facet |
School of Chemistry, Chemical Engineering and Biotechnology Wang, Qiaojuan Wang, Jianyue Rui, Wenjuan Yang, Dan Wan, Xiaoyue Zhou, Chunmei Li, Renhong Liu, Wen Dai, Yihu Yang, Yanhui |
format |
Article |
author |
Wang, Qiaojuan Wang, Jianyue Rui, Wenjuan Yang, Dan Wan, Xiaoyue Zhou, Chunmei Li, Renhong Liu, Wen Dai, Yihu Yang, Yanhui |
author_sort |
Wang, Qiaojuan |
title |
Metal-carbonate interface promoted activity of Ag/MgCO₃ catalyst for aqueous-phase formaldehyde reforming into hydrogen |
title_short |
Metal-carbonate interface promoted activity of Ag/MgCO₃ catalyst for aqueous-phase formaldehyde reforming into hydrogen |
title_full |
Metal-carbonate interface promoted activity of Ag/MgCO₃ catalyst for aqueous-phase formaldehyde reforming into hydrogen |
title_fullStr |
Metal-carbonate interface promoted activity of Ag/MgCO₃ catalyst for aqueous-phase formaldehyde reforming into hydrogen |
title_full_unstemmed |
Metal-carbonate interface promoted activity of Ag/MgCO₃ catalyst for aqueous-phase formaldehyde reforming into hydrogen |
title_sort |
metal-carbonate interface promoted activity of ag/mgco₃ catalyst for aqueous-phase formaldehyde reforming into hydrogen |
publishDate |
2023 |
url |
https://hdl.handle.net/10356/170666 |
_version_ |
1779156367046606848 |