Modified Ni-carbonate interfaces for enhanced CO₂ methanation activity: tuned reaction pathway and reconstructed surface carbonates

A Ni/Zr-La2O2CO3 catalyst with interfaces between Ni metal and Zr-modified carbonate support was used for atmospheric CO2 methanation reaction, exhibiting 81% conversion and 99.6% CH4 selectivity at 300 °C. The Zr4+ ions incorporated in La2O2CO3 lattices properly strengthened the Ni-carbonate intera...

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Main Authors: Shen, Xuqiang, Wang, Zizhou, Wang, Qiaojuan, Tumurbaatar, Chantsalmaa, Bold, Tungalagtamir, Liu, Wen, Dai, Yihu, Tang, Yongming, Yang, Yanhui
Other Authors: School of Chemical and Biomedical Engineering
Format: Journal Article
Language:English
Published: 2022
Subjects:
Online Access:https://hdl.handle.net/10356/163924
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author Shen, Xuqiang
Wang, Zizhou
Wang, Qiaojuan
Tumurbaatar, Chantsalmaa
Bold, Tungalagtamir
Liu, Wen
Dai, Yihu
Tang, Yongming
Yang, Yanhui
author2 School of Chemical and Biomedical Engineering
author_facet School of Chemical and Biomedical Engineering
Shen, Xuqiang
Wang, Zizhou
Wang, Qiaojuan
Tumurbaatar, Chantsalmaa
Bold, Tungalagtamir
Liu, Wen
Dai, Yihu
Tang, Yongming
Yang, Yanhui
author_sort Shen, Xuqiang
collection NTU
description A Ni/Zr-La2O2CO3 catalyst with interfaces between Ni metal and Zr-modified carbonate support was used for atmospheric CO2 methanation reaction, exhibiting 81% conversion and 99.6% CH4 selectivity at 300 °C. The Zr4+ ions incorporated in La2O2CO3 lattices properly strengthened the Ni-carbonate interaction for enhancing the Ni dispersion and hydrogen activation ability of the catalyst. The Zr-modification could also tune the surface basic property for promoting the adsorptive dissociation of CO2. In-situ DRIFT spectra demonstrated that only the hydrogenation reaction pathway of formate intermediates was proceeded in Ni/La2O2CO3-catalyzed CO2 methanation. As a contrast, the hydrogenation pathways of CO and formate intermediates with relatively high activity were co-existed at the modified Ni-Zr-La2O2CO3 interfaces. Furthermore, the isotopic data evidenced that dynamic reconstruction and interconversion of the surface carbonate species occurred in the reaction, which might contribute to the key steps of CO2 dissociation and intermediates transformation.
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spelling ntu-10356/1639242022-12-22T03:03:38Z Modified Ni-carbonate interfaces for enhanced CO₂ methanation activity: tuned reaction pathway and reconstructed surface carbonates Shen, Xuqiang Wang, Zizhou Wang, Qiaojuan Tumurbaatar, Chantsalmaa Bold, Tungalagtamir Liu, Wen Dai, Yihu Tang, Yongming Yang, Yanhui School of Chemical and Biomedical Engineering Engineering::Chemical engineering Heterogeneous Catalysis Ni Catalyst A Ni/Zr-La2O2CO3 catalyst with interfaces between Ni metal and Zr-modified carbonate support was used for atmospheric CO2 methanation reaction, exhibiting 81% conversion and 99.6% CH4 selectivity at 300 °C. The Zr4+ ions incorporated in La2O2CO3 lattices properly strengthened the Ni-carbonate interaction for enhancing the Ni dispersion and hydrogen activation ability of the catalyst. The Zr-modification could also tune the surface basic property for promoting the adsorptive dissociation of CO2. In-situ DRIFT spectra demonstrated that only the hydrogenation reaction pathway of formate intermediates was proceeded in Ni/La2O2CO3-catalyzed CO2 methanation. As a contrast, the hydrogenation pathways of CO and formate intermediates with relatively high activity were co-existed at the modified Ni-Zr-La2O2CO3 interfaces. Furthermore, the isotopic data evidenced that dynamic reconstruction and interconversion of the surface carbonate species occurred in the reaction, which might contribute to the key steps of CO2 dissociation and intermediates transformation. We thank National Natural Science Foundation of China (22178161) and National Key R&D Program of China (2018YFE0122600) for financial support. 2022-12-22T03:03:38Z 2022-12-22T03:03:38Z 2022 Journal Article Shen, X., Wang, Z., Wang, Q., Tumurbaatar, C., Bold, T., Liu, W., Dai, Y., Tang, Y. & Yang, Y. (2022). Modified Ni-carbonate interfaces for enhanced CO₂ methanation activity: tuned reaction pathway and reconstructed surface carbonates. Journal of Catalysis, 413, 48-58. https://dx.doi.org/10.1016/j.jcat.2022.06.001 0021-9517 https://hdl.handle.net/10356/163924 10.1016/j.jcat.2022.06.001 2-s2.0-85132337577 413 48 58 en Journal of Catalysis © 2022 Elsevier Inc. All rights reserved.
spellingShingle Engineering::Chemical engineering
Heterogeneous Catalysis
Ni Catalyst
Shen, Xuqiang
Wang, Zizhou
Wang, Qiaojuan
Tumurbaatar, Chantsalmaa
Bold, Tungalagtamir
Liu, Wen
Dai, Yihu
Tang, Yongming
Yang, Yanhui
Modified Ni-carbonate interfaces for enhanced CO₂ methanation activity: tuned reaction pathway and reconstructed surface carbonates
title Modified Ni-carbonate interfaces for enhanced CO₂ methanation activity: tuned reaction pathway and reconstructed surface carbonates
title_full Modified Ni-carbonate interfaces for enhanced CO₂ methanation activity: tuned reaction pathway and reconstructed surface carbonates
title_fullStr Modified Ni-carbonate interfaces for enhanced CO₂ methanation activity: tuned reaction pathway and reconstructed surface carbonates
title_full_unstemmed Modified Ni-carbonate interfaces for enhanced CO₂ methanation activity: tuned reaction pathway and reconstructed surface carbonates
title_short Modified Ni-carbonate interfaces for enhanced CO₂ methanation activity: tuned reaction pathway and reconstructed surface carbonates
title_sort modified ni carbonate interfaces for enhanced co₂ methanation activity tuned reaction pathway and reconstructed surface carbonates
topic Engineering::Chemical engineering
Heterogeneous Catalysis
Ni Catalyst
url https://hdl.handle.net/10356/163924
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