Strong metal-support interaction for 2D materials: application in noble metal/TiB₂ heterointerfaces and their enhanced catalytic performance for formic acid dehydrogenation
Strong metal-support interaction (SMSI) is a phenomenon commonly observed on heterogeneous catalysts. Here, direct evidence of SMSI between noble metal and 2D TiB2 supports is reported. The temperature-induced TiB2 overlayers encapsulate the metal nanoparticles, resulting in core-shell nanostructure...
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sg-ntu-dr.10356-1607142022-08-01T07:08:16Z Strong metal-support interaction for 2D materials: application in noble metal/TiB₂ heterointerfaces and their enhanced catalytic performance for formic acid dehydrogenation Li, Renhong Liu, Zhiqi Trinh, Quang Thang Miao, Ziqiang Chen, Shuang Qian, Kaicheng Wong, Roong Jien Xi, Shibo Yan, Yong Borgna, Armando Liang, Shipan Wei, Tong Dai, Yihu Wang, Peng Tang, Yu Yan, Xiaoqing Choksi, Tej S. Liu, Wen School of Chemical and Biomedical Engineering Cambridge Centre for Advanced Research and Education Engineering::Chemical engineering Formic Acid Dehydrogenation Hydrogen Production Strong metal-support interaction (SMSI) is a phenomenon commonly observed on heterogeneous catalysts. Here, direct evidence of SMSI between noble metal and 2D TiB2 supports is reported. The temperature-induced TiB2 overlayers encapsulate the metal nanoparticles, resulting in core-shell nanostructures that are sintering-resistant with metal loadings as high as 12.0 wt%. The TiOx -terminated TiB2 surfaces are the active sites catalyzing the dehydrogenation of formic acid at room temperature. In contrast to the trade-off between stability and activity in conventional SMSI, TiB2 -based SMSI promotes catalytic activity and stability simultaneously. By optimizing the thickness and coverage of the overlayer, the Pt/TiB2 catalyst displays an outstanding hydrogen productivity of 13.8 mmol g-1 cat h-1 in 10.0 m aqueous solution without any additive or pH adjustment, with >99.9% selectivity toward CO2 and H2 . Theoretical studies suggest that the TiB2 overlayers are stabilized on different transition metals through an interplay between covalent and electrostatic interactions. Furthermore, the computationally determined trends in metal-TiB2 interactions are fully consistent with the experimental observations regarding the extent of SMSI on different transition metals. The present research introduces a new means to create thermally stable and catalytically active metal/support interfaces for scalable chemical and energy applications. National Research Foundation (NRF) The authors are grateful for financial supports from the National Natural Science Foundation of China (Nos. 21872123, 21902027, and U19B2003) and Zhejiang Provincial Natural Science Foundation of China (No. LY18B030007). T.S.C. and W.L. acknowledge funding from National Research Foundation of Singapore under its Campus for Research Excellence and Technological Enterprise (CREATE) programme. 2022-08-01T07:08:16Z 2022-08-01T07:08:16Z 2021 Journal Article Li, R., Liu, Z., Trinh, Q. T., Miao, Z., Chen, S., Qian, K., Wong, R. J., Xi, S., Yan, Y., Borgna, A., Liang, S., Wei, T., Dai, Y., Wang, P., Tang, Y., Yan, X., Choksi, T. S. & Liu, W. (2021). Strong metal-support interaction for 2D materials: application in noble metal/TiB₂ heterointerfaces and their enhanced catalytic performance for formic acid dehydrogenation. Advanced Materials, 33(32), 2101536-. https://dx.doi.org/10.1002/adma.202101536 0935-9648 https://hdl.handle.net/10356/160714 10.1002/adma.202101536 34216405 2-s2.0-85109170008 32 33 2101536 en Advanced Materials © 2021 Wiley-VCH GmbH. All rights reserved. |
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Engineering::Chemical engineering Formic Acid Dehydrogenation Hydrogen Production Li, Renhong Liu, Zhiqi Trinh, Quang Thang Miao, Ziqiang Chen, Shuang Qian, Kaicheng Wong, Roong Jien Xi, Shibo Yan, Yong Borgna, Armando Liang, Shipan Wei, Tong Dai, Yihu Wang, Peng Tang, Yu Yan, Xiaoqing Choksi, Tej S. Liu, Wen Strong metal-support interaction for 2D materials: application in noble metal/TiB₂ heterointerfaces and their enhanced catalytic performance for formic acid dehydrogenation |
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Strong metal-support interaction (SMSI) is a phenomenon commonly observed on heterogeneous catalysts. Here, direct evidence of SMSI between noble metal and 2D TiB2 supports is reported. The temperature-induced TiB2 overlayers encapsulate the metal nanoparticles, resulting in core-shell nanostructures that are sintering-resistant with metal loadings as high as 12.0 wt%. The TiOx -terminated TiB2 surfaces are the active sites catalyzing the dehydrogenation of formic acid at room temperature. In contrast to the trade-off between stability and activity in conventional SMSI, TiB2 -based SMSI promotes catalytic activity and stability simultaneously. By optimizing the thickness and coverage of the overlayer, the Pt/TiB2 catalyst displays an outstanding hydrogen productivity of 13.8 mmol g-1 cat h-1 in 10.0 m aqueous solution without any additive or pH adjustment, with >99.9% selectivity toward CO2 and H2 . Theoretical studies suggest that the TiB2 overlayers are stabilized on different transition metals through an interplay between covalent and electrostatic interactions. Furthermore, the computationally determined trends in metal-TiB2 interactions are fully consistent with the experimental observations regarding the extent of SMSI on different transition metals. The present research introduces a new means to create thermally stable and catalytically active metal/support interfaces for scalable chemical and energy applications. |
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School of Chemical and Biomedical Engineering |
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School of Chemical and Biomedical Engineering Li, Renhong Liu, Zhiqi Trinh, Quang Thang Miao, Ziqiang Chen, Shuang Qian, Kaicheng Wong, Roong Jien Xi, Shibo Yan, Yong Borgna, Armando Liang, Shipan Wei, Tong Dai, Yihu Wang, Peng Tang, Yu Yan, Xiaoqing Choksi, Tej S. Liu, Wen |
format |
Article |
author |
Li, Renhong Liu, Zhiqi Trinh, Quang Thang Miao, Ziqiang Chen, Shuang Qian, Kaicheng Wong, Roong Jien Xi, Shibo Yan, Yong Borgna, Armando Liang, Shipan Wei, Tong Dai, Yihu Wang, Peng Tang, Yu Yan, Xiaoqing Choksi, Tej S. Liu, Wen |
author_sort |
Li, Renhong |
title |
Strong metal-support interaction for 2D materials: application in noble metal/TiB₂ heterointerfaces and their enhanced catalytic performance for formic acid dehydrogenation |
title_short |
Strong metal-support interaction for 2D materials: application in noble metal/TiB₂ heterointerfaces and their enhanced catalytic performance for formic acid dehydrogenation |
title_full |
Strong metal-support interaction for 2D materials: application in noble metal/TiB₂ heterointerfaces and their enhanced catalytic performance for formic acid dehydrogenation |
title_fullStr |
Strong metal-support interaction for 2D materials: application in noble metal/TiB₂ heterointerfaces and their enhanced catalytic performance for formic acid dehydrogenation |
title_full_unstemmed |
Strong metal-support interaction for 2D materials: application in noble metal/TiB₂ heterointerfaces and their enhanced catalytic performance for formic acid dehydrogenation |
title_sort |
strong metal-support interaction for 2d materials: application in noble metal/tib₂ heterointerfaces and their enhanced catalytic performance for formic acid dehydrogenation |
publishDate |
2022 |
url |
https://hdl.handle.net/10356/160714 |
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1743119477330935808 |