Mg-stabilized subnanometer Rh particles in zeolite Beta as highly efficient catalysts for selective hydrogenation
Nanoparticles are of interest in heterogeneous catalysis because of their excellent activity associated with atoms in a low coordination environment. However, their high reactivity becomes a drawback where selectivity is desired, compounded by their propensity towards agglomeration. Here, we show th...
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sg-ntu-dr.10356-1639232022-12-22T02:47:48Z Mg-stabilized subnanometer Rh particles in zeolite Beta as highly efficient catalysts for selective hydrogenation Zhang, Hongwei Zhong, Lixiang Bin Samsudin, Ismail Okumura, Kazu Tan, Hui-Ru Li, Shuzhou Jaenicke, Stephan Chuah, Gaik-Khuan School of Materials Science and Engineering Science::Chemistry Rhodium Subnanometric Clusters Nanoparticles are of interest in heterogeneous catalysis because of their excellent activity associated with atoms in a low coordination environment. However, their high reactivity becomes a drawback where selectivity is desired, compounded by their propensity towards agglomeration. Here, we show that stable subnanometric Rh particles can be prepared in a Mg-doped zeolite Beta based on the electrostatic interaction of the negatively charged zeolitic framework and the Rh3+ precursor. The Mg ions are incorporated into the zeolite framework whereas the Rh is located in the channels adjacent to the Mg. With only 0.27 and 0.5 wt% Mg and Rh, respectively, the Rh/Mg-Beta catalysts were highly active with > 94 % selectivity for the hydrogenation of phenol to cyclohexanone, an important intermediate for the production of Nylon. Key to the selectivity is the formation of the C=O double bond early in the reaction sequence, aided by the basicity of the Mg-Beta support. H. Zhang thanks NUS for a research fellowship from FOS ARC Tier 1 grant R-143-000-B07-114. Financial support under FOS ARC Tier 1 grants R-143-000-B07-114 and R-143-000-667-114 and KFUPM-NUS Collaborative Agreement R-143-003-617-597 is gratefully acknowledged. 2022-12-22T02:47:47Z 2022-12-22T02:47:47Z 2022 Journal Article Zhang, H., Zhong, L., Bin Samsudin, I., Okumura, K., Tan, H., Li, S., Jaenicke, S. & Chuah, G. (2022). Mg-stabilized subnanometer Rh particles in zeolite Beta as highly efficient catalysts for selective hydrogenation. Journal of Catalysis, 405, 489-498. https://dx.doi.org/10.1016/j.jcat.2021.11.026 0021-9517 https://hdl.handle.net/10356/163923 10.1016/j.jcat.2021.11.026 2-s2.0-85120775566 405 489 498 en R-143-000-B07-114 R-143-000-667-114 R-143-003-617-597 Journal of Catalysis © 2021 Elsevier Inc. All rights reserved. |
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Science::Chemistry Rhodium Subnanometric Clusters Zhang, Hongwei Zhong, Lixiang Bin Samsudin, Ismail Okumura, Kazu Tan, Hui-Ru Li, Shuzhou Jaenicke, Stephan Chuah, Gaik-Khuan Mg-stabilized subnanometer Rh particles in zeolite Beta as highly efficient catalysts for selective hydrogenation |
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Nanoparticles are of interest in heterogeneous catalysis because of their excellent activity associated with atoms in a low coordination environment. However, their high reactivity becomes a drawback where selectivity is desired, compounded by their propensity towards agglomeration. Here, we show that stable subnanometric Rh particles can be prepared in a Mg-doped zeolite Beta based on the electrostatic interaction of the negatively charged zeolitic framework and the Rh3+ precursor. The Mg ions are incorporated into the zeolite framework whereas the Rh is located in the channels adjacent to the Mg. With only 0.27 and 0.5 wt% Mg and Rh, respectively, the Rh/Mg-Beta catalysts were highly active with > 94 % selectivity for the hydrogenation of phenol to cyclohexanone, an important intermediate for the production of Nylon. Key to the selectivity is the formation of the C=O double bond early in the reaction sequence, aided by the basicity of the Mg-Beta support. |
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School of Materials Science and Engineering |
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School of Materials Science and Engineering Zhang, Hongwei Zhong, Lixiang Bin Samsudin, Ismail Okumura, Kazu Tan, Hui-Ru Li, Shuzhou Jaenicke, Stephan Chuah, Gaik-Khuan |
format |
Article |
author |
Zhang, Hongwei Zhong, Lixiang Bin Samsudin, Ismail Okumura, Kazu Tan, Hui-Ru Li, Shuzhou Jaenicke, Stephan Chuah, Gaik-Khuan |
author_sort |
Zhang, Hongwei |
title |
Mg-stabilized subnanometer Rh particles in zeolite Beta as highly efficient catalysts for selective hydrogenation |
title_short |
Mg-stabilized subnanometer Rh particles in zeolite Beta as highly efficient catalysts for selective hydrogenation |
title_full |
Mg-stabilized subnanometer Rh particles in zeolite Beta as highly efficient catalysts for selective hydrogenation |
title_fullStr |
Mg-stabilized subnanometer Rh particles in zeolite Beta as highly efficient catalysts for selective hydrogenation |
title_full_unstemmed |
Mg-stabilized subnanometer Rh particles in zeolite Beta as highly efficient catalysts for selective hydrogenation |
title_sort |
mg-stabilized subnanometer rh particles in zeolite beta as highly efficient catalysts for selective hydrogenation |
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2022 |
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https://hdl.handle.net/10356/163923 |
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1753801110487826432 |