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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Main Authors: Zhang, Hongwei, Zhong, Lixiang, Bin Samsudin, Ismail, Okumura, Kazu, Tan, Hui-Ru, Li, Shuzhou, Jaenicke, Stephan, Chuah, Gaik-Khuan
Other Authors: School of Materials Science and Engineering
Format: Article
Language:English
Published: 2022
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Online Access:https://hdl.handle.net/10356/163923
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Institution: Nanyang Technological University
Language: English
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spelling 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.
institution Nanyang Technological University
building NTU Library
continent Asia
country Singapore
Singapore
content_provider NTU Library
collection DR-NTU
language English
topic Science::Chemistry
Rhodium
Subnanometric Clusters
spellingShingle 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
description 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.
author2 School of Materials Science and Engineering
author_facet 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
publishDate 2022
url https://hdl.handle.net/10356/163923
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