Stepwise and Controllable Synthesis of Mesoporous Heterotrimetallic Catalysts Based on Predesigned Al4Ln4 Metallocycles

Abstract The motivation for making heterometallic compounds stemmed from their emergent synergistic properties and enhanced capabilities for applications. However, the atomically precisely controlled synthesis of heterometallic compounds remains a daunting challenge of the complications that arise w...

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Main Authors: Dan Luo, Chen‐Hui Liu, Yi‐Bo Chen, San‐Tai Wang, Wei‐Hui Fang, Jian Zhang
Format: Article
Language:English
Published: Wiley 2024-01-01
Series:Advanced Science
Subjects:
Online Access:https://doi.org/10.1002/advs.202305833
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author Dan Luo
Chen‐Hui Liu
Yi‐Bo Chen
San‐Tai Wang
Wei‐Hui Fang
Jian Zhang
author_facet Dan Luo
Chen‐Hui Liu
Yi‐Bo Chen
San‐Tai Wang
Wei‐Hui Fang
Jian Zhang
author_sort Dan Luo
collection DOAJ
description Abstract The motivation for making heterometallic compounds stemmed from their emergent synergistic properties and enhanced capabilities for applications. However, the atomically precisely controlled synthesis of heterometallic compounds remains a daunting challenge of the complications that arise when applying several metals and linkers. Herein, a stepwise and controlled method is reported for the accurate addition of second and third metals to homometallic aluminum macrocycles based on the synergistic coordination and hard‐soft acid‐base theory. These heterometallic compounds showed a good Lewis acid catalytic effect, and the addition of hetero‐metals significantly improved the catalytic effect and rate, among that the conversion rate of compound AlOC‐133 reached 99.9% within half an hour. This method combines both the independent controllability of stepwise assembly with the universality of one‐step methods. Based on the large family of clusters, the establishment of this method paves the way for the controllable and customized molecular‐level synthesis of heterometallic materials and creates materials customized for preferential application.
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spelling doaj.art-7ade961cce5546568ff179f6d1326bf02024-01-13T04:23:06ZengWileyAdvanced Science2198-38442024-01-01112n/an/a10.1002/advs.202305833Stepwise and Controllable Synthesis of Mesoporous Heterotrimetallic Catalysts Based on Predesigned Al4Ln4 MetallocyclesDan Luo0Chen‐Hui Liu1Yi‐Bo Chen2San‐Tai Wang3Wei‐Hui Fang4Jian Zhang5State Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 P. R. ChinaState Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 P. R. ChinaState Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 P. R. ChinaState Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 P. R. ChinaState Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 P. R. ChinaState Key Laboratory of Structural Chemistry Fujian Institute of Research on the Structure of Matter Chinese Academy of Sciences Fuzhou Fujian 350002 P. R. ChinaAbstract The motivation for making heterometallic compounds stemmed from their emergent synergistic properties and enhanced capabilities for applications. However, the atomically precisely controlled synthesis of heterometallic compounds remains a daunting challenge of the complications that arise when applying several metals and linkers. Herein, a stepwise and controlled method is reported for the accurate addition of second and third metals to homometallic aluminum macrocycles based on the synergistic coordination and hard‐soft acid‐base theory. These heterometallic compounds showed a good Lewis acid catalytic effect, and the addition of hetero‐metals significantly improved the catalytic effect and rate, among that the conversion rate of compound AlOC‐133 reached 99.9% within half an hour. This method combines both the independent controllability of stepwise assembly with the universality of one‐step methods. Based on the large family of clusters, the establishment of this method paves the way for the controllable and customized molecular‐level synthesis of heterometallic materials and creates materials customized for preferential application.https://doi.org/10.1002/advs.202305833catalysiscompoundscoordination assemblycyanosilylationheterometallic materialsporous frameworks
spellingShingle Dan Luo
Chen‐Hui Liu
Yi‐Bo Chen
San‐Tai Wang
Wei‐Hui Fang
Jian Zhang
Stepwise and Controllable Synthesis of Mesoporous Heterotrimetallic Catalysts Based on Predesigned Al4Ln4 Metallocycles
Advanced Science
catalysis
compounds
coordination assembly
cyanosilylation
heterometallic materials
porous frameworks
title Stepwise and Controllable Synthesis of Mesoporous Heterotrimetallic Catalysts Based on Predesigned Al4Ln4 Metallocycles
title_full Stepwise and Controllable Synthesis of Mesoporous Heterotrimetallic Catalysts Based on Predesigned Al4Ln4 Metallocycles
title_fullStr Stepwise and Controllable Synthesis of Mesoporous Heterotrimetallic Catalysts Based on Predesigned Al4Ln4 Metallocycles
title_full_unstemmed Stepwise and Controllable Synthesis of Mesoporous Heterotrimetallic Catalysts Based on Predesigned Al4Ln4 Metallocycles
title_short Stepwise and Controllable Synthesis of Mesoporous Heterotrimetallic Catalysts Based on Predesigned Al4Ln4 Metallocycles
title_sort stepwise and controllable synthesis of mesoporous heterotrimetallic catalysts based on predesigned al4ln4 metallocycles
topic catalysis
compounds
coordination assembly
cyanosilylation
heterometallic materials
porous frameworks
url https://doi.org/10.1002/advs.202305833
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