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Nano Research 2023, 16(8): 11334-11341 https://doi.org/10.1007/s12274-023-5750-7
Research Article | Issue | Published: 20 May 2023

Dynamically modulated synthesis of hollow metal-organic frameworks for selective hydrogenation reactions

Show Author's Information Liyun Xiao1,  Chuanqi Cheng2,  Zhixi Li1,  Chaoyang Zheng1,  Jing Du1,  Meina Song1,  Yue Wan1,  Shaopeng Li1,  Guo Jun3,  Meiting Zhao1( )
Department of Chemistry, Institute of Molecular Aggregation Science, Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Tianjin University, Tianjin 300072, China
Institute of New Energy Materials, School of Materials Science and Engineering, Tianjin University, Tianjin 300072, China
State Key Laboratory of Separation Membranes and Membrane Processes, School of Chemistry, Tiangong University, Tianjin 300387, China
Keywords:
metal-organic frameworks (MOFs), selective hydrogenation, nitrobenzene, hollow structure, dynamically modulated synthesis
Topics:
Organic frameworks
Cite this article:
Xiao L, Cheng C, Li Z, et al. Dynamically modulated synthesis of hollow metal-organic frameworks for selective hydrogenation reactions. Nano Research, 2023, 16(8): 11334-11341. https://doi.org/10.1007/s12274-023-5750-7
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Abstract Full text Electronic supplementary material About this article

Hollow metal-organic frameworks (MOFs) have attracted increasing attention in the field of catalysis in recent years due to their unique cavity structure with fast mass-diffusion rates and easily accessible active sites. Here, we report the use of dynamic modulators, which are formed by the in-situ imine condensation reaction of 4-aminobenzoic acid and 4-formylbenzoic acid, to regulate the growth of MOFs to synthesize well-defined hollow thioether functionalized UiO-67 (denoted as H-UiO-67-S) single crystals. After supporting Pd nanoparticles, the designed catalysts Pd@H-UiO-67-S show excellent conversion (> 99.9%), selectivity (> 99.9%), and stability (10 cycles) in the selective hydrogenation of nitrobenzenes with other reducible groups. Density functional theory calculations and the experimental results reveal that Pd nanoparticles not only selectively adsorb the nitro-groups on nitrobenzene, but also restrict the adsorption of the aniline product, due to the interaction of thioether with Pd in the confined pores of H-UiO-67-S, finally result in a significant increase in selectivity of nitro-hydrogenation.


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Electronic supplementary material
About this article

Dynamically modulated synthesis of hollow metal-organic frameworks for selective hydrogenation reactions

Show Author's information Liyun Xiao1, Chuanqi Cheng2, Zhixi Li1, Chaoyang Zheng1, Jing Du1, Meina Song1, Yue Wan1, Shaopeng Li1, Guo Jun3, Meiting Zhao1( )
Department of Chemistry, Institute of Molecular Aggregation Science, Tianjin Key Laboratory of Molecular Optoelectronic Sciences, Tianjin University, Tianjin 300072, China
Institute of New Energy Materials, School of Materials Science and Engineering, Tianjin University, Tianjin 300072, China
State Key Laboratory of Separation Membranes and Membrane Processes, School of Chemistry, Tiangong University, Tianjin 300387, China

Abstract

Hollow metal-organic frameworks (MOFs) have attracted increasing attention in the field of catalysis in recent years due to their unique cavity structure with fast mass-diffusion rates and easily accessible active sites. Here, we report the use of dynamic modulators, which are formed by the in-situ imine condensation reaction of 4-aminobenzoic acid and 4-formylbenzoic acid, to regulate the growth of MOFs to synthesize well-defined hollow thioether functionalized UiO-67 (denoted as H-UiO-67-S) single crystals. After supporting Pd nanoparticles, the designed catalysts Pd@H-UiO-67-S show excellent conversion (> 99.9%), selectivity (> 99.9%), and stability (10 cycles) in the selective hydrogenation of nitrobenzenes with other reducible groups. Density functional theory calculations and the experimental results reveal that Pd nanoparticles not only selectively adsorb the nitro-groups on nitrobenzene, but also restrict the adsorption of the aniline product, due to the interaction of thioether with Pd in the confined pores of H-UiO-67-S, finally result in a significant increase in selectivity of nitro-hydrogenation.

Keywords: metal-organic frameworks (MOFs), selective hydrogenation, nitrobenzene, hollow structure, dynamically modulated synthesis

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Publication history
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Acknowledgements

Publication history

Received: 03 March 2023
Revised: 09 April 2023
Accepted: 16 April 2023
Published: 20 May 2023
Issue date: August 2023

Copyright

© Tsinghua University Press 2023

Acknowledgements

Acknowledgements

The authors acknowledge financial support from the National Natural Science Foundation of China (Nos. 21905195, M. T. Z. and 22103055, J. G.), Natural Science Foundation of Tianjin City (No. 20JCYBJC00800, M. T. Z.), Science and Technology Plans of Tianjin (No. 21ZYJDJC00050, J. G.), and PEIYANG Young Scholars Program of Tianjin University (No. 2020XRX-0023, M. T. Z.).

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