Volume 64, Issue 24 e202424690

Research Article

Structurally Engineering Multi-Shell Hollow Zeolite Single Crystals via Defect-Directed Oriented-Kinetics Transformation and Their Heterostructures for Hydrodeoxygenation Reaction

Guangrui Chen

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P.R. China

International Center of Future Science, Jilin University, Changchun, 130012 P.R. China

Both authors contributed equally to this work.

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Peihong She,

Peihong She

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P.R. China

International Center of Future Science, Jilin University, Changchun, 130012 P.R. China

Both authors contributed equally to this work.

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Ji Han,

Ji Han

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P.R. China

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Junyan Li,

Junyan Li

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P.R. China

Center for High-resolution Electron Microscopy (CℏEM), School of Physical Science and Technology, ShanghaiTech University, Shanghai, 201210 P.R. China

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Ge Tian,

Ge Tian

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P.R. China

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Yuanbo Sun,

Yuanbo Sun

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P.R. China

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Yanjing Gao,

Yanjing Gao

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P.R. China

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Guoju Yang,

Guoju Yang

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P.R. China

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Zhenheng Diao,

Zhenheng Diao

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P.R. China

School of Chemical Engineering, Changchun University of Technology, Changchun, 130012 P.R. China

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Buyuan Guan,

Corresponding Author

Buyuan Guan

[email protected]

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P.R. China

International Center of Future Science, Jilin University, Changchun, 130012 P.R. China

E-mail: [email protected]; [email protected]

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Jihong Yu,

Corresponding Author

Jihong Yu

[email protected]

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P.R. China

International Center of Future Science, Jilin University, Changchun, 130012 P.R. China

E-mail: [email protected]; [email protected]

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Guangrui Chen,

Guangrui Chen

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P.R. China

International Center of Future Science, Jilin University, Changchun, 130012 P.R. China

Both authors contributed equally to this work.

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Peihong She,

Peihong She

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P.R. China

International Center of Future Science, Jilin University, Changchun, 130012 P.R. China

Both authors contributed equally to this work.

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Ji Han,

Ji Han

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P.R. China

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Junyan Li,

Junyan Li

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P.R. China

Center for High-resolution Electron Microscopy (CℏEM), School of Physical Science and Technology, ShanghaiTech University, Shanghai, 201210 P.R. China

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Ge Tian,

Ge Tian

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P.R. China

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Yuanbo Sun,

Yuanbo Sun

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P.R. China

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Yanjing Gao,

Yanjing Gao

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P.R. China

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Guoju Yang,

Guoju Yang

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P.R. China

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Zhenheng Diao,

Zhenheng Diao

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P.R. China

School of Chemical Engineering, Changchun University of Technology, Changchun, 130012 P.R. China

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Buyuan Guan,

Corresponding Author

Buyuan Guan

[email protected]

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P.R. China

International Center of Future Science, Jilin University, Changchun, 130012 P.R. China

E-mail: [email protected]; [email protected]

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Jihong Yu,

Corresponding Author

Jihong Yu

[email protected]

State Key Laboratory of Inorganic Synthesis and Preparative Chemistry, College of Chemistry, Jilin University, Changchun, 130012 P.R. China

International Center of Future Science, Jilin University, Changchun, 130012 P.R. China

E-mail: [email protected]; [email protected]

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First published: 14 April 2025

https://doi.org/10.1002/anie.202424690

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Graphical Abstract

A defect-directed oriented-kinetics transformation strategy is developed to prepare multi-shell hollow aluminosilicate ZSM-5 zeolite (MFI) crystals with single-crystalline feature, hierarchical macro-/mesoporosity, controllable shell number, and high structural stability. The resultant multi-shell hollow Ni-loaded ZSM-5 zeolite catalysts exhibit significantly enhanced catalytic activity in the hydrodeoxygenation of stearic acid into liquid fuels.

Abstract

Single-crystalline multi-shell hollow porous materials with high compartment capacity, large active surface area, and superior structural stability are expected to unlock tremendous potential across diverse critical applications. However, their synthetic methodology has not yet been well established. Here, we develop a defect-directed oriented-kinetics transformation approach to prepare multi-shell hollow aluminosilicate ZSM-5 zeolite (MFI) crystals with single-crystalline feature, hierarchical macro-/mesoporosity, controllable shell number, and high structural stability. The methodology lies in the creation of zeolite precursors consisting of multiple inhomogeneous layers with gradient-distributed defects along the [100] and [010] directions and irregularly discrete defects-rich regions along the [001] direction via continuous epitaxial growth. Subsequently, the locations with more defects could be preferentially etched to form voids or mesopores, meanwhile oriented recrystallization interconnects the nanoshells into a unified architecture along the [001] direction. Benefiting from the easily accessible bifunctional metal/acid sites and the capability for reactant accumulation, the resultant multi-shell hollow Ni-loaded zeolite catalysts show significantly enhanced catalytic activity in the hydrodeoxygenation of stearic acid into liquid fuels. The insight gained from this systematic study will facilitate the rational design and synthesis of diverse multi-shell hollow structured single-crystalline porous materials for a broad range of potential applications.

Conflict of Interests

The authors declare no conflict of interest.

Open Research

Data Availability Statement

The data that support the findings of this study are available from the corresponding author upon reasonable request.

Supporting Information

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Volume64, Issue24

June 10, 2025

e202424690

Structurally Engineering Multi-Shell Hollow Zeolite Single Crystals via Defect-Directed Oriented-Kinetics Transformation and Their Heterostructures for Hydrodeoxygenation Reaction

Graphical Abstract

Abstract

Conflict of Interests

Open Research

Data Availability Statement

Supporting Information

References

References

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Structurally Engineering Multi-Shell Hollow Zeolite Single Crystals via Defect-Directed Oriented-Kinetics Transformation and Their Heterostructures for Hydrodeoxygenation Reaction

Graphical Abstract

Abstract

Conflict of Interests

Open Research

Data Availability Statement

Supporting Information

References

References

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