Spatial segregation of catalytic sites within Pd doped H-ZSM-5 for fatty acid hydrodeoxygenation to alkanes

Spatial control over features within multifunctional catalysts can unlock efficient one-pot cascade reactions, which are themselves a pathway to aviation biofuels via hydrodeoxygenation. A synthesis strategy that encompasses spatial orthogonality, i.e., one in which different catalytic species are deposited exclusively within discrete locations of a support architecture, is one solution that permits control over potential interactions between different sites and the cascade process. Here, we report a Pd doped hierarchical zeolite, in which Pd nanoparticles are selectively deposited within the mesopores, while acidity is retained solely within the micropores of ZSM-5. This spatial segregation facilitates hydrodeoxygenation while suppressing undesirable decarboxylation and decarbonation, yielding significant enhancements in activity (30.6 vs 3.6 mol<sub>dodecane</sub> mol<sub>Pd</sub><sup>-1</sup> h<sup>-1</sup>) and selectivity (C<sub>12</sub>:C<sub>11</sub> 5.2 vs 1.9) relative to a conventionally prepared counterpart (via wet impregnation). Herein, multifunctional material design can realise efficient fatty acid hydrodeoxygenation, thus advancing the field and inspiring future developments in rationalised catalyst design.

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Publication Details

Journal
Nature Communications
Published
2024-09-04
DOI
https://doi.org/10.1038/s41467-024-51925-2
Citations
39
Primary Topic
Catalysis and Hydrodesulfurization Studies
Type
article
Field-Weighted Citation Impact
8.29

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article

Spatial segregation of catalytic sites within Pd doped H-ZSM-5 for fatty acid hydrodeoxygenation to alkanes

Xiaolei Fan, Nicole Hondow, Carmine D’Agostino, Min Hu et al.
39 citations
Nature Communications
Catalysis and Hydrodesulfurization Studies
8.29
article

Spatial segregation of catalytic sites within Pd doped H-ZSM-5 for fatty acid hydrodeoxygenation to alkanes

Xiaolei Fan, Nicole Hondow, Carmine D’Agostino, Min Hu, Constantinos Theodoropoulos, Christopher M. A. Parlett, Dario Luis Fernandez Ainaga, Boya Qiu, Yilai Jiao, Ushna Khalid, Xiaoxia Ou, Ben F. Spencer, Xiangli Zhong, Shengzhe Ding, Yani Peng
article en
39 citations

Abstract

Spatial control over features within multifunctional catalysts can unlock efficient one-pot cascade reactions, which are themselves a pathway to aviation biofuels via hydrodeoxygenation. A synthesis strategy that encompasses spatial orthogonality, i.e., one in which different catalytic species are deposited exclusively within discrete locations of a support architecture, is one solution that permits control over potential interactions between different sites and the cascade process. Here, we report a Pd doped hierarchical zeolite, in which Pd nanoparticles are selectively deposited within the mesopores, while acidity is retained solely within the micropores of ZSM-5. This spatial segregation facilitates hydrodeoxygenation while suppressing undesirable decarboxylation and decarbonation, yielding significant enhancements in activity (30.6 vs 3.6 mol<sub>dodecane</sub> mol<sub>Pd</sub><sup>-1</sup> h<sup>-1</sup>) and selectivity (C<sub>12</sub>:C<sub>11</sub> 5.2 vs 1.9) relative to a conventionally prepared counterpart (via wet impregnation). Herein, multifunctional material design can realise efficient fatty acid hydrodeoxygenation, thus advancing the field and inspiring future developments in rationalised catalyst design.

Nature CommunicationsVol. 15(1)
University of Leeds (GB), University of Nottingham Ningbo China (CN), Wenzhou University (CN), Chinese Academy of Sciences (CN), Diamond Light Source (GB), University of Manchester (GB), Henry Royce Institute (GB), Research Complex at Harwell (GB), Beijing Chemical Industry Research Institute (China) (CN), Wenzhou Institute of Industrial Science (CN), University of Bologna (IT)
University of Manchester, European Commission, National Natural Science Foundation of China, China Scholarship Council, UK Catalysis Hub, Punjab Educational Endowment Fund, Engineering and Physical Sciences Research Council, Natural Science Foundation of Zhejiang Province
Openalex Percentile: Top 1%
Catalysis and Hydrodesulfurization Studies
8.29
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