Encapsulation of Pt species into MFI zeolite with tunable acid sites boosts reductive amination towards tertiary amines

IF 3.5 3区工程技术 Q2 ENGINEERING, CHEMICAL

AIChE Journal Pub Date : 2024-12-20 DOI:10.1002/aic.18710

Zhuo Xiong, Biao Meng, Cailing Chen, Xiaoling Liu, Chao Wu, Yue Wu, Meng Xu, Hongzhong Xu, Yihu Dai, Yu Han, Yu Zhou, Shibo Xi, Jun Wang

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引用次数: 0

Abstract

Noble metal-catalyzed reductive amination of carbonyl compounds using molecular hydrogen is a promising green route for amine synthesis, but a challenge remains to boost the atomic efficiency of noble metal species. Herein, MFI zeolite encapsulated Pt species with tunable Si/Al ratios were synthesized to allow the formation of Pt nanoparticles (NPs) with almost the same loading amount, particle size, and electronic state. Confining Pt NPs allows the spatial satisfaction for the synergy of metal centers and acid sites, and Pt@ZSM-5(100) with a moderate Si/Al ratio performed high efficiency in the conversion of carbonyl compounds and boosted high TOF of 23,409 h⁻¹ in reductive amination of benzaldehyde. Combined with structure refinement, x-ray absorption fine structure (XAFS), in situ Fourier transforms infrared (FTIR) spectroscopy, and theoretical calculation, the study indicated that modulating the Si/Al ratio enables the fine rationalization of the microenvironment. The moderate Si/Al ratio causes suitable acid intensity that significantly contributes to the carbonyl compound activation and product desorption.

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来源期刊

AIChE Journal 工程技术-工程：化工

CiteScore

7.10

自引率

10.80%

发文量

411

审稿时长

3.6 months

期刊介绍： The AIChE Journal is the premier research monthly in chemical engineering and related fields. This peer-reviewed and broad-based journal reports on the most important and latest technological advances in core areas of chemical engineering as well as in other relevant engineering disciplines. To keep abreast with the progressive outlook of the profession, the Journal has been expanding the scope of its editorial contents to include such fast developing areas as biotechnology, electrochemical engineering, and environmental engineering. The AIChE Journal is indeed the global communications vehicle for the world-renowned researchers to exchange top-notch research findings with one another. Subscribing to the AIChE Journal is like having immediate access to nine topical journals in the field. Articles are categorized according to the following topical areas: Biomolecular Engineering, Bioengineering, Biochemicals, Biofuels, and Food Inorganic Materials: Synthesis and Processing Particle Technology and Fluidization Process Systems Engineering Reaction Engineering, Kinetics and Catalysis Separations: Materials, Devices and Processes Soft Materials: Synthesis, Processing and Products Thermodynamics and Molecular-Scale Phenomena Transport Phenomena and Fluid Mechanics.