Investigating size-dependent selectivity in benzaldehyde reductive amination via Ni nanoparticles
Selectivity control is a fundamental focus in catalysis chemistry, as it directly reflects the efficiency and efficacy of catalytic processes. While catalysis often involves intricate and cascade reaction steps using nanoparticle (NP) catalysts, the mechanism behind the size effect of nanoparticles...
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Elsevier
2025-06-01
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| Series: | Materials Today Catalysis |
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| Online Access: | http://www.sciencedirect.com/science/article/pii/S2949754X25000134 |
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| author | Yunong Li Ching Kit Tommy Wun Tianxiang Chen Tsz Woon Benedict Lo |
| author_facet | Yunong Li Ching Kit Tommy Wun Tianxiang Chen Tsz Woon Benedict Lo |
| author_sort | Yunong Li |
| collection | DOAJ |
| description | Selectivity control is a fundamental focus in catalysis chemistry, as it directly reflects the efficiency and efficacy of catalytic processes. While catalysis often involves intricate and cascade reaction steps using nanoparticle (NP) catalysts, the mechanism behind the size effect of nanoparticles on product selectivity has not been fully explored. We herein prepared a series of Ni-containing zeolitic catalysts in which the Ni NPs are uniformly supported on the mesopores and outer surfaces of H-ZSM-5 zeolites. The dynamic formation of Ni NPs from highly dispersed Ni precursors was monitored using transmission electron microscopy, in-situ X-ray pair distribution function, and in-situ X-ray absorption fine structure analysis. The metal nanoparticle size was carefully controlled between 3.72(5) nm and 11.91(7) by controlling the reduction temperature. We evaluated the catalytic performance of Ni NPs using the reductive amination of benzaldehyde in batch reactors at low temperatures. This reaction inherently favors the formation of a series of products, suffering highly from selectivity issues. Our results revealed a size-dependent behavior in reaction efficiency, with the catalyst achieving the highest catalytic activity (93 % selectivity in primary amine) at a particle size of 5.62(3) nm. This optimal performance is attributed to a balanced interplay between hydrogenation and amination capabilities. These findings highlight the intricate relationship between nanoparticle size and catalytic performance, emphasizing the necessity for precise optimization in catalyst design to enhance selectivity and sustainability in industrial applications. |
| format | Article |
| id | doaj-art-e41f8bcedf46453c8bf9e3049bdf2bdb |
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| issn | 2949-754X |
| language | English |
| publishDate | 2025-06-01 |
| publisher | Elsevier |
| record_format | Article |
| series | Materials Today Catalysis |
| spelling | doaj-art-e41f8bcedf46453c8bf9e3049bdf2bdb2025-08-20T02:07:31ZengElsevierMaterials Today Catalysis2949-754X2025-06-01910010010.1016/j.mtcata.2025.100100Investigating size-dependent selectivity in benzaldehyde reductive amination via Ni nanoparticlesYunong Li0Ching Kit Tommy Wun1Tianxiang Chen2Tsz Woon Benedict Lo3State Key Laboratory of Chemical Biology and Drug Discovery, Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hom, Hong Kong SAR; The Hong Kong Polytechnic University Shenzhen Research Institute, The Hong Kong Polytechnic University, Shenzhen 518057, ChinaState Key Laboratory of Chemical Biology and Drug Discovery, Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hom, Hong Kong SAR; The Hong Kong Polytechnic University Shenzhen Research Institute, The Hong Kong Polytechnic University, Shenzhen 518057, ChinaState Key Laboratory of Chemical Biology and Drug Discovery, Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hom, Hong Kong SAR; The Hong Kong Polytechnic University Shenzhen Research Institute, The Hong Kong Polytechnic University, Shenzhen 518057, China; Corresponding authors at: State Key Laboratory of Chemical Biology and Drug Discovery, Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hom, Hong Kong SAR.State Key Laboratory of Chemical Biology and Drug Discovery, Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hom, Hong Kong SAR; The Hong Kong Polytechnic University Shenzhen Research Institute, The Hong Kong Polytechnic University, Shenzhen 518057, China; Department of Applied Physics, The Hong Kong Polytechnic University, Hung Hom, Hong Kong SAR; Corresponding authors at: State Key Laboratory of Chemical Biology and Drug Discovery, Department of Applied Biology and Chemical Technology, The Hong Kong Polytechnic University, Hung Hom, Hong Kong SAR.Selectivity control is a fundamental focus in catalysis chemistry, as it directly reflects the efficiency and efficacy of catalytic processes. While catalysis often involves intricate and cascade reaction steps using nanoparticle (NP) catalysts, the mechanism behind the size effect of nanoparticles on product selectivity has not been fully explored. We herein prepared a series of Ni-containing zeolitic catalysts in which the Ni NPs are uniformly supported on the mesopores and outer surfaces of H-ZSM-5 zeolites. The dynamic formation of Ni NPs from highly dispersed Ni precursors was monitored using transmission electron microscopy, in-situ X-ray pair distribution function, and in-situ X-ray absorption fine structure analysis. The metal nanoparticle size was carefully controlled between 3.72(5) nm and 11.91(7) by controlling the reduction temperature. We evaluated the catalytic performance of Ni NPs using the reductive amination of benzaldehyde in batch reactors at low temperatures. This reaction inherently favors the formation of a series of products, suffering highly from selectivity issues. Our results revealed a size-dependent behavior in reaction efficiency, with the catalyst achieving the highest catalytic activity (93 % selectivity in primary amine) at a particle size of 5.62(3) nm. This optimal performance is attributed to a balanced interplay between hydrogenation and amination capabilities. These findings highlight the intricate relationship between nanoparticle size and catalytic performance, emphasizing the necessity for precise optimization in catalyst design to enhance selectivity and sustainability in industrial applications.http://www.sciencedirect.com/science/article/pii/S2949754X25000134Ni nanoparticleSize effectReductive amination reactionPrecise controlIn-situ characterizationCatalyst design |
| spellingShingle | Yunong Li Ching Kit Tommy Wun Tianxiang Chen Tsz Woon Benedict Lo Investigating size-dependent selectivity in benzaldehyde reductive amination via Ni nanoparticles Materials Today Catalysis Ni nanoparticle Size effect Reductive amination reaction Precise control In-situ characterization Catalyst design |
| title | Investigating size-dependent selectivity in benzaldehyde reductive amination via Ni nanoparticles |
| title_full | Investigating size-dependent selectivity in benzaldehyde reductive amination via Ni nanoparticles |
| title_fullStr | Investigating size-dependent selectivity in benzaldehyde reductive amination via Ni nanoparticles |
| title_full_unstemmed | Investigating size-dependent selectivity in benzaldehyde reductive amination via Ni nanoparticles |
| title_short | Investigating size-dependent selectivity in benzaldehyde reductive amination via Ni nanoparticles |
| title_sort | investigating size dependent selectivity in benzaldehyde reductive amination via ni nanoparticles |
| topic | Ni nanoparticle Size effect Reductive amination reaction Precise control In-situ characterization Catalyst design |
| url | http://www.sciencedirect.com/science/article/pii/S2949754X25000134 |
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