{"title":"强金属载体相互作用驱动的超小高熵合金纳米颗粒选择性加氢合成","authors":"Ren Tu, Hui Yang, Yan Sun, Kaili Liang, Bingsen Zhang, Charles Q. Jia, Shixian Wang, Yujian Wu, Xudong Fan, Enchen Jiang, Xiwei Xu","doi":"10.1016/j.jcat.2025.116468","DOIUrl":null,"url":null,"abstract":"High-entropy alloys (HEAs) have garnered significant attention due to their nearly infinite number of unprecedented active sites. However, the synthesis of ultrasmall HEA nanoparticles remains challenging due to their inherent thermodynamic instability. In this study, we demonstrate that a strong metal-support interaction (SMSI) can effectively suppress agglomeration through interfacial stabilization. By leveraging a quenching-based approach, we successfully synthesized HEA catalysts with ultralow loading (<0.17 wt%), ultrasmall particle sizes (<3.7 nm), and an SMSI-induced encapsulation layer. The formation of this protective layer enables precise control over the structural and electronic properties of catalyst. To probe the catalytic performance, cinnamaldehyde was employed as a model α,β-unsaturated aldehyde in selective hydrogenation reactions. The results reveal that a lower Pt ratio in HEA-Cu8Pt2 enhances HCAL selectivity, reaching 93.6 %, which is attributed to the modified interfacial electronic environment between TiO<sub>2</sub> and HEA, promoting Pt<sup>2+</sup> species formation and strong hydrogen spillover. This work provides new insights into the design and regulation of ultrasmall HEA catalysts through SMSI effects.","PeriodicalId":346,"journal":{"name":"Journal of Catalysis","volume":"29 1","pages":""},"PeriodicalIF":6.5000,"publicationDate":"2025-10-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":"0","resultStr":"{\"title\":\"Strong metal support interaction driven synthesis of ultrasmall high entropy alloy nanoparticles for selective hydrogenation\",\"authors\":\"Ren Tu, Hui Yang, Yan Sun, Kaili Liang, Bingsen Zhang, Charles Q. Jia, Shixian Wang, Yujian Wu, Xudong Fan, Enchen Jiang, Xiwei Xu\",\"doi\":\"10.1016/j.jcat.2025.116468\",\"DOIUrl\":null,\"url\":null,\"abstract\":\"High-entropy alloys (HEAs) have garnered significant attention due to their nearly infinite number of unprecedented active sites. However, the synthesis of ultrasmall HEA nanoparticles remains challenging due to their inherent thermodynamic instability. In this study, we demonstrate that a strong metal-support interaction (SMSI) can effectively suppress agglomeration through interfacial stabilization. By leveraging a quenching-based approach, we successfully synthesized HEA catalysts with ultralow loading (<0.17 wt%), ultrasmall particle sizes (<3.7 nm), and an SMSI-induced encapsulation layer. The formation of this protective layer enables precise control over the structural and electronic properties of catalyst. To probe the catalytic performance, cinnamaldehyde was employed as a model α,β-unsaturated aldehyde in selective hydrogenation reactions. The results reveal that a lower Pt ratio in HEA-Cu8Pt2 enhances HCAL selectivity, reaching 93.6 %, which is attributed to the modified interfacial electronic environment between TiO<sub>2</sub> and HEA, promoting Pt<sup>2+</sup> species formation and strong hydrogen spillover. This work provides new insights into the design and regulation of ultrasmall HEA catalysts through SMSI effects.\",\"PeriodicalId\":346,\"journal\":{\"name\":\"Journal of Catalysis\",\"volume\":\"29 1\",\"pages\":\"\"},\"PeriodicalIF\":6.5000,\"publicationDate\":\"2025-10-08\",\"publicationTypes\":\"Journal Article\",\"fieldsOfStudy\":null,\"isOpenAccess\":false,\"openAccessPdf\":\"\",\"citationCount\":\"0\",\"resultStr\":null,\"platform\":\"Semanticscholar\",\"paperid\":null,\"PeriodicalName\":\"Journal of Catalysis\",\"FirstCategoryId\":\"92\",\"ListUrlMain\":\"https://doi.org/10.1016/j.jcat.2025.116468\",\"RegionNum\":1,\"RegionCategory\":\"化学\",\"ArticlePicture\":[],\"TitleCN\":null,\"AbstractTextCN\":null,\"PMCID\":null,\"EPubDate\":\"\",\"PubModel\":\"\",\"JCR\":\"Q2\",\"JCRName\":\"CHEMISTRY, PHYSICAL\",\"Score\":null,\"Total\":0}","platform":"Semanticscholar","paperid":null,"PeriodicalName":"Journal of Catalysis","FirstCategoryId":"92","ListUrlMain":"https://doi.org/10.1016/j.jcat.2025.116468","RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":null,"EPubDate":"","PubModel":"","JCR":"Q2","JCRName":"CHEMISTRY, PHYSICAL","Score":null,"Total":0}
Strong metal support interaction driven synthesis of ultrasmall high entropy alloy nanoparticles for selective hydrogenation
High-entropy alloys (HEAs) have garnered significant attention due to their nearly infinite number of unprecedented active sites. However, the synthesis of ultrasmall HEA nanoparticles remains challenging due to their inherent thermodynamic instability. In this study, we demonstrate that a strong metal-support interaction (SMSI) can effectively suppress agglomeration through interfacial stabilization. By leveraging a quenching-based approach, we successfully synthesized HEA catalysts with ultralow loading (<0.17 wt%), ultrasmall particle sizes (<3.7 nm), and an SMSI-induced encapsulation layer. The formation of this protective layer enables precise control over the structural and electronic properties of catalyst. To probe the catalytic performance, cinnamaldehyde was employed as a model α,β-unsaturated aldehyde in selective hydrogenation reactions. The results reveal that a lower Pt ratio in HEA-Cu8Pt2 enhances HCAL selectivity, reaching 93.6 %, which is attributed to the modified interfacial electronic environment between TiO2 and HEA, promoting Pt2+ species formation and strong hydrogen spillover. This work provides new insights into the design and regulation of ultrasmall HEA catalysts through SMSI effects.
期刊介绍:
The Journal of Catalysis publishes scholarly articles on both heterogeneous and homogeneous catalysis, covering a wide range of chemical transformations. These include various types of catalysis, such as those mediated by photons, plasmons, and electrons. The focus of the studies is to understand the relationship between catalytic function and the underlying chemical properties of surfaces and metal complexes.
The articles in the journal offer innovative concepts and explore the synthesis and kinetics of inorganic solids and homogeneous complexes. Furthermore, they discuss spectroscopic techniques for characterizing catalysts, investigate the interaction of probes and reacting species with catalysts, and employ theoretical methods.
The research presented in the journal should have direct relevance to the field of catalytic processes, addressing either fundamental aspects or applications of catalysis.