Ultra-Dilute high-entropy alloy catalyst with core-shell structure for high-active hydrogenation of furfural to furfuryl alcohol at mild temperature

• Published in: Chemical engineering journal (Lausanne, Switzerland : 1996) Switzerland : 1996), 2023-01, Vol.452, p.139526, Article 139526
• Main Authors: Tu, Ren, Liang, Kaili, Sun, Yan, Wu, Yangwen, Lv, Wei, Jia, Charles Q, Jiang, Enchen, Wu, Yujian, Fan, Xudong, Zhang, Bing, Lu, Qiang, Zhang, Bingsen, Xu, Xiwei
• Format: Article
• Language: English
• Subjects: Core-shell structure; Furfural; High-entropy alloy; Hydrogenation; Ultra-dilute alloy
• ISSN: 1385-8947; 1873-3212
• DOI: 10.1016/j.cej.2022.139526

[Display omitted] •Ultra-dilute HEA with core–shell structure was synthesized via reduction temperature driven.•The role of each constituent metal site in ultra-dilute HEA was studied.•Atomically dispersed Zn and electron-rich Cu resulted in 87.32% furfuryl alcohol yield at 90℃.•Cu precipitation in ultra-dilute HEA inhibited the selective hydrogenation of furfural.•DFT proved atomically dispersed Zn was the active sites for the adsorption of furfural. Furfuryl Alcohol (FOL) from the catalytic hydrogenation of furfural represented a promising intermediate for industrial application. However, the high selectively of FOL in mild temperature was limited due to the over hydrogenation. Here, we synthesized the novel ultra-dilute high-entropy alloys (HEAs) with multiple metal sites and core–shell structure for boosting the selectivity of furfural hydrogenation to furfuryl alcohol. The results showed that the furfural was converted to FOL with the conversion of 87.32% and selectivity of 100% at 90℃ over ultra-dilute HEA (NiCoCuZnFe/C-800). The catalyst had redistribution of electrons between Cu (2.00) and atomically dispersed Zn (1.65) due to the different electronegativity. The electron-rich Cu repelled the furan ring and prevented the over hydrogenation, while the atomically dispersed Zn presented the strongest –CHO adsorption performance. Moreover, the core–shell structure enhanced the stability of the catalysts during hydrogenation reaction and the porous carbon shell improved the transferring of furfural and electronic.