Bimetallic Synergy Effects of Phyllosilicate‐Derived NiCu@SiO2 Catalysts for 1,4‐Butynediol Direct Hydrogenation to 1,4‐Butanediol.
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| Title: | Bimetallic Synergy Effects of Phyllosilicate‐Derived NiCu@SiO |
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| Authors: | Wang, Changzhen1 (AUTHOR) czwang@sxu.edu.cn, Tian, Yani1 (AUTHOR), Wu, Ruifang1 (AUTHOR), Li, Haitao1 (AUTHOR), Yao, Benzhen2 (AUTHOR), Zhao, Yongxiang1 (AUTHOR) yxzhao@sxu.edu.cn, Xiao, Tiancun2 (AUTHOR) xiao.tiancun@chem.ox.ac.uk |
| Source: | ChemCatChem. 10/7/2019, Vol. 11 Issue 19, p4777-4787. 11p. |
| Subjects: | Butanediol, Allyl alcohol, Hydrogenation, Bimetallic catalysts, Metal nanoparticles, Hydrogenolysis |
| Abstract: | Hydrogenation of 1,4‐butynediol (BYD) to 1,4‐butanediol (BDO) is a two‐step process, with an initial hydrogenation of BYD to 1,4‐butenediol (BED) and the subsequent hydrogenation of BED to BDO. However, the BYD hydrogenation also involves many side reactions originated from the isomerization of BED. In order to inhibit the isomerization pathways, phyllosilicate‐derived bimetallic NiCu@SiO2 catalysts have been developed for efficient C≡C/C=C hydrogenation in this work. Due to the formation of phyllosilicate matrix and highly dispersed metal nanoparticles, NiCu@SiO2 showed total BYD conversion with extremely high BDO selectivity compared to a conventional impregnated Ni/SiO2 catalyst. A remarkable result of NiCu@SiO2 catalysts is that a new type of bimetallic catalytic sites responsible for the high hydrogenation activity can be differentiated from the Ni phyllosilicate matrix by the induction of Cu species, and these neighboring bimetallic sites with the help of weak acid phyllosilicate interface, can realize to stabilize the activated BED species (allyl alcohol form) adsorbed on the cooperative active sites, thus to avoid its isomerization to aldehyde form and unexpected C=O hydrogenolysis. Consequently, it enhanced the selectivity to the diol products BDO significantly. Owing to the benign improvement of three center synergy effect, 9Ni1Cu@SiO2 possesses the optimum BYD direct hydrogenation ability with a rarely reported high selectivity of 90.5–94.5 % at 50 °C and 1 MPa. [ABSTRACT FROM AUTHOR] |
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| Database: | Engineering Source |
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| Abstract: | Hydrogenation of 1,4‐butynediol (BYD) to 1,4‐butanediol (BDO) is a two‐step process, with an initial hydrogenation of BYD to 1,4‐butenediol (BED) and the subsequent hydrogenation of BED to BDO. However, the BYD hydrogenation also involves many side reactions originated from the isomerization of BED. In order to inhibit the isomerization pathways, phyllosilicate‐derived bimetallic NiCu@SiO2 catalysts have been developed for efficient C≡C/C=C hydrogenation in this work. Due to the formation of phyllosilicate matrix and highly dispersed metal nanoparticles, NiCu@SiO2 showed total BYD conversion with extremely high BDO selectivity compared to a conventional impregnated Ni/SiO2 catalyst. A remarkable result of NiCu@SiO2 catalysts is that a new type of bimetallic catalytic sites responsible for the high hydrogenation activity can be differentiated from the Ni phyllosilicate matrix by the induction of Cu species, and these neighboring bimetallic sites with the help of weak acid phyllosilicate interface, can realize to stabilize the activated BED species (allyl alcohol form) adsorbed on the cooperative active sites, thus to avoid its isomerization to aldehyde form and unexpected C=O hydrogenolysis. Consequently, it enhanced the selectivity to the diol products BDO significantly. Owing to the benign improvement of three center synergy effect, 9Ni1Cu@SiO2 possesses the optimum BYD direct hydrogenation ability with a rarely reported high selectivity of 90.5–94.5 % at 50 °C and 1 MPa. [ABSTRACT FROM AUTHOR] |
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| ISSN: | 18673880 |
| DOI: | 10.1002/cctc.201901052 |
