Lei Yang,Shiyi Yu,Chong Peng,Xiangchen Fang,Zhenmin Cheng,Zhiming Zhou
A series of nonprecious monometallic Ni/AlSBA-15 and bimetallic Ni M (M = Zn, Ga, Cu, or Fe)/AlSBA-15 catalysts were prepared using a urea precipitation method and applied to the semihydrogenation of phenylacetylene. The catalysts were characterized by various techniques, showing that the Ni particle size of catalyst can be tuned by adjusting the Al content, and NiZn and NiGa supported catalysts exhibited geometric and electronic effects that originated from the bimetallic alloy. Among all the catalysts studied, NiZn 3 /AlSBA-15, with a turnover frequency of 10.89 s −1 comparable to that of precious Pd-based catalysts, presented the highest selectivity to styrene (90.3%) at nearly 100% conversion of phenylacetylene in semibatch operation. This catalyst was further evaluated in a continuous fixed-bed reactor for semihydrogenation of a model C 8 aromatic fraction of pyrolysis gasoline (a mixture of phenylacetylene, styrene, ethylbenzene and xylene), which aimed at assessing its practical application of recovering styrene from pyrolysis gasoline. The results showed that at complete conversion of phenylacetylene, the styrene concentration in the product was always kept at a stable level and higher than its initial concentration over 100 h of time on stream, demonstrating high selectivity and good stability of NiZn 3 /AlSBA-15. Finally, the application of NiZn 3 /AlSBA-15 was extended to other phenylacetylene derivatives.
Wenpeng Han,Shujuan Wang,Yajie Liu,Chaoqun Li,Ningning Yuan,Ligong Zhou,Mingxing Tang,Hui Ge
The transformation of biomass to liquid fuels and chemicals is of great interests. Herein, a series of reduced NiZn-CT (CT represents calcination temperature) catalysts with flower-like morphology and uniform particle sizes were prepared by co-precipitation method and used for hydrogenolysis of 5-hydroxymethylfural (HMF) to 2,5-dimethyfuran (DMF). The characterizations evidenced the formation of NiZn alloy phase in the catalysts through the strong metal-support interaction (SMSI), which had high C-O hydrogenolysis ability. The synergy of hydrogenation and C-O hydrogenolysis is essential for HMF to DMF, and we surprisingly found that this synergistic effect can be achieved just by controlling calcination temperature to regulated SMSI between Ni and ZnO. By this way, 99% DMF yield was gained at 180 °C for 4 h under 2 MPa H 2 over reduced NiZn-450 catalyst. More importantly, the active centers of this Ni/ZnO catalyst exhibited outstanding stability. There was no significant decrease in activity after reusing 9 times. The current research provided an easy-made catalytic system for HMF hydrogenolysis.
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