期刊
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
卷 5, 期 12, 页码 11280-11289出版社
AMER CHEMICAL SOC
DOI: 10.1021/acssuschemeng.7b01813
关键词
Biomass; 5-Hydroxymethylfurfural; Hydrogenation; Ni; Intermetallic
资金
- Major State Basic Research Development Program of China [2012CB215305]
- National Science Foundation in Jiangsu Province [BK20170707]
5-Hydroxymethylfurfural (HMF) is an important platform chemical derived from C-6 sugars and cellulose. The formed 2,5-dimethylfuran (DMF) via hydrogenolysis of HMF was denoted as a promising and sustainable fuel candidate. The further improvement of DMF yield is the central premise of this work, which is based on the elucidation of the relationship between catalytic performance and active sites. Herein, a NiZn alloy catalyst was formed through Zn inclusion to Ni by controllable reduction of the NiZnAI hydrotalcite-derived NiO-ZnO-Al2O3 mixed oxide. The combination of temperature-programmed reduction (TPR), in situ X-ray diffraction (XRD), CO-adsorbed infrared spectroscopy (CO-IR), and X-ray photoelectron spec troscopy (XPS) revealed that the surface of the NiZn catalyst was composed of beta 1-NiZn while the bulk was composed of a-NiZn. Moreover, the surface Ni atoms were geometrically isolated by Zn atoms and modulated to be electron-rich. Finally, the rate of C=O/C-O hydrogenolysis over C=C/C C hydrogenation for NiZn alloy catalyst was approximately three times higher than that of monometallic Ni catalyst. A 93.6% yield of DMF was obtained over NiZn alloy catalyst. The greatly improved DMF yield was thus attributed to the electron modification and isolation of Ni atoms due to the formation of NiZn alloy.
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