Qingxiang Zhang,Dengqian Zhang,Zhen Wang,Zheng Liu,Yukun Xi,Wei Zhang,Chen Zhang,Yin Liu
Catalytic transfer hydrodechlorination of plastic pyrolysis oil on supported transition-metal catalysts using isopropanol as a hydrogen donor was investigated in this work. The catalysts were characterized by N2 adsorption, X-ray diffraction, hydrogen temperature-programmed desorption, and X-ray photoelectron spectroscopy, and the reaction products were identified by GC-MS. Among various Al2O3-supported transition-metal (Cu, Co, Ni) catalysts, Cu/Al2O3 exhibited the best catalytic transfer hydrodechlorination performance due to the superior activation ability of Cu/Al2O3 for isopropanol. The doping of Ni in Cu/Al2O3 significantly enhanced its catalytic activity due to the inherent excellent hydrogenation activity of Ni, good metal dispersion, and strong Ni–Cu interaction in Ni–Cu/Al2O3. GC-MS results revealed that chlorobenzene was hydrogenated to benzene and HCl, and isopropanol was dehydrogenated to form acetone, which was subsequently transformed to methyl isobutyl ketone. The reactivities of three representative organochlorine compounds followed the order of chlorobenzene > tetrachloroethane > tetrachloroethylene. Ultradeep dechlorination of real plastic pyrolysis oil was achieved by catalytic transfer hydrodechlorination over the optimal 15Ni-10Cu/Al2O3 catalyst. The chlorine content of real plastic pyrolysis oil was reduced from 61.7 to 0.5 mg/L with a chlorine removal of 99.2% after reaction for 3 h at the reaction temperature of 210 °C.
Zhenbing Xie,Bingfeng Chen,Haoran Wu,Mingyang Liu,Huizhen Liu,Jianling Zhang,Guanying Yang,Buxing Han
Transformation of biomass or biomass-based feedstocks into fuels or valuable chemicals is of great importance for the sustainable development of our society. Mesoporous Al2O3–ZrO2 with different Al : Zr molar ratios was prepared by the sol–gel method, and Cu–Ni/Al2O3–ZrO2 catalysts were fabricated by the impregnation method. The catalytic performances of the bifunctional catalysts were studied in the selective hydrogenation of levulinic acid (LA) into 2-methyltetrahydrofuran (MTHF). It was demonstrated that both Cu : Ni and Al : Zr ratios affected the selectivity to MTHF significantly. The bimetallic catalysts Cu–Ni/Al2O3–ZrO2 containing 10 wt% Ni and 10 wt% Cu gave 99.8% MTHF selectivity at full conversion of LA when the Al : Zr ratio was 9 : 1. The outstanding catalytic performance of the catalyst is related to the mesoporous structure, the acidic properties of the support and the synergistic effect between Cu and Ni. The catalyst could be reused five times without a considerable loss of catalytic activity and selectivity.
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