We studied the hydrogenation of 2‐ethylanthraquinone（eAQ） over Pd/SiO2/COR（COR = cordierite） monometallic and Pd‐M/SiO2/COR（M = Ni, Fe, Mn, and Cu） bimetallic monolithic catalysts, which were prepared by the c...We studied the hydrogenation of 2‐ethylanthraquinone（eAQ） over Pd/SiO2/COR（COR = cordierite） monometallic and Pd‐M/SiO2/COR（M = Ni, Fe, Mn, and Cu） bimetallic monolithic catalysts, which were prepared by the co‐impregnation method. Detailed investigations showed that the particle sizes and structures of the Pd‐M（M = Ni, Fe, Mn, and Cu） bimetallic monolithic catalysts were great‐ly affected by the second metal M and the mass ratio of Pd to the second metal M. By virtue of the small particle size and the strong interaction between Pd and Ni of Pd‐Ni alloy, Pd‐Ni bimetallic monolithic catalysts with the mass ratio of Pd/Ni = 2 achieved the highest H2O2 yield（7.5 g/L） and selectivity（95.3%）. Moreover, density functional theory calculations were performed for eAQ ad‐sorption to gain a better mechanistic understanding of the molecule‐surface interactions between eAQ and the Pd（1 1 1） or PdM（1 1 1）（M = Ni, Fe, Mn, and Cu） surfaces. It was found that the high activity of the bimetallic Pd‐Ni catalyst was a result of strong chemisorption between Pd3Ni1（1 1 1） and the carbonyl group of eAQ.展开更多
A periodic packing mode of trickle-bed reactor (TBR) for the gas limited reaction was proposed. Hy-drogenation of 2-ethylanthraquinone over Pd/Al2O3 in a laboratory-scale TBR was taken as a test reaction for determini...A periodic packing mode of trickle-bed reactor (TBR) for the gas limited reaction was proposed. Hy-drogenation of 2-ethylanthraquinone over Pd/Al2O3 in a laboratory-scale TBR was taken as a test reaction for determining whether the periodic packing mode is advantageous. The effects of operating conditions and packing type on TBR performance were experimentally examined to demonstrate the cause-effect relationships. A mathe-matic model of TBR considering axial dispersion and fractional wetting was developed to quantitatively illuminate the reason of performance enhancement.展开更多
基金supported by the National Natural Science Foundation of China (21476009, 21406007, U1462104)~~
文摘We studied the hydrogenation of 2‐ethylanthraquinone（eAQ） over Pd/SiO2/COR（COR = cordierite） monometallic and Pd‐M/SiO2/COR（M = Ni, Fe, Mn, and Cu） bimetallic monolithic catalysts, which were prepared by the co‐impregnation method. Detailed investigations showed that the particle sizes and structures of the Pd‐M（M = Ni, Fe, Mn, and Cu） bimetallic monolithic catalysts were great‐ly affected by the second metal M and the mass ratio of Pd to the second metal M. By virtue of the small particle size and the strong interaction between Pd and Ni of Pd‐Ni alloy, Pd‐Ni bimetallic monolithic catalysts with the mass ratio of Pd/Ni = 2 achieved the highest H2O2 yield（7.5 g/L） and selectivity（95.3%）. Moreover, density functional theory calculations were performed for eAQ ad‐sorption to gain a better mechanistic understanding of the molecule‐surface interactions between eAQ and the Pd（1 1 1） or PdM（1 1 1）（M = Ni, Fe, Mn, and Cu） surfaces. It was found that the high activity of the bimetallic Pd‐Ni catalyst was a result of strong chemisorption between Pd3Ni1（1 1 1） and the carbonyl group of eAQ.
基金the State Key Development Program for Basic Research of China (No. G2000048005) the SINOPEC (No.X503023).
文摘A periodic packing mode of trickle-bed reactor (TBR) for the gas limited reaction was proposed. Hy-drogenation of 2-ethylanthraquinone over Pd/Al2O3 in a laboratory-scale TBR was taken as a test reaction for determining whether the periodic packing mode is advantageous. The effects of operating conditions and packing type on TBR performance were experimentally examined to demonstrate the cause-effect relationships. A mathe-matic model of TBR considering axial dispersion and fractional wetting was developed to quantitatively illuminate the reason of performance enhancement.
