Selective hydrogenation of chloronitrobenzene(CNB) to chloroaniline(CAN) catalyzed by water-soluble Ru/Pt bimetallic catalyst in an aqueous-organic biphasic system was studied. It was found that the catalytic activity...Selective hydrogenation of chloronitrobenzene(CNB) to chloroaniline(CAN) catalyzed by water-soluble Ru/Pt bimetallic catalyst in an aqueous-organic biphasic system was studied. It was found that the catalytic activity increased obviously due to the addition of platinum. Ru/Pt bimetallic catalysts exhibited a strong synergistic effect when the molar ratio of Pt was in the range of 5%—80%. Under the mild conditions including a temperature of 25 ℃, a hydrogen pressure of 1.0 MPa and a Pt molar ratio of 20%, the conversion of p-chloronitrobenzene(p-CNB) reached 99.9%, with the selectivity to p-chloroaniline(p-CAN) equating to 99.4%. The Ru/Pt catalyst also showed high activity and selectivity for the hydrogenation of other chloro- and dichloro-nitrobenzenes with different substituted positions. In addition, the catalyst can be recycled five times without significant loss of activity.展开更多
The effect of rare earths （Sm, Pr, Ce, Nd and La） on the hydrogenation properties ofp-chloronitrobenzene （CNB） over Pt/CNTs catalyst was studied in ethanol at 303 K and normal pressure. The results exhibited that ...The effect of rare earths （Sm, Pr, Ce, Nd and La） on the hydrogenation properties ofp-chloronitrobenzene （CNB） over Pt/CNTs catalyst was studied in ethanol at 303 K and normal pressure. The results exhibited that the hydrogenation of p-CNB could be carried out over PtMOx/CNTs catalysts. Both catalytic activities and yields ofp-chloroaniline （CAN） were all improved. PtCeOx/ CNTs catalyst exhibited the best catalytic activity （TOF was 0.47 s^-1） and the highest yield of p-CAN （97.5 mol%）. PtCeOx/CNTs （1.0 wt%） catalyst exhibited good stability on the hydrogenation of p-CNB.展开更多
The effects of palladium addition and the reduction methods on Au/TiO2 were investigated. Pd was loaded on TiO2 firstly by incipient-wetness impregnation, Au was then loaded by deposition-precipitation method. The nom...The effects of palladium addition and the reduction methods on Au/TiO2 were investigated. Pd was loaded on TiO2 firstly by incipient-wetness impregnation, Au was then loaded by deposition-precipitation method. The nominal loadings of Au and Pd were 1 wt% and 0.01 wt%. The bimetallic catalysts were reduced by heating at 453 K, by flowing H2 at 423 K, or by NaBH4 at 298 K. The catalysts were characterized by ICP, XRD, TEM, HRTEM, TPR and XPS. Hydrogenation of p-chloronitrobenzene was carried out at 1.2 MPa H2 pressure and 353 K. The results showed that even adding very small amount of Pd could enhance activity and selectivity of p-chloroaniline significantly. Pd and Au formed alloy and Pd could donate partial electron to Au. Pd metal on the surface of alloy could adsorb hydrogen and enhanced the activity. The pretreatment methods did not change particle size significantly, all were below 4 nm. The sample reduced by NaBH4 could have higher concentration of Au0 and sustain small Au particle size, resulting in high activity.展开更多
研究了稀土元素对高分子负载Pt催化剂催化氢化氯代硝基苯反应的影响。结果表明:稀土元素的存在抑制了氯代硝基苯加氢反应活性,对产物氯代苯胺的选择性有不同程度的提高;碱NaOH存在时,PVP Pr Pt给出了90.8%的邻氯苯胺选择性,使用PVP La P...研究了稀土元素对高分子负载Pt催化剂催化氢化氯代硝基苯反应的影响。结果表明:稀土元素的存在抑制了氯代硝基苯加氢反应活性,对产物氯代苯胺的选择性有不同程度的提高;碱NaOH存在时,PVP Pr Pt给出了90.8%的邻氯苯胺选择性,使用PVP La Pt时得到97 2%的间氯苯胺选择性,PVP Ce Pt催化体系获得了98.2%的对氯苯胺选择性。展开更多
基金the financial supports of the Natural Science Foundation of China(No.21303139)the Open Project of Chemical Synthesis and Pollution Control Key Laboratory of Sichuan Province(No.CSPC2013-1)+1 种基金the Key Fund Project of Educational Department of Sichuan Province(No.14ZA0126)the Doctoral Initiating Fund of China West Normal University(No.10B010)
文摘Selective hydrogenation of chloronitrobenzene(CNB) to chloroaniline(CAN) catalyzed by water-soluble Ru/Pt bimetallic catalyst in an aqueous-organic biphasic system was studied. It was found that the catalytic activity increased obviously due to the addition of platinum. Ru/Pt bimetallic catalysts exhibited a strong synergistic effect when the molar ratio of Pt was in the range of 5%—80%. Under the mild conditions including a temperature of 25 ℃, a hydrogen pressure of 1.0 MPa and a Pt molar ratio of 20%, the conversion of p-chloronitrobenzene(p-CNB) reached 99.9%, with the selectivity to p-chloroaniline(p-CAN) equating to 99.4%. The Ru/Pt catalyst also showed high activity and selectivity for the hydrogenation of other chloro- and dichloro-nitrobenzenes with different substituted positions. In addition, the catalyst can be recycled five times without significant loss of activity.
文摘The effect of rare earths （Sm, Pr, Ce, Nd and La） on the hydrogenation properties ofp-chloronitrobenzene （CNB） over Pt/CNTs catalyst was studied in ethanol at 303 K and normal pressure. The results exhibited that the hydrogenation of p-CNB could be carried out over PtMOx/CNTs catalysts. Both catalytic activities and yields ofp-chloroaniline （CAN） were all improved. PtCeOx/ CNTs catalyst exhibited the best catalytic activity （TOF was 0.47 s^-1） and the highest yield of p-CAN （97.5 mol%）. PtCeOx/CNTs （1.0 wt%） catalyst exhibited good stability on the hydrogenation of p-CNB.
文摘The effects of palladium addition and the reduction methods on Au/TiO2 were investigated. Pd was loaded on TiO2 firstly by incipient-wetness impregnation, Au was then loaded by deposition-precipitation method. The nominal loadings of Au and Pd were 1 wt% and 0.01 wt%. The bimetallic catalysts were reduced by heating at 453 K, by flowing H2 at 423 K, or by NaBH4 at 298 K. The catalysts were characterized by ICP, XRD, TEM, HRTEM, TPR and XPS. Hydrogenation of p-chloronitrobenzene was carried out at 1.2 MPa H2 pressure and 353 K. The results showed that even adding very small amount of Pd could enhance activity and selectivity of p-chloroaniline significantly. Pd and Au formed alloy and Pd could donate partial electron to Au. Pd metal on the surface of alloy could adsorb hydrogen and enhanced the activity. The pretreatment methods did not change particle size significantly, all were below 4 nm. The sample reduced by NaBH4 could have higher concentration of Au0 and sustain small Au particle size, resulting in high activity.
文摘研究了稀土元素对高分子负载Pt催化剂催化氢化氯代硝基苯反应的影响。结果表明:稀土元素的存在抑制了氯代硝基苯加氢反应活性,对产物氯代苯胺的选择性有不同程度的提高;碱NaOH存在时,PVP Pr Pt给出了90.8%的邻氯苯胺选择性,使用PVP La Pt时得到97 2%的间氯苯胺选择性,PVP Ce Pt催化体系获得了98.2%的对氯苯胺选择性。
