The adsorption of Pd(Ⅱ), Pt(IV) and Cu(Ⅱ) in static and dynamic conditions on chemically modified silica containing sulfide sulfur (number of grafted functional groups of the sorbent was 0.2 (CMS-S 0.2) and 0 3 mmol...The adsorption of Pd(Ⅱ), Pt(IV) and Cu(Ⅱ) in static and dynamic conditions on chemically modified silica containing sulfide sulfur (number of grafted functional groups of the sorbent was 0.2 (CMS-S 0.2) and 0 3 mmol/g (CMS-S 0.3)) was studied. It is established that an increase in the acidity of the sorption of Pd(Ⅱ) and Pt(Ⅳ) decreases, whereas the Cu(Ⅱ) does not change. Time to reach the constant values of the sorption is 15 min. In equal conditions, the sorption decreases in the number of Pd(Ⅱ)>Pt(IV)>Cu(Ⅱ). Based on retrieved data suggested that the sorption of Pd(Ⅱ) proceeds according the coordination mechanism. In the case of sorption from solutions with a high palladium content can be polymerization of adsorbed complexes in the sorbent phase. Worked out the optimal conditions for the separation of pairs of Pd(Ⅱ)-Pt(Ⅳ) and Pd(Ⅱ)-Cu(Ⅱ) under dynamic conditions with the extraction of palladium(Ⅱ) in the eluate is above 95%.展开更多
The purpose of this work is to synthesize the catalytic systems containing palladium nanoparticles and using hydroxycarbonates of yttrium and cerium as supports,and to test the catalytic activity of the obtained catal...The purpose of this work is to synthesize the catalytic systems containing palladium nanoparticles and using hydroxycarbonates of yttrium and cerium as supports,and to test the catalytic activity of the obtained catalysts in the Suzuki cross-couping reaction.Nanocomposites Pd/Y(OH)CO 3 and Pd/Ce(OH)CO 3 were synthesized according to two methods:the first one-simultaneous production of nanoscale substrate and immobilization of palladium nanoparticles on its surface(nanocomposites 1),the second one-the prior synthesis of polyvinylpyrrolidone stabilized palladium nanoparticles followed by their immobilization on the nano sized substrate surface(nanocomposites 2).The reaction between phenylboronic acid and iodobenzene is chosen as a model one.The dependence of the catalytic activity of catalysts on the method of their synthesis was established.It was established that nanocomposites 2 exhibit higher catalytic activity in the selected reaction compared to the nanocomposites 1.The TOF values for the nanocomposites 1 are 6663~14617 h 1 when using the substrate Ce(OH)CO 3 and 13774~27084 h 1 when using the substrate Y(OH)CO 3,while the nanocomposites 2 reveal TOF = 87287 h 1 for the substrate Ce(OH)CO 3 and TOF = 97746 h 1 for the substrate Y(OH)CO 3 under other equal conditions.In addition,nanocomposites 2 "work" at room temperature giving a high yield of the desired product.It is noted that the support nanoparticles Y(OH)CO 3 and Ce(OH)CO 3 also exhibit catalytic activity.The yield of the final product of the reaction using them as catalysts is 55%(TOF = 11 and 8 h 1,respectively).Thus,the use of yttrium and cerium hydroxycarbonates as supports allows to decrease the palladium content in the nanocomposites to 0.01%~1% and,consequently,reduce the cost of the catalyst while maintaining its high catalytic activity.展开更多
文摘The adsorption of Pd(Ⅱ), Pt(IV) and Cu(Ⅱ) in static and dynamic conditions on chemically modified silica containing sulfide sulfur (number of grafted functional groups of the sorbent was 0.2 (CMS-S 0.2) and 0 3 mmol/g (CMS-S 0.3)) was studied. It is established that an increase in the acidity of the sorption of Pd(Ⅱ) and Pt(Ⅳ) decreases, whereas the Cu(Ⅱ) does not change. Time to reach the constant values of the sorption is 15 min. In equal conditions, the sorption decreases in the number of Pd(Ⅱ)>Pt(IV)>Cu(Ⅱ). Based on retrieved data suggested that the sorption of Pd(Ⅱ) proceeds according the coordination mechanism. In the case of sorption from solutions with a high palladium content can be polymerization of adsorbed complexes in the sorbent phase. Worked out the optimal conditions for the separation of pairs of Pd(Ⅱ)-Pt(Ⅳ) and Pd(Ⅱ)-Cu(Ⅱ) under dynamic conditions with the extraction of palladium(Ⅱ) in the eluate is above 95%.
文摘The purpose of this work is to synthesize the catalytic systems containing palladium nanoparticles and using hydroxycarbonates of yttrium and cerium as supports,and to test the catalytic activity of the obtained catalysts in the Suzuki cross-couping reaction.Nanocomposites Pd/Y(OH)CO 3 and Pd/Ce(OH)CO 3 were synthesized according to two methods:the first one-simultaneous production of nanoscale substrate and immobilization of palladium nanoparticles on its surface(nanocomposites 1),the second one-the prior synthesis of polyvinylpyrrolidone stabilized palladium nanoparticles followed by their immobilization on the nano sized substrate surface(nanocomposites 2).The reaction between phenylboronic acid and iodobenzene is chosen as a model one.The dependence of the catalytic activity of catalysts on the method of their synthesis was established.It was established that nanocomposites 2 exhibit higher catalytic activity in the selected reaction compared to the nanocomposites 1.The TOF values for the nanocomposites 1 are 6663~14617 h 1 when using the substrate Ce(OH)CO 3 and 13774~27084 h 1 when using the substrate Y(OH)CO 3,while the nanocomposites 2 reveal TOF = 87287 h 1 for the substrate Ce(OH)CO 3 and TOF = 97746 h 1 for the substrate Y(OH)CO 3 under other equal conditions.In addition,nanocomposites 2 "work" at room temperature giving a high yield of the desired product.It is noted that the support nanoparticles Y(OH)CO 3 and Ce(OH)CO 3 also exhibit catalytic activity.The yield of the final product of the reaction using them as catalysts is 55%(TOF = 11 and 8 h 1,respectively).Thus,the use of yttrium and cerium hydroxycarbonates as supports allows to decrease the palladium content in the nanocomposites to 0.01%~1% and,consequently,reduce the cost of the catalyst while maintaining its high catalytic activity.