Supported copper catalyst, preparation method and application thereof, and method for preparing propylene oxide by oxidation of propylene
A copper catalyst and catalyst technology, applied in chemical instruments and methods, physical/chemical process catalysts, organic compound/hydride/coordination complex catalysts, etc., can solve problems such as unsatisfactory PO selectivity and decreased PO selectivity. , to achieve the effect of good stability, high activity and good selectivity
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[0054] According to the preparation method of the present invention, the phosphorus-containing organic ligands that meet the aforementioned requirements include, but are not limited to, compounds selected from phosphoric acid esters and / or phosphite esters, preferably selected from aromatic phosphoric acid esters or aromatic compounds having the following structure: One or more of group phosphites:
[0055]
[0056] Where R 1 , R 2 , R 3 , R 4 , R 5 Each is a substituted or unsubstituted aryl group; R 6 , R 7 , R 8 , R 9 , R 10 , R 11 Each is a substituted or unsubstituted arylene group, R 12 , R 13 Is C 1 -C 6 The alkylene group or a substituted or unsubstituted arylene group, R 14 , R 15 , R 16 , R 17 Each is a substituted or unsubstituted aryl group.
[0057] Preferably, R 1 , R 2 , R 3 , R 4 , R 5 Each substituted C 6 -C 10 The aryl group or unsubstituted aryl group; R 6 , R 7 , R 8 , R 9 , R 10 , R 11 Each substituted C 6 -C 10 The arylene group or unsubstituted arylene group, ...
Embodiment 1
[0099] Prepare 5 wt% Cu / SiO 2 / DOPO(P / Cu=1(mol / mol)) catalyst
[0100] SiO 2 Carrier (Grvisil Grade 62, specific surface area is 380m 2 / g, the pore size is 15 nanometers, 60-200 mesh) before use, activated at 250 ℃ for 4 hours, 5.56 grams of CuCl 2 ·H 2 O was dissolved in 77.7 g of deionized water, and the solution was added dropwise to 36 g of SiO 2 In the carrier, continue to stir the carrier during the dripping process to make the solution uniformly absorbed. After the solution is dripped, the carrier particles are completely wetted by the solution, but there is no free-flowing solution. The obtained solid is dried at 120°C for 4 hours and then at 300°C in an air atmosphere Calcined in medium for 4 hours to obtain a copper oxide-loaded carrier;
[0101] Take 0.3758 grams of 9,10-dihydro-9-oxa-10-phosphaphenanthrene-10-oxide (DOPO) was dissolved in 30 mL of toluene, 2.0 g of the aforementioned copper oxide-loaded carrier was added, stirred at 50°C for 4 hours, then the solvent w...
Embodiment 2
[0106] Prepare 5 wt% Cu / Al 2 O 3 / TPP(P / Cu=0.5(mol / mol)) catalyst
[0107] Al 2 O 3 The carrier was activated at 350°C for 4 hours before use, and 7.72 g of CuCl 2 ·H 2 O is dissolved in 54 grams of deionized water, and the solution is added dropwise to 50 grams of Al 2 O 3 In the carrier, continue to stir the carrier during the dripping process to make the solution uniformly absorbed. After the solution is dripped, the carrier particles are completely wetted by the solution, but there is no free-flowing solution. The obtained solid is dried at 120°C for 4 hours and then at 300°C in an air atmosphere Calcined in medium for 4 hours to obtain a copper oxide-loaded carrier;
[0108] Dissolve 0.2836 g of triphenyl phosphate (TPP) in 30 mL of toluene, add 2.0 g of the roasted copper oxide-loaded carrier, stir at 50°C for 4 hours, and then rotate and evaporate to remove the solvent. The resulting solid is heated at 120°C. Dry for 4 hours to obtain a catalyst.
[0109] Temperature programm...
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