• 专利标题:   Preparation of supported nickel-palladium bimetallic catalyst in oxidative coupling reaction, involves mixing sodium chloropalladate and nickel chloride, adding graphene oxide and deionized water, preparing supported bimetallic nickel-palladium doped gallium oxide catalyst, drying, and grinding.
  • 专利号:   CN113318754-A
  • 发明人:   HUANG F, WANG J, WANG X, SUN J, HUANG S, HUANG Y, FANG H, LI C, LI K, WANG B, CHEN J, SUN M
  • 专利权人:   HUANG S
  • 国际专利分类:   B01J023/89, C07D277/66, C07D417/10
  • 专利详细信息:   CN113318754-A 31 Aug 2021 B01J-023/89 202187 Pages: 13 Chinese
  • 申请详细信息:   CN113318754-A CN10697626 23 Jun 2021
  • 优先权号:   CN10697626

▎ 摘  要

NOVELTY - Preparation of supported nickel-palladium bimetallic catalyst involves (i) taking 10 mL 0.010-0.020 mol/L sodium chloropalladate, 10 mL 0.010-0.020 mol/L nickel chloride solution into 100 mL round bottom flask (A), magnetically stirring to completely and uniformly mixing sodium chloropalladate and nickel chloride to obtain solution which is transparent red-brown, (ii) adding 8-12 mg graphene oxide (GO) and 20 mL deionized water into a 100 mL round bottom flask (B), ultrasonically reacting for 1-2 hours, (iii) gradually adding the graphene oxide aqueous solution in round-bottom flask (B) to round-bottom flask (A), (iv) using 1.0 mol/L sodium hydroxide solution to adjust the pH value of the mixed solution in the flask to 8-9, (v) accurately weighing 0.9930 g sodium borohydride and dissolving in 25 mL deionized water, (vii) preparing supported bimetallic nickel-palladium doped gallium oxide catalyst, and (viii) placing the obtained catalyst in a vacuum drying, and grinding. USE - Preparation of supported nickel-palladium bimetallic catalyst in oxidative coupling reaction (claimed). ADVANTAGE - The method enables preparation of supported nickel-palladium bimetallic catalyst having excellent dispersibility, catalytic activity, catalytic efficiency and stability, reduced agglomeration, conversion rate of 83%, and which is recycled for after 5 times. DETAILED DESCRIPTION - Preparation of supported nickel-palladium bimetallic catalyst involves (i) taking 10 mL 0.010-0.020 mol/L sodium chloropalladate , 10 mL 0.010-0.020 mol/L nickel chloride solution into 100 mL round bottom flask (A), magnetically stirring to completely and uniformly mixing sodium chloropalladate and nickel chloride to obtain solution which is transparent red-brown, (ii) adding 8-12 mg graphene oxide (GO) and 20 mL deionized water into a 100 mL round bottom flask (B), ultrasonically reacting for 1-2 hours until the graphene oxide is completely dissolved in the deionized water to obtain solution which is muddy yellow, (iii) gradually adding the graphene oxide aqueous solution in round-bottom flask (B) to round-bottom flask (A) at dropping rate of 50-65 drops per minute, performing ultrasonic treatment while dropping, continuously ultrasonically treating for 1-2 hours, uniformly mixing the graphene oxide aqueous solution with sodium chloropalladate and nickel chloride solution, (iv) using 1.0 mol/L sodium hydroxide solution to adjust the pH value of the mixed solution in the flask to 8-9, (v) accurately weighing 0.9930 g sodium borohydride and dissolving in 25 mL deionized water, (vi) placing the round bottom flask (A) in an oil bath for magnetic stirring at a speed of 1200 rpm, gradually increasing the oil bath temperature to 82-85 degrees C and the temperature rise rate of 3 degrees C/minute, suspending 1 mL 0.95-1.15 mol/L sodium borohydride solution on the mouth of round-bottom flask (A) with a 1 mL syringe, dripping 1 mL sodium borohydride solution into round-bottom flask (A) drop by drop within 30 minutes, gradually changing the solution from reddish brown and it turns black, heating the oil bath and magnetically stirring for 3-5 hours, cooling to room temperature and standing overnight, (vii) centrifuging the reaction solution in a centrifuge tube for 15-30 minutes, using a rubber-tip dropper to slowly remove the upper layer of the centrifuge tube and keep the bottom of the centrifuge tube, washing the precipitate with deionized water for 3 times and absolute ethanol for 3 times to completely remove other impurities in the precipitate, washing, centrifuging and removing the upper layer solution to obtain the supported bimetallic nickel-palladium doped gallium oxide catalyst, and (viii) placing the obtained catalyst in a vacuum drying oven at 60 degrees C for 24 hours, drying in a vacuum, and grinding into three times with a quartz mill into a fine black powder, and weighing for later use as a catalyst. An INDEPENDENT CLAIM is included for use of supported nickel-palladium bimetallic catalyst in oxidative coupling reaction, which involves weighing 3-10 mg nickel-palladium doped gallium oxide catalyst into the reaction tube with condensation device, adding 1-3 mL chlorobenzene (PhCl), placing in an ultrasonically processing for 8-15 minutes, and dispersing the nickel-palladium doped gallium oxide in solvent, adding 0.2 mmol 2-phenylbenzothiazole, 2 mL toluene and 15-26 mol% N-hydroxyphthalimide (NHPI), heating to 100-120 degrees C in an oil bath under an oxygen atmosphere, magnetically stirring for 20-28 hours and at a speed of 1200 rpm, and (c) using ethyl acetate as the extractant to extract the reaction product.