US 12,017,206 B2
Preparation method of Cu—Pd—CeO2/γ—Al2O3@NP catalyst and synthesis method of benzopyrazine compounds
Feng Feng, Zhejiang (CN); Xiaonian Li, Zhejiang (CN); Lingling Guo, Zhejiang (CN); Yanxia Sun, Zhejiang (CN); Chunshan Lu, Zhejiang (CN); Qunfeng Zhang, Zhejiang (CN); Jiatong Jin, Zhejiang (CN); and Xiaoliang Xu, Zhejiang (CN)
Assigned to ZHEJIANG UNIVERSITY OF TECHNOLOGY, Zhejiang (CN)
Filed by ZHEJIANG UNIVERSITY OF TECHNOLOGY, Zhejiang (CN)
Filed on Sep. 28, 2022, as Appl. No. 17/955,012.
Claims priority of application No. 202111160999.2 (CN), filed on Sep. 30, 2021.
Prior Publication US 2023/0095076 A1, Mar. 30, 2023
Int. Cl. C07D 241/42 (2006.01); B01J 21/04 (2006.01); B01J 23/89 (2006.01); B01J 37/00 (2006.01); B01J 37/02 (2006.01); B01J 37/04 (2006.01); B01J 37/08 (2006.01)
CPC B01J 23/894 (2013.01) [B01J 21/04 (2013.01); B01J 37/009 (2013.01); B01J 37/024 (2013.01); B01J 37/04 (2013.01); B01J 37/088 (2013.01); C07D 241/42 (2013.01)] 13 Claims
 
1. A preparation method of a Cu—Pd—CeO2/γ-Al2O3@NP catalyst, in the Cu—Pd—CeO2/γ-Al2O3@NP catalyst, a total loading amounts of N and P is 1.2%˜4.8%, a loading amount of Cu is 0.5%˜5 wt %, a loading amount of Pd is 0.5%˜5 wt %, and a loading amount of Ce is 5%˜15 wt %; the preparation method comprises the following steps:
(1) mixing γ-Al2O3 with deionized water, stirring the mixture to obtain a slurry, heating the slurry to 70-90° C., then adding a solution of cerium-containing compound, subjecting the mixture to stirring and impregnation at a constant temperature of 70-90° C. for 2˜6 h, adding ammonia water dropwise to adjust the pH value of the solution to 9˜10, continuing to stir the resulting solution at the constant temperature for 2-6 h, cooling it to room temperature and filtering it, washing the filter cake with deionized water until the filtrate becomes neutral, drying it at 80˜120° C. for 5˜9 h in the air, and then calcining it at 600˜800° C. for 2˜4 h in the air to obtain a CeO2/γ-Al2O3 carrier;
(2) mixing the CeO2/γ-Al2O3 carrier with an aqueous solution of ammonium phosphate, subjecting the mixture to stirring and impregnation at 30˜50° C. for 1˜3 hpurs, then drying it at 80-120° C. for 5˜9 h in the air, and then calcining the dried product at 400-600° C. for 1-3 hours in the air to obtain a CeO2/γ-Al2O3@NP carrier;
(3) mixing the CeO2/γ-Al2O3@NP carrier with deionized water, stirring the mixture to obtain a slurry, heated it to 60˜100° C., then adding certain amounts of a palladium-containing compound solution and a copper-containing compound solution, subjecting the mixture to stirring and impregnation at the constant temperature for 3˜7 h; cooling it to room temperature, adding an alkaline solution dropwise to adjust the pH value to 8˜10, stirring the resulting solution at the constant temperature for 0.5˜1.5 h, filtering it, washing the filter cake with deionized water until the filtrate becomes neutral; dry it at 80-120° C. in the air for 5-9 h; then calcining the dried product at 200-300° C. for 2-6 h in the air, and finally reducing the calcined product with hydrogen at 200-300° C. for 1˜3 h, thereby obtaining the Cu—Pd—CeO2/γ-Al2O3@NP catalyst.