PdCl2-CuCl2/Li-Al-O催化CO和亚硝酸乙酯合成碳酸二乙酯的研究  

Synthesis of diethyl carbonate from CO and ethyl nitrite over PdCl_2-CuCl_2/Li-Al-O

作　　者：李文龙[1] 董玲玉[1] 李扬[1] 刘亚华[1] 袁小金[1] 王科[1] 

机构地区：[1]西南化工研究设计院有限公司,国家碳一化学工程技术研究中心,工业排放气综合利用国家重点实验室,四川成都610225

出　　处：《天然气化工—C1化学与化工》2017年第2期1-4,共4页Natural Gas Chemical Industry

摘　　要：通过LiNO_3对γ-Al_2O_3改性并进行PdCl_2和CuCl_2负载,制备了PdCl_2-CuCl_2/Li-Al-O催化剂,同时采用固定床反应器考察了催化剂对CO低压气相合成碳酸二乙酯的催化性能,探讨了载体n(Li)/n(Al),不同溶剂,Pd、Cu负载量及浸渍方式对催化剂催化性能的影响。结果表明,Li的添加能够提高催化剂的催化活性,最佳的n(Li)/n(Al)为0.15;选用0.1M的盐酸或者稀氨水做活性组分的溶剂来制备催化剂,同样能提高催化剂的活性;金属Pd负载的质量分数为2%,n(Cu)/n(Pd)=1时,催化剂的性能最佳,而浸渍方式对催化剂活性影响不大。The Li-Al-O spinel supports were synthesized by modifying γ-Al2O3 with Li＋, then the PdCl2-CuCl2/Li-Al-O catalysts were prepared by introducing PdCl2 and CuCl2 to the Li-Al-O spinel supports. The effects of preparation conditions including the Li/ Al mole ratios, solvents, Cu and Pd loadings and impregnation methods on the catalytic performances of the catalysts in low pressure vapor-phase synthesis of diethyl carbonate from CO and ethyl nitrite were investigated by evaluating their catalytic activity in a continuous fixed-bed reactor. The results showed that adding Li^＋ improved the catalytic activity, and the optimized Li/Al mole ratio was of 0.15. Using 0.1M HCl or 0.1M NH3· H2O as solvent also increased the catalytic activity. Suitable Pd-loading was 2% by mass, and the optimized Cu/Pd mole ratio was of 1, while the impregnation methods had little effect on the activity of catalyst.

关 键 词：碳酸二乙酯 合成 Pd-Cu催化剂 锂铝尖晶石载体 亚硝酸乙酯 

分 类 号：O643.3[理学—物理化学] TQ426[理学—化学]