基于Cu-HKUST-1材料的Cu/Cu_2O/CuO三元复合催化剂的优化制备及其应用研究

Preparation of Cu/Cu_2O/CuO composite catalyst based on Cu-HKUST-1 and its application

以硝酸铜,均苯三甲酸为原料,采用溶剂热合成法首先制备了铜基金属有机骨架材料(Cu-HKUST-1),然后采用气氛焙烧法制备了一系列三元铜基复合催化剂(Cu/Cu_2O/CuO)。通过调控灼烧时氮气和空气的配合比,实现了Cu/Cu_2O/CuO中铜(Cu)、氧化亚铜(Cu_2O)和氧化铜(CuO)三相含量的调控。研究结果表明:Cu/Cu_2O/CuO中的Cu、Cu_2O和CuO三者比列含量微观可调,随着空气比例微量增加,Cu/Cu_2O/CuO中Cu的含量逐渐减少,Cu_2O和CuO含量明显增多,通过气氛调节可以实现Cu、Cu_2O和CuO三相配合比的优化组合。在对对硝基苯酚还原实验中,在氮气∶空气的配合比为200mL∶2mL条件下制备的Cu/Cu_2O/CuO催化效果最好,反应约45s对对硝基苯酚的降解率超过90%。

Cu-HKUST-1 was prepared by a solvothermal method using copper nitrate and trimesic acid.Then a series of Cu/Cu2O/CuO ternary copper-based composite catalysts were prepared by sintering Cu-HKUST-1 under different atmospheres.By changing the proportion of nitrogen and oxygen in annealing gas,the content of Cu,Cu2O and CuO in Cu/Cu2O/CuO catalysts can be effectively adjusted.The results showed that Cu,Cu2O and CuO in catalysts can be rationally modulated,i.e.,the trace increase of air in annealing stream can lead to the decreasing of Cu,whereas the content of Cu2O and CuO increased.The optimization of Cu,Cu2O and CuO can be realized by adjusting the annealing atmosphere.In the catalytic reduction of p-nitrophenol,the optimized Cu/Cu2O/CuO catalysts（N2∶Air=200 mL∶2 mL）exhibited the highest catalytic activity and it took 45 sto obtain a conversion rate of above 90%.