采用合成交换法成功制备双金属铜基有机金属骨架材料Alx/HKUST-1(x=1/24,1/12,1/6,1/3),并采用X射线衍射(XRD)、扫描电子显微镜(SEM)、比表面积分析(BET)、热重分析(TG)、红外光谱(IR)、X射线光电子能谱(XPS)以及H2程序升温还原(H2-TPR)技术对其进行表征.研究结果表明,Alx/HKUST-1维持前躯体(HKUST-1)的正八面体结构,掺铝(Al3+)后,HKUST-1的热稳性和还原性能均得到提高.Al1/12/HKUST-1表现出最佳的催化活性,温度为210℃时,催化脱硝率达到100%,相比HKUST-1降低了50℃.催化反应后,Al1/12/HKUST-1中Al、Cu和O的价态种类没有发生改变,但是不同价态的Al、Cu和O的含量比值发生了明显变化.Alx/HKUST-1的催化过程遵循Langmuir?Hinshelwood反应机理.
Alx/HKUST-1(x=1/24, 1/12, 1/6, 1/3), one of the bimetallic copper-based organic framework materials, was successfully prepared by the synthetic exchange method and characterized by X-ray diffraction (XRD), scanning electron microscopy (SEM), specific surface area (BET), thermogravimetric analysis (TG), infrared spectra (IR), X-ray photoelectron spectroscopy (XPS), and H2-temperature programmed reduction (H2-TPR). The findings indicated that Alx/HKUST-1 maintained the octahedral morphology of its precursor (HKUST-1). The thermal stability and catalytic reduction ability of HKUST-1 skeleton were improved by doping aluminum (Al3+). Al1/12/HKUST-1 showed the best performance among all samples, with a nitric oxide (NO) conversion rate of 100% at 210 ℃ (50 ℃ lower than that of HKUST-1). The valence kind of Al, Cu, and O in Al1/12/HKUST-1 did not change after the catalytic reaction, but the contents of Al, Cu, and O in different forms changed significantly. The catalytic process of the Alx/HKUST-1 followed a Langmuir?Hinshelwood mechanism.