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研究论文

胡晴,赵玲,张浩龙,段曌,白依静,袁海洋,郭怀成.金属有机骨架材料MOF-5利用C₃H₆选择性催化还原NO的研究[J].环境科学学报,2020,40(3):819-826

Study on the selective catalytic reduction of NO by C₃H₆ with metal organic material MOF-5

摘要：采用溶剂热法在不同温度（120、150、180℃）、不同时间（12、24、48 h）条件下制备MOF-5催化剂，利用热重分析仪（TG）、X射线衍射仪（XRD）、傅立叶红外光谱仪（FT-IR）对其进行表征，研究不同条件下MOF-5样品的水热稳定性及特征官能团、化学键等指标.结果表明，利用溶剂热法制备的MOF-5样品稳定性良好，390℃结构开始坍塌.对比FT-IR、XRD等表征结果，选择图线形状最好、出峰位置最多的120℃、24 h条件下的MOF-5样品作为载体，对其进行了Cu的负载，负载量依次为1%、3%、5%.根据TG曲线，选择在MOF-5维持稳定结构、同时与尾气排放环境中的温度较为接近的350℃作为反应温度，利用傅立叶原位红外技术考察不同负载量的Cu-MOF-5在不同温度条件下对NO吸附能力大小、吸附过程中间物的变化情况，初步研究以C₃H₆作为还原剂时的富氧HC-SCR反应的机理.根据原位红外反应结果看出，NO₃^-、—CNO、—CN是重要的中间产物，且以3% Cu负载量的催化剂中间产物变化最为丰富，催化效果最优.

Abstract：MOF-5 catalyst was prepared by solvothermal method at different temperature and time conditions. It was characterized using thermogravimetric analyzer (TG), X-ray diffractometer (XRD) and Fourier transform infrared spectroscopy (FT-IR). The prepared MOF-5 catalyst showed well hydrothermal stability. Their structure began to collapse at 390℃. Compared with FT-IR and XRD results, MOF-5 samples with the best shape and the most peak position were selected as the carrier at 120℃ and 24 hours. The Cu loading was 1%, 3% and 5% respectively. According to the TG curve, 350℃ is selected as the reaction temperature. Fourier in situ infrared technology is used to investigate the adsorption capacity of Cu-MOF-5 with different loading amount under different temperature conditions. C₃H₆ is regard as the reducing agent for the oxygen rich HC-SCR reaction. Furthermore, in situ FTIR experiments revealed that NO₃^-, -CNO, -CN are important intermediates. It is demonstrated that 3% Cu-MOF-5 exhibited the most abundant intermediates and the best catalytic activity.

Key words：metal-organic frameworks NO In situ FTIR selective catalytic reduction (SCR)