MOF-74 as an Efficient Catalyst for the Low-Temperature Selective Catalytic Reduction of NOx with NH3

被引:237
作者
Jiang, Haoxi [1 ,2 ]
Wang, Qianyun [1 ,2 ]
Wang, Huiqin [1 ,2 ]
Chen, Yifei [1 ,2 ]
Zhang, Minhua [1 ,2 ]
机构
[1] Tianjin Univ, R&D Ctr Petrochem Technol, Minist Educ, Key Lab Green Chem Technol, Tianjin 300072, Peoples R China
[2] Collaborat Innovat Ctr Chem Sci & Engn, Tianjin 300072, Peoples R China
基金
中国国家自然科学基金;
关键词
metal-organic framework; MOF-74; selective catalytic reduction (SCR); DeNO(x); density functional theory (DFT); SO2; resistance; METAL-ORGANIC FRAMEWORKS; IRON(II) COORDINATION SITES; FT-IR; CARBON-DIOXIDE; SCR CATALYSTS; MIXED OXIDES; ADSORPTION; OXIDATION; AMMONIA; MECHANISM;
D O I
10.1021/acsami.6b08851
中图分类号
TB3 [工程材料学];
学科分类号
0805 ; 080502 ;
摘要
In this work, Mn-MOF-74 with hollow spherical structure and Co-MOF-74 with petal-like shape have been prepared successfully via the hydrothermal method. The catalysts were characterized using X-ray diffraction (XRD), Fourier transform infrared spectroscopy (FT-IR), thermogravimetry-mass spectrum analysis (TG-MS), N-2 adsorption/desorption, scanning electron microscopy (SEM), and X-ray photoelectron spectroscopy (XPS). It is found that MOF-74(Mn, Co) exhibits the capability for selective catalytic reduction (SCR) of NOx at low temperatures. Both experimental (temperature-programmed desorption, TPD) and computational methods have shown that Co-MOF-74 and Mn-MOF-74 owned high adsorption and activation abilities for NO and NH3. The catalytic activities of Mn-MOF-74 and Co-MOF-74 for low-temperature denitrification (deNO(x)) in the presence of NH3 were 99% at 220 degrees C and 70% at 210 degrees C, respectively. It is found that the coordinatively unsaturated metal sites (CUSs) in M-MOF-74 (M = Mn and Co) played important roles in SCR reaction. M-MOF-74 (M = Mn and Co), especially Mn-MOF-74, showed excellent catalytic performance for low-temperature SCR. In addition, in the reaction process, NO conversion on Mn-MOF-74 decreased with the introduction of H2O and SO2 and almost recovered when gas was cut off. However, for Co-MOP-74, SO2 almost has no effect on the catalytic activity. This work showed that MOF-74 could be used prospectively as deNO(x) catalyst.
引用
收藏
页码:26817 / 26826
页数:10
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