Nanosize Effect of Al2O3 in Ag/Al2O3 Catalyst for the Selective Catalytic Oxidation of Ammonia

被引:215
作者
Wang, Fei [1 ,2 ]
Ma, Jinzhu [1 ,2 ,3 ]
He, Guangzhi [1 ]
Chen, Min [1 ,2 ]
Zhang, Changbin [1 ,2 ]
He, Hong [1 ,2 ,3 ]
机构
[1] Chinese Acad Sci, Res Ctr Ecoenvironm Sci, State Key Joint Lab Environm Simulat & Pollut Con, Beijing 100085, Peoples R China
[2] Univ Chinese Acad Sci, Beijing 100049, Peoples R China
[3] Chinese Acad Sci, Inst Urban Environm, Ctr Excellence Reg Atmospher Environm, Xiamen 361021, Peoples R China
基金
中国国家自然科学基金; 国家重点研发计划;
关键词
ammonia (NH3); Ag/Al2O3; low-temperature oxidation; reaction pathway; N-2(-) mechanism; MIXED-METAL OXIDES; COPPER-BASED CATALYSTS; SILVER-BASED CATALYSTS; CU-MG-AL; LOW-TEMPERATURE; INFRARED-SPECTROSCOPY; SULFATE FORMATION; AG CATALYSTS; SLIP AMMONIA; FT-IR;
D O I
10.1021/acscatal.7b03799
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
Ammonia (NH3) has potentially harmful effects on human health and has recently been found to be an important factor in the formation of haze; thus, its emission control is urgent, especially during haze pollution periods. In this work, two kinds of Ag/Al2O3 catalysts with different Al2O3 particle sizes (micro-Al2O3 and nano-Al2O3) were prepared and tested for the selective catalytic oxidation of ammonia (NH3-SCO). It was shown that Ag/nano-Al2O3 was much more active than Ag/micro-Al2O3 for NH3-SCO in the low-temperature range. The results of characterization by BET, TEM, NH3-TPD, XRD, H-2-TPR, UV vis, and XAFS revealed that Ag/nano-Al2O3 possesses much smaller Ag particles and more metallic Ag species (Ag-NPs,) and also contains abundant acid sites, which facilitate the adsorption and dissociation of NH3, therefore resulting in much higher NH3-SCO activity. In addition, on the basis of in situ DRIFTS, kinetic measurements, and DFT calculation results, we discovered that the NH3-SCO reaction over Ag/nano-Al2O3 follows a reaction pathway we call the N-2(-) mechanism.
引用
收藏
页码:2670 / 2682
页数:25
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