Heteropoly acids (HPAs) have been effectively utilized in selective catalytic reduction (SCR) of NO to improve the NH 3 absorption capacity and alkaline/alkali metal resistance for SCR catalysts. However, despite the promise on super-acidities, their other properties that would work on SCR process are still lack of exploration. In this study, a 12-tungstaphosphoric acid (H 3 PW 12 O 40 , HPW) was selected to modify a well-reported CeO 2 catalyst. The resulted CeO 2 /HPW catalyst was subsequently utilized for SCR of NO with excess NH 3 , which revealed a significantly promoted performance in SCR reaction. DRIFT analyses showed that the unique NO 2 absorption capacity of HPW could prevent the NO 2 being further oxidized into nitrate species and the abundant Brønsted acid sites could effectively retain the NH 3 , avoiding them being over-oxidized at evaluated temperatures. The presence of NO 2 was demonstrated able to induce a so called “fast SCR” reaction over the CeO 2 /HPW catalyst, which effectively facilitated the SCR reaction. Furthermore, we have also constructed a CeO 2 @HPW catalyst, which showed an enhanced SO 2 poisoning resistance in SCR reaction.
Junli Wang,Shaojuan Zeng,Feng Huo,Dawei Shang,Hongyan He,Lu Bai,Xiangping Zhang,Jianwei Li
A large number of NH 3 emissions from industries, such as ammonia plant purge gas , tail gases of urea plants and ammonium molybdate plants, inevitably cause serious air pollution problems, such as fog and haze, which has raised extensive attentions worldwide. However, the commercial methods, like water scrubbing and acid scrubbing, substantially transfer the NH 3 pollute from gas phase to liquid or solid phase, which does not mean total elimination. How to realize efficiently separate and recover NH 3 form NH 3 -containing gas mixtures is still a great challenge. In order to develop efficient absorbents for NH 3 removal, a series of metal (copper (Cu), stannum (Sn), nickel (Ni), manganese (Mn), cadmium (Cd), zinc (Zn), ferrum (Fe)) ionic liquids (MILs) were synthesized, and their physicochemical properties and NH 3 absorption performance were systematically investigated. The results implied that the incorporation of metal center into ILs has a great effect on NH 3 absorption. Among the investigated MILs, bis(1-butyl-3-methyl imidazolium) copper tetrachloride salt ([Bmim] 2 [CuCl 4 ]) and bis(1-butyl-3-methyl imidazolium) stannum tetrachloride salt ([Bmim] 2 [SnCl 4 ]) show excellent NH 3 absorption capacities up to 0.172 gNH 3 ·gIL −1 and 0.106 gNH 3 ·gIL −1 , respectively, which are far more than most of the conventional ILs. Moreover, the high selectivity for NH 3 /N 2 , NH 3 /CO 2 and NH 3 /O 2 of [Bmim] 2 [CuCl 4 ] and [Bmim] 2 [SnCl 4 ] indicated that these MILs can selectively separate NH 3 from NH 3 -containing gases. The absorption mechanism was further studied using Fourier transform infrared (FT-IR) spectroscopy and quantitative chemical calculations. It was demonstrated that the chemical complexation between [Bmim] 2 [CuCl 4 ] and NH 3 plays a dominant role in NH 3 absorption, but the stronger hydrogen bonding between [Bmim] 2 [SnCl 4 ] and NH 3 enhances the absorption performance. In addition, [Bmim] 2 [SnCl 4 ] can keep good stability after five absorption and desorption cycles, implying this MIL shows great potentials as an efficient and reversible absorbent for NH 3 capture applications.
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