Influence of ammonium nitrate on the crystallisation of ammonium sulfate.

This study aims to explore the influence mechanism of ammonium nitrate produced by ozone denitrification on the crystallisation of ammonium sulfate, a by-product of ammonia desulfurisation. The laser method was used to study the influence of ammonium nitrate on the solubility and metastable zone width of ammonium sulfate. An experiment on the influence of ammonium nitrate on the particle size of ammonium sulfate was designed, and the influence mechanism was explored through scanning electron microscopy and X-ray diffraction. The findings showed that the addition of ammonium nitrate increased the size and aspect ratio of ammonium sulfate crystals. The addition of ammonium nitrate inhibited the dissolution of ammonium sulfate and widened its metastable zone. The addition of ammonium nitrate covered the active sites of crystal nucleus growth, which inhibited the formation of crystal nuclei to a certain extent, and crystal growth dominated the crystallisation process. Moreover, the addition of ammonium nitrate induced the preferred orientation of the specific crystal plane of ammonium sulfate, and the addition of a small concentration of ammonium nitrate decreased the crystallinity of ammonium sulfate. The research results can provide a reference for crystallisation optimisation and quality improvement of ammonium sulfate in the ammonia desulfurisation process.

CO + NH3 coupling denitration at low temperatures over manganese/activated carbon catalysts.

To explore the mechanism of low-temperature carbon monoxide and ammonia (CO + NH3) coupling denitration of manganese/activated carbon (Mn/AC) catalysts, Mn/AC series catalysts were prepared using the impregnation method with AC activated by nitric acid as a precursor and manganese nitrate as a precursor. We characterized the surface morphology, pore structure, active component phase, functional group, and active component valence change law of the Mn/AC catalyst. The denitration rate order with different Mn loadings is 7Mn/AC > 9Mn/AC > 5Mn/AC. When the Mn loading was 7%, the catalyst's surface was smooth, with a good pore structure and uniform surface distribution of metal particles. These features increased the reacting gas's contact area, improving the denitration rate. The reason for this was oxygen chemisorption on the catalyst's surface. The Mn4+ and the number of oxygen-containing functional groups on the catalyst surface increase after Mn loading increases; this provides more active sites for denitration and promotes the reaction's conversion to fast selective catalytic reduction. The low-temperature CO + NH3 coupling denitration of Mn/AC catalysts conforms to the Langmuir-Hinshelwood mechanism when the temperature is lower than 230 °C and the Eley-Rideal mechanism when the temperature is higher than 230 °C. The research results can provide new ideas for low-temperature flue gas denitration.

Mechanism of Zn salt-induced deactivation of a Cu/activated carbon catalyst for low-temperature denitration via CO-SCR.

In the process of industrial flue gas denitration, the presence of heavy metals, especially Zn salts, is known to lead to the deactivation of the denitration catalysts. However, the specific mechanism of the catalyst deactivation remains unclear. In this paper, the mechanism of the ZnCl2- and ZnSO4-induced deactivation of low-temperature denitration catalysts in the carbon oxide (CO) selective catalytic reduction (CO-SCR) reaction was investigated using a Cu/activated carbon (AC) catalyst, in which HNO3/AC was used as the carrier. Cu/AC, ZnCl2-Cu/AC, and ZnSO4-Cu/AC catalysts were prepared by the incipient wetness impregnation method. The physicochemical properties of the catalyst were examined via the Brunauer-Emmett-Teller method, X-ray diffraction, X-ray photoelectron spectroscopy, and Fourier transform infrared spectroscopy analyses, which proved the mechanism of catalyst denitrification and enabled the elucidation of the toxicity mechanism of the Zn salts on the Cu/AC catalyst for CO-SCR denitration at low temperatures. The results show that Zn doping reduces the physical adsorption of CO and NO and decreases the concentration of Cu2+ and chemisorbed oxygen (Oß), leading to the reduction of active sites and oxygen vacancies, thus inhibiting the denitration reaction. Moreover, ZnCl2 is more toxic than ZnSO4 because Cl- not only occupies oxygen vacancies but also inhibits Oß migration. In contrast, SO4 2- increases the surface acidity and promotes Oß supplementation. This study can provide a reference for the development of CO-SCR denitration catalysts with high resistance to Zn salt poisoning.