Currently, activated coke is widely used in the removal of multiple pollutants from industrial flue gas. In this paper, a series of novel FexLayOz/AC catalysts was prepared by the incipient wetness impregnation for NH3-SCR denitrification reaction. The introduction of Fe-La bimetal oxides significantly improved the denitrification performance of activated coke at mid-high temperature, and 4% Fe0.3La0.7O1.5/AC exhibited a superior NOx conversion efficiency of 90.1% at 400 °C. The catalysts were further characterized by BET, SEM, XRD, Raman, EPR, XPS, FTIR, NH3-TPD, H2-TPR, et al., whose results showed that the perovskite-type oxide of LaFeO3 and oxygen vacancies were produced on the catalysts’ surfaces during roasting. Fe-La doping enhanced the amount of acid sites (mainly Lewis and other stronger acid sites) and the content of multifarious oxygen species, which were beneficial for NOx removal at mid-high temperature. Moreover, it was investigated that the effect of released CO from activated coke at mid-high temperature on the NOx removal through the lifetime test, in which it was found that a large amount of CO produced by pyrolysis of activated coke could promote the NOx removal, and long-term escaping of CO on the activated coke carrier did not have a significant negative impact on catalytic performance. The results of the TG-IR test showed that volatile matter is released from the activated coke while TG results showed that the weight loss rate of 4% Fe0.3La0.7O1.5/AC only was 0.0015~0.007%/min at 300–400 °C. Hence, 4% Fe0.3La0.7O1.5/AC had excellent thermal stability and denitrification performance to be continuously used at mid-high temperature. Finally, the mechanisms were proposed on the basis of experiments and characterization results.
Activated carbon was one of the main adsorptions utilized in elemental mercury (Hg0) removal from coal combustion flue gas. However, the high cost and low physical adsorption efficiency of activated carbon injection (ACI) limited its application. In this study, an ultra-high efficiency (nearly 100%) catalyst sorbent-Sex/Activated carbon (Sex/AC) was synthesized and applied to remove Hg0 in the simulated flue gas, which exhibited 120 times outstanding adsorption performance versus the conventional activated carbon. The Sex/AC reached 17.98 mg/g Hg0 adsorption capacity at 160 °C under the pure nitrogen atmosphere. Moreover, it maintained an excellent mercury adsorption tolerance, reaching the efficiency of Hg0 removal above 85% at the NO and SO2 conditions in a bench-scale fixed-bed reactor. Characterized by the multiple methods, including BET, XRD, XPS, kinetic and thermodynamic analysis, and the DFT calculation, we demonstrated that the ultrahigh mercury removal performance originated from the activated Se species in Sex/AC. Chemical adsorption plays a dominant role in Hg0 removal: Selenium anchored on the surface of AC would capture Hg0 in the flue gas to form an extremely stable substance-HgSe, avoiding subsequent Hg0 released. Additionally, the oxygen-containing functional groups in AC and the higher BET areas promote the conversion of Hg0 to HgO. This work provided a novel and highly efficient carbon-based sorbent -Sex/AC to capture the mercury in coal combustion flue gas.
To enhance the dispersion of active sites, modification of the AC supports with different acid solution might result in various surface oxygen groups which act as anchoring sites for metallic precursor to stay and improve the reactivity between AC supports and copper precursor. In the present work, the AC support is tailored with HCl and HNO(3), respectively. The pore structure, surface oxygen groups of the AC support and catalysts as well as catalyst dispersion before and after acid treatments are systematically studied by BET, pH(slurry), TPD, and XRPD analyses. It is found that the order of activity in DeSO(2) reaction is as follows: Cu/AC-HCl>Cu/AC>Cu/AC-HNO(3). The same sequence is also observed for the pore structure of AC supports, the catalyst dispersion, but not for the amounts of CO(2) evolving during TPD experiments of supports. The key role of acid treatment on carbon surface chemistry and pore structure, which are closely related to catalyst dispersion and adsorption capacity, is examined to rationalize these findings. Furthermore, under the NO/NH(3)=1 the NO could be selective catalytic reduction with NH(3) in the presence of O(2), which catalyzed by fresh and spent AC-supported catalyst. 相似文献
Recently, modification of surface structure of activated carbons in order to improve their adsorption performance toward especial pollutants has gained great interest. Oxygen-containing functional groups have been devoted as the main responsible for heavy metal binding on the activated carbon surface; their introduction or enhancement needs specific modification and impregnation methods. In the present work, olive stones activated carbon (COSAC) undergoes surface modifications in gaseous phase using ozone (O3) and in liquid phase using nitric acid (HNO3). The activated carbon samples were characterized using N2 adsorption–desorption isotherm, SEM, pHpzc, FTIR, and Boehm titration. The activated carbon parent (COSAC) has a high surface area of 1194 m2/g and shows a predominantly microporous structure. Oxidation treatments with nitric acid and ozone show a decrease in both specific surface area and micropore volumes, whereas these acidic treatments have led to a fixation of high amount of surface oxygen functional groups, thus making the carbon surface more hydrophilic. Activated carbon samples were used as an adsorbent matrix for the removal of Co(II), Ni(II), and Cu(II) heavy metal ions from aqueous solutions. Adsorption isotherms were obtained at 30 °C, and the data are well fitted to the Redlich–Peterson and Langmuir equation. Results show that oxidized COSACs, especially COSAC(HNO3), are capable to remove more Co(II), Cu(II), and Ni(II) from aqueous solution. Nitric acid-oxidized olive stones activated carbon was tested in its ability to remove metal ions from binary systems and results show an important maximum adsorbed amount as compared to single systems. 相似文献
Fe2O3 and CeO2 modified activated coke (AC) synthesized by the equivalent-volume impregnation were employed to remove elemental mercury (Hg0) from simulated flue gas at a low temperature. Effects of the mass ratio of Fe2O3 and CeO2, reaction temperature, and individual flue gas components including O2, NO, SO2, and H2O (g) on Hg0 removal efficiency of impregnated AC were investigated. The samples were characterized by Brunauer–Emmett–Teller (BET), X-ray diffraction (XRD), scanning electron microscopy (SEM), and X-ray photoelectron spectroscopy (XPS). Results showed that with optimal mass percentage of 3 % Fe2O3 and 3 % CeO2 on Fe3Ce3/AC, the Hg0 removal efficiency could reach an average of 88.29 % at 110 °C. Besides, it was observed that O2 and NO exhibited a promotional effect on Hg0 removal, H2O (g) exerted a suppressive effect, and SO2 showed an insignificant inhibition without O2 to some extent. The analysis of XPS indicated that the main species of mercury on used Fe3Ce3/AC was HgO, which implied that adsorption and catalytic oxidation were both included in Hg0 removal. Furthermore, the lattice oxygen, chemisorbed oxygen, and/or weakly bonded oxygen species made a contribution to Hg0 oxidation. 相似文献
The degradation of paracetamol in aqueous solutions in the presence of hydrogen peroxide was carried out by photochemistry, electrolysis and photoelectrolysis using modified 100 pores per inch reticulated vitreous carbon electrodes. The electrodes were coated with catalysts such as TiO2 and CuO/TiO2/Al2O3 by electrophoresis followed by heat treatment. The results of the electrolysis with bare reticulated vitreous carbon electrodes show that 90% paracetamol degradation occurs in 4 h at 1.3 V vs. SCE, forming intermediates such as benzoquinone and carboxylic acids followed by their complete mineralisation. When the electrolysis was carried out with the modified electrodes such as TiO2/RVC, 90% degradation was achieved in 2 h while with CuO/TiO2/Al2O3/RVC, 98% degradation took only 1 h. The degradation was also carried out in the presence of UV reaching 95% degradation with TiO2/RVC/UV and 99% with CuO/TiO2/Al2O3/RVC/UV in 1 h. The reactions were followed by spectroscopy UV-Vis, HPLC and total organic carbon analysis. These studies show that the degradation of paracetamol follows a pseudo-first order reaction kinetics. 相似文献