Novel Cs-Mg-Al mixed oxide with improved mobility of oxygen species for passive NO_(x)adsorption

The development of passive NO_(x)adsorbers with cost-benefit and high NO_(x)storage capacity remains an on-going challenge to after-treatment technologies at lower temperatures associated with cold-start NO_(x)emissions.Herein,Cs_(1)Mg_(3)Al catalyst prepared by sol-gel method was cyclic tested in NO_(x)storage under 5 vol%water.At 100°C,the NO_(x)storage capacity(1219 μmol g^(-1))was much higher than that of Pt/BaO/Al_(2)O_(3)(610 μmol g^(-1)).This provided new insights for non-noble metal catalysts in low-temperature passive NO_(x)adsorption.The addition of Cs improved the mobility of oxygen species and thus improved the NO_(x)storage capacity.The XRD,XPS,IR spectra and in situ DRIFTs with NH3 probe showed an interaction between CsO_(x)and AlO_(x)sites via oxygen species formed on Cs_(1)Mg_(3)Al catalyst.The improved mobility of oxygen species inferred from O2-TPD was consistent with high NO_(x)storage capacity related to enhanced formation of nitrate and additional nitrite species by NO_(x)oxidation.Moreover,the addition of Mg might improve the stability of Cs_(1)Mg_(3)Al by stabilizing surface active oxygen species in cyclic experiments.

The effect of cations(NH_4^+,Na^+,K^+,and Ca^(2+)) on chemical deactivation of commercial SCR catalyst by bromides

Alkali and alkaline‐earth metals from fly ash have a significant deactivation effect on catalysts used for selective catalytic reduction of NOx by NH3(NH3‐SCR).Bromides are considered effective additives to improve Hg0 oxidation on SCR catalysts.In this work,the effects of different bromides(NH4Br,NaBr,KBr,and CaBr2)on a commercial V2O5‐WO3/TiO2 catalyst were studied.NOx conversion decreased significantly over the KBr‐poisoned catalyst(denoted as L‐KBr),while that over NaBr‐and CaBr2‐poisoned catalysts(denoted as L‐NaBr and L‐CaBr,respectivity)decreased to a lesser extent compared with the fresh sample.Poor N2 selectivity was observed over L‐NaBr,L‐KBr and L‐CaBr catalysts.The decrease in the ratio of chemisorbed oxygen to total surface oxygen(Oα/(Oα+Oβ+Ow)),reducibility and surface acidity might contribute to the poor activity and N2 selectivity over L‐KBr catalyst.The increased Oαratio was conducive to the enhanced reducibility of L‐CaBr.Combined with enhanced surface acidity,this might offset the negative effect of the loss of active sites by CaBr2 covering.The overoxidation of NH3 and poor N2 selectivity in NH3 oxidation should retard the SCR activity at high temperatures over L‐CaBr catalyst.The increased basicity might contribute to increased NOx adsorption on L‐KBr and L‐CaBr catalysts.A correlation between the acid‐basic and redox properties of bromide‐poisoned catalysts and their catalytic properties is established.

Catalytic oxidation of CO over Pt/Fe3O4 catalysts:Tuning O2 activation and CO adsorption

The self-inhibition behavior due to CO poisoning on Pt metal particles strongly impairs the performance of CO oxidation.It is an effective method to use reducible metal oxides for supporting Pt metal particles to avoid self-inhibition and to improve catalytic performance.In this work,we used in situ reductions of chloroplatinic acid on commercial Fe3O4 powder to prepare heterogeneousstructured Pt/Fe3O4 catalysts in the solution of ethylene glycol.The heterogeneous Pt/Fe3O4 catalysts achieved a better catalytic performance of CO oxidation compared with the Fe3O4 powder.The temperatures of 50%and 90%CO conversion were achieved above 260℃and 290℃at Pt/Fe3O4,respectively.However,they are accomplished on Fe3O4 at temperatures higher than 310℃.XRD,XPS,and H2-TPR results confirmed that the metallic Pt atoms have a strong synergistic interaction with the Fe3O4 supports.TGA results and transient DRIFTS results proved that the Pt metal particles facilitate the release of lattice oxygen and the formation of oxygen vacancies on Fe3O4.The combined results of O2-TPD and DRIFTS indicated that the activation step of oxygen molecules at surface oxygen vacancies could potentially be the rate-determining step of the catalytic CO oxidation at Pt/Fe3O4 catalysts.The reaction pathway involves a Pt-assisted Mars-van Krevelen(MvK)mechanism.

Chemical poison and regeneration of SCR catalysts for NOx removal from stationary sources

Selective catalytic reduction （SCR） of NOx with NH3 is an effective technique to remove NOx from stationary sources, such as coal-fired power plant and industrial boilers. Some of elements in the fly ash deactivate the catalyst due to strong chemisorptions on the active sites. The poisons may act by simply blocking active sites or alter the adsorption behaviors of reactants and products by an electronic interaction. This review is mainly focused on the chemical poisoning on V2O5-based catalysts, environmental-benign catalysts and low temperature catalysts. Several common poisons including alkali/alkaline earth metals, SO2 and heavy metals etc. are referred and their poisoning mechanisms on catalysts are discussed. The regeneration methods of poisoned catalysts and the development of poison-resistance catalysts are also compared and analyzed. Finally, future research directions in developing poisoning resistance catalysts and facile efficient regeneration methods for SCR catalysts are proposed.