Petros G. Savva

Novel catalytic and mechanistic studies on wastewater denitrification with hydrogen

The present work reports up-to-date information regarding the reaction mechanism of the catalytic hydrogenation of nitrates in water media. In the present mechanistic study, an attempt is made, for the first time, to elucidate the crucial role of several catalysts and reaction parameters in the mechanism of the NO(3)(-)/H(2) reaction. Steady-state isotopic transient kinetic analysis (SSITKA) experiments coupled with ex situ diffuse reflectance infrared Fourier transform spectroscopy (DRIFTS) were performed on supported Pd-Cu catalysts for the NO(3)(-)/H(2) and NO(3)(-)/H(2)/O(2) reactions. The latter experiments revealed that the formation and surface coverage of various adsorbed active intermediate N-species on the support or Pd/Cu metal surface is significantly favored in the presence of TiO(2) in the support mixture and in the presence of oxygen in the reactions gaseous feed stream. The differences in the reactivity of these adsorbed N-species, found in the present work, adequately explain the large effect of the chemical composition of the support and the gas feed composition on catalyst behaviour (activity and selectivity). The present study leads to solid mechanistic evidence concerning the presence of a hydrogen spillover process from the metal to the support. Moreover, this study shows that Cu clusters are active sites for the reduction of nitrates to nitrites.

The effect of several parameters on catalytic denitrification of water by the use of H2 in the presence of O2 over metal supported catalysts.

The present paper involves a detailed study of the selective catalytic reduction of nitrates in aqueous mediums by the use of H2 in the presence of O2 over monometallic and bimetallic supported catalysts. In this study, an attempt has been made to improve the denitrification efficiency (XNO3(-), SN2) of several catalysts by regulating some experimental parameters that are involved in the process. Therefore, the effects of the type of reactor (semi-batch reactor vs continuous flow reactor), the nature of the active phase (Pd, Cu, and Pd-Cu) and the particle size of γ-Al2O3 spheres (particle diameter = 1.8 mm and 3 mm) on catalytic activity and reaction selectivity, as well as the adsorption capacity of γ-Al2O3 spheres for nitrates, were examined. As the review indicates, most of the research has so far been conducted on batch or semi-batch reactors. This study successfully demonstrates the benefits of using a continuous flow reactor in terms of catalytic activity (XNO3(-), %) and reaction selectivity (SN2, %). Another important aspect of this study is the crucial role of bimetallic Pd-Cu clusters for the prevention of NH4(+) formation. Moreover, the use of 1.8 mm diameter γ-Al2O3 spheres as a support was proved to significantly enhance the catalytic performance of bimetallic Pd-Cu catalysts towards nitrate reduction compared to 3 mm diameter γ-Al2O3 spheres. This difference may be attributed to mass (NO3(-), OH(-)) transfer effects (external mass transfer phenomena).

Catalytic removal of pharmaceutical compounds in water medium under an H2 stream over various metal-supported catalysts: A promising process

To date, very few prescriptive studies have been reported in the literature concerning the catalytic removal of pharmaceutical substances in wastewater using H2 in the presence of O2 for the in situ formation of H2O2, while the mechanism of the reaction has not been studied in detail yet. Hydrogen peroxide is a potent oxidizing agent used extensively in catalytic wet air oxidation (CWAO) applications and can be used for the elimination of pharmaceuticals from waste water. In the present work, an attempt has been made to elucidate the actual effects of the in situ production of hydrogen peroxide on the CWAO of pharmaceuticals. Therefore, the effects of the nature of the active phase (Pd, Pt, and Rh), as well as the feed gas composition have been examined toward the reaction at hand. The results showed that 1% Pd/Al2O3 and 1% Rh/Al2O3 are the most effective catalysts for the elimination of paracetamol from the reaction medium using hydrogen-rich streams, having a conversion of up to 70% in 2 h. A maximum conversion of paracetamol of 90% was obtained in just 30 min of reaction over 1 wt.% Rh/Al2O3, when using pure hydrogen in the feed. Total organic carbon measurements performed over the latter catalyst showed that practically no organic carbon is removed from the liquid phase, indicating the conversion of paracetamol to a different organic (probably aromatic) compound, through hydrogenation. Toxicity tests that followed showed a dramatic decrease in the toxicity of the products solution, indicating that paracetamol hydrogenation might be a promising method for the elimination of its toxicity.

The new concept of antimicrobial catalysis: disinfection of ships ballast water

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