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1.
RSC Adv ; 14(7): 4575-4586, 2024 Jan 31.
Artigo em Inglês | MEDLINE | ID: mdl-38318608

RESUMO

Efficient carbon monoxide oxidation is important to reduce its impacts on both human health and the environment. Following a sustainable synthesis route toward new catalysts, nanosized Co3O4 was synthesized based on extracts of microalgae: Spirulina platensis, Chlorella vulgaris, and Haematococcus pluvialis. Using the metabolites in the extract and applying different calcination temperatures (450, 650, 800 °C) led to Co3O4 catalysts with distinctly different properties. The obtained Co3O4 nanomaterials exhibited octahedral, nanosheet, and spherical morphologies with structural defects and surface segregation of phosphorous and potassium, originating from the extracts. The presence of P and K in the oxide nanostructures significantly improved their catalytic CO oxidation activity. When normalized by the specific surface area, the microalgae-derived catalysts exceeded a commercial benchmark catalyst. In situ studies revealed differences in oxygen mobility and carbonate formation during the reaction. The obtained insights may facilitate the development of new synthesis strategies for manufacturing highly active Co3O4 nanocatalysts.

2.
Top Catal ; 66(19-20): 1539-1552, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-37830054

RESUMO

Syngas can be produced from biomethane via Partial Oxidation of Methane (POM), being an attractive route since it is ecofriendly and sustainable. In this work, catalysts of Ni supported on MgO-ZrO2 solid solutions, prepared by a one-step polymerization method, were characterized by HRTEM/EDX, XRD, XPS, H2-TPR, and in situ XRD. All catalysts, including Ni/ZrO2 and Ni/MgO as reference, were tested for POM (CH4:O2 molar ratio 2, 750 ºC, 1 atm). NiO/MgO/ZrO2 contained two solid-solutions, MgO-ZrO2 and NiO-MgO, as revealed by XRD and XPS. Ni (30 wt%) supported on MgO-ZrO2 solid solution exhibited high methane conversion and hydrogen selectivity. However, depending on the MgO amount (0, 4, 20, 40, 100 molar percent) major differences in NiO reducibility, growth of Ni0 crystallite size during H2 reduction and POM, and in carbon deposition rates were observed. Interestingly, catalysts with lower MgO content achieved the highest CH4 conversion (~ 95%), high selectivity to H2 (1.7) and CO (0.8), and low carbon deposition rates (0.024 g carbon.gcat-1 h-1) with Ni4MgZr (4 mol% MgO) turning out to be the best catalyst. In situ XRD during POM indicated metallic Ni nanoparticles (average crystallite size of 31 nm), supported by MgO-ZrO2 solid solution, with small amounts of NiO-MgO being present as well. The presence of MgO also influenced the morphology of the carbon deposits, leading to filaments instead of amorphous carbon. A combustion-reforming mechanism is suggested and using a MgO-ZrO2 solid solution support strongly improves catalytic performance, which is attributed to effective O2, CO2 and H2O activation at the Ni/MgO-ZrO2 interface.

3.
Ind Eng Chem Res ; 62(40): 16254-16267, 2023 Oct 11.
Artigo em Inglês | MEDLINE | ID: mdl-37841414

RESUMO

The greenhouse gas reduction as well as the utilization of more renewable and clean energy via a dry reforming reaction is of interest. The impact of a CeMgZnAl oxide quad-blend-supported Ni catalyst on performance and anticoking during dry reforming reactions at 700 °C was studied. A high Ce-Mg/Zn ratio, as seen in the CeMg0.5ZnAl-supported nickel catalyst, enhances lattice oxygen, and the presence of strong basic sites, along with the creation of the carbonate intermediate species, is accompanied by the production of gaseous CO through a gasification reaction between the carbon species and Ni-COads-lin site. The phenomena caused the outstanding performance of the Ni/CeMg0.5ZnAl catalyst-CH4 (84%),CO2 (83%) conversions, and the H2/CO (0.80) ratio; moreover, its activity was also stable throughout 30 h.

4.
Top Catal ; 66(15-16): 1129-1142, 2023.
Artigo em Inglês | MEDLINE | ID: mdl-37724312

RESUMO

As supported CuO is well-known for low temperature activity, CuO/CeO2 nanosphere catalysts were synthesized and tested for CO oxidation and preferential oxidation of CO (PROX) in excess H2. For the first reaction, ignition was observed at 95 °C, whereas selective PROX occurred in a temperature window from 50 to 100 °C. The catalytic performance was independent of the initial oxidation state of the catalyst (CuO vs. Cu0), suggesting that the same active phase is formed under reaction conditions. Density functional modeling was applied to elucidate the intermediate steps of CO oxidation, as well as those of the comparably less feasible H2 transformation. In the simulations, various Cu and vacancy sites were probed as reactive centers enabling specific pathways. Supplementary Information: The online version contains supplementary material available at 10.1007/s11244-023-01848-x.

5.
ACS Omega ; 8(12): 11364-11372, 2023 Mar 28.
Artigo em Inglês | MEDLINE | ID: mdl-37008144

RESUMO

Monitoring the disinfection process and swimming pool water quality is essential for the prevention of microbial infections and associated diseases. However, carcinogenic and chronic-toxic disinfection by-products (DBPs) are formed with reactions between disinfectants and organic/inorganic matters. DBP precursors in swimming pools originate from anthropogenic sources (body secretions, personal care products, pharmaceuticals, etc.) or chemicals used in pools. Temporal (48 weeks) water quality trends of trihalomethanes (THMs), haloacetic acids (HAAs), haloacetonitriles (HANs), and halonitromethanes (HNMs) in two swimming pools (SP-A and SP-B) and precursor-DBP relationships were investigated in this study. Weekly samples were taken from swimming pools, and several physical/chemical water quality parameters, absorbable organic halides (AOX), and DBPs were determined. THMs and HAAs were the most detected DBP groups in pool water. While chloroform was determined to be the dominant THM compound, dichloroacetic acid and trichloroacetic acid were the dominant HAA compounds. The average AOX concentrations were measured to be 304 and 746 µg/L as Cl- in SP-A and SP-B, respectively. Although the amount of AOX from unknown chlorinated by-products in SP-A did not vary temporally, a significant increase in unknown DBP concentrations in SP-B was observed over time. AOX concentrations of chlorinated pool waters were determined to be an important parameter that can be used to estimate DBP concentrations.

6.
Catal Sci Technol ; 13(3): 624-636, 2023 Feb 06.
Artigo em Inglês | MEDLINE | ID: mdl-36760342

RESUMO

The sensing of volatile organic compounds by composites containing metal oxide semiconductors is typically explained via adsorption-desorption and surface electrochemical reactions changing the sensor's resistance. The analysis of molecular processes on chemiresistive gas sensors is often based on indirect evidence, whereas in situ or operando studies monitoring the gas/surface interactions enable a direct insight. Here we report a cross-disciplinary approach employing spectroscopy of working sensors to investigate room temperature methanol detection, contrasting well-characterized nanocomposite (TiO2@rGO-NC) and reduced-graphene oxide (rGO) sensors. Methanol interactions with the sensors were examined by (quasi) operando-DRIFTS and in situ-ATR-FTIR spectroscopy, the first paralleled by simultaneous measurements of resistance. The sensing mechanism was also studied by mass spectroscopy (MS), revealing the surface electrochemical reactions. The operando and in situ spectroscopy techniques demonstrated that the sensing mechanism on the nanocomposite relies on the combined effect of methanol reversible physisorption and irreversible chemisorption, sensor modification over time, and electron/O2 depletion-restoration due to a surface electrochemical reaction forming CO2 and H2O.

7.
Environ Technol ; : 1-10, 2022 Jul 25.
Artigo em Inglês | MEDLINE | ID: mdl-35849543

RESUMO

Sustainable operation is an essential challenge in many municipal wastewater treatment plants. Among many types of wastewater mixed in a sewer, healthcare wastewaters need special attention due to their hazardous substance content, which can be toxic to activated sludge. This study compared the acute inhibitory effects of healthcare wastewaters (HW) and medical laboratory wastewater (MLW) on conventional activated sludge (CAS) and membrane bioreactor (MBR). The sensitivity test showed that nitrifying bacteria (NBs) in MBR sludge have higher resistance to acute toxicity than the CAS. Compared with HW, MLW caused much higher inhibition on both sludges. When the ratio of HW in the tested domestic wastewater was 10%, inhibition of NBs was 39% in AS, while it was 31% in MBR. When the ratio of MLW in the tested domestic wastewater was only 10%, 72% of NBs in AS and 57% of NBs in MBR were already inhibited. The higher resistance of NB in MBR may be explained by the diversity of microorganisms in the MBR operated at high sludge ages. The findings of this study may be used to estimate the acute inhibition effect of HW and MLW discharged directly to the sewage at higher loads.

8.
J Phys Condens Matter ; 34(35)2022 Jun 29.
Artigo em Inglês | MEDLINE | ID: mdl-35588721

RESUMO

Co3O4is a well-known low temperature CO oxidation catalyst, but it often suffers from deactivation. We have thus examined room temperature (RT) CO oxidation on Co3O4catalysts by operando DSC, TGA and MS measurements, as well as by pulsed chemisorption to differentiate the contributions of CO adsorption and reaction to CO2. Catalysts pretreated in oxygen at 400 °C are most active, with the initial interaction of CO and Co3O4being strongly exothermic and with maximum amounts of CO adsorption and reaction. The initially high RT activity then levels-off, suggesting that the oxidative pretreatment creates an oxygen-rich reactive Co3O4surface that upon reaction onset loses its most active oxygen. This specific active oxygen is not reestablished by gas phase O2during the RT reaction. When the reaction temperature is increased to 150 °C, full conversion can be maintained for 100 h, and even after cooling back to RT. Apparently, deactivating species are avoided this way, whereas exposing the active surface even briefly to pure CO leads to immediate deactivation. Computational modeling using DFT helped to identify the CO adsorption sites, determine oxygen vacancy formation energies and the origin of deactivation. A new species of CO bonded to oxygen vacancies at RT was identified, which may block a vacancy site from further reaction unless CO is removed at higher temperature. The interaction between oxygen vacancies was found to be small, so that in the active state several lattice oxygen species are available for reaction in parallel.

9.
Environ Sci Pollut Res Int ; 29(33): 50256-50270, 2022 Jul.
Artigo em Inglês | MEDLINE | ID: mdl-35226271

RESUMO

In this study, copper recovery and sensor integration for concentrate flows of membrane processes were studied. In the first phase, cementation tests for copper recovery were carried out with various different Fe/Cu stoichiometric ratios, copper concentrations, temperatures, and stirring speeds. The effects of the parameters which were stirring speed, temperature, stoichiometric ratio, and concentration in the solution on the cementation process were determined. In the second phase, a novel electroanalytical sensor was applied to concentrate flow. The application of cementation within the scope of precious metal recovery from concentrate streams by integrating a sensor to the process as an innovative online-sensing-approach is conducted. Four different copper concentrations (64, 128, 512, 1280 mg/L) and 5 different Fe/Cu stoichiometric ratios for these concentrations were studied. For concentrations of 64 mg/L and 128 mg/L, 1/1, 2/1, 5/1, 7/1, 10/1 Fe/Cu ratios and for both 512 mg/L and 1280 mg/L concentrations, 1/1, 1.25/1, 1.5/1, 1.75/1, 2/1 Fe/Cu ratios were applied. The cumulative average of ICP-MS linearity of developed electroanalytical sensor was 94.9%. The efficient recovery of copper from the concentrate flows with the sensor integrated-cementation process has a strong potential for "Industry 4.0" applications with enhanced automation levels.


Assuntos
Cimentação , Cobre , Metais , Rios
10.
Chemistry ; 27(68): 16947-16955, 2021 Dec 06.
Artigo em Inglês | MEDLINE | ID: mdl-33913575

RESUMO

In an effort to combine the favorable catalytic properties of Co3 O4 and CeO2 , nanocomposites with different phase distribution and Co3 O4 loading were prepared and employed for CO oxidation. Synthesizing Co3 O4 -modified CeO2 via three different sol-gel based routes, each with 10.4 wt % Co3 O4 loading, yielded three different nanocomposite morphologies: CeO2 -supported Co3 O4 layers, intermixed oxides, and homogeneously dispersed Co. The reactivity of the resulting surface oxygen species towards CO were examined by temperature programmed reduction (CO-TPR) and flow reactor kinetic tests. The first morphology exhibited the best performance due to its active Co3 O4 surface layer, reducing the light-off temperature of CeO2 by about 200 °C. In contrast, intermixed oxides and Co-doped CeO2 suffered from lower dispersion and organic residues, respectively. The performance of Co3 O4 -CeO2 nanocomposites was optimized by varying the Co3 O4 loading, characterized by X-ray diffraction (XRD) and N2 sorption (BET). The 16-65 wt % Co3 O4 -CeO2 catalysts approached the conversion of 1 wt % Pt/CeO2 , rendering them interesting candidates for low-temperature CO oxidation.

11.
Chem Sci ; 12(16): 5774-5786, 2021 Apr 28.
Artigo em Inglês | MEDLINE | ID: mdl-35342542

RESUMO

Converting CO2 directly from the air to fuel under ambient conditions is a huge challenge. Thus, there is an urgent need for CO2 conversion protocols working at room temperature and atmospheric pressure, preferentially without any external energy input. Herein, we employ magnesium (nanoparticles and bulk), an inexpensive and the eighth-most abundant element, to convert CO2 to methane, methanol and formic acid, using water as the sole hydrogen source. The conversion of CO2 (pure, as well as directly from the air) took place within a few minutes at 300 K and 1 bar, and no external (thermal, photo, or electric) energy was required. Hydrogen was, however, the predominant product as the reaction of water with magnesium was favored over the reaction of CO2 and water with magnesium. A unique cooperative action of Mg, basic magnesium carbonate, CO2, and water enabled this CO2 transformation. If any of the four components was missing, no CO2 conversion took place. The reaction intermediates and the reaction pathway were identified by 13CO2 isotopic labeling, powder X-ray diffraction (PXRD), nuclear magnetic resonance (NMR) and in situ attenuated total reflectance-Fourier transform infrared spectroscopy (ATR-FTIR), and rationalized by density-functional theory (DFT) calculations. During CO2 conversion, Mg was converted to magnesium hydroxide and carbonate, which may be regenerated. Our low-temperature experiments also indicate the future prospect of using this CO2-to-fuel conversion process on the surface of Mars, where CO2, water (ice), and magnesium are abundant. Thus, even though the overall process is non-catalytic, it could serve as a step towards a sustainable CO2 utilization strategy as well as potentially being a first step towards a magnesium-driven civilization on Mars.

12.
J Phys Chem C Nanomater Interfaces ; 124(43): 23674-23682, 2020 Oct 29.
Artigo em Inglês | MEDLINE | ID: mdl-33154784

RESUMO

Pd nanoparticles (1 wt %; mean size ∼4 nm) were supported on ∼2 µm sized, but few nanometers thick, graphene nanoplatelets (GNPs) and compared to 1 wt % Pd on activated carbon or γ-alumina. Catalyst morphology, specific surface area, and Pd particle size were characterized by SEM, BET, and TEM, respectively. H2-TPD indicated that GNPs intercalated hydrogen, which may provide additional H2 supply to the Pd nanoparticles during C2H4 hydrogenation. Whereas the two types of Pd/GNPs (NaOH vs calcinated) catalysts were less active than Pd/C and Pd/Al2O3 below 40 °C, at 55 °C they were about 3-4 times more active. As for example Pd/GNPs (NaOH) and Pd/Al2O3 exhibited not too different mean Pd particle size (3.7 vs 2.5 nm, respectively), the higher activity is attributed to the additional hydrogen supply likely by the metal/support interface, as suggested by the varying C2H4 and H2 orders on the different supports. Operando XANES measurements during C2H4 hydrogenation revealed the presence of Pd hydride. The Pd hydride was more stable for Pd/GNPs (NaOH) than for Pd/C, once more pointing to a better hydrogen supply by graphene nanoplatelets.

13.
Eur J Inorg Chem ; 2019(30): 3503-3510, 2019 Aug 15.
Artigo em Inglês | MEDLINE | ID: mdl-31588182

RESUMO

The catalytic hydrogenation of different aldehydes to the corresponding alcohols was investigated using an FeII hydride pincer complex as catalyst in the supported ionic liquid phase (SILP) reaction mode. Two different ionic liquids of the type [X4441][NTf2] with X=N or P were applied with mesoporous silica gel as support, which was coated first with a chemisorbed monolayer of the corresponding modified IL to remove acidic surface OH-groups and to prevent IL leaching. Quantitative conversion with turn-over frequencies in the order of 1000 h- 1 were obtained for various aromatic and heteroaromatic aldehydes and highly selective aldehyde reduction was observed also for substrates containing reducible C=C bonds. Aldehydes with longer aliphatic chains or cycloalkyl substituents, however, showed no conversion here, in contrast to a previous study with an imidazolium-based ionic liquid. These differences were ascribed primarily to differences in substrate/ionic liquid interactions. Whereas [N4441][NTf2] and [P4441][NTf2] gave essentially identical results for different substrates in single-batch reactions, prolonged use of the catalyst in repeated reaction cycles lead to a quick drop-off in catalyst activity in [P4441][NTf2], but a continuous, quantitative conversion in [N4441][NTf2].

14.
J Nanosci Nanotechnol ; 19(2): 743-757, 2019 02 01.
Artigo em Inglês | MEDLINE | ID: mdl-30360150

RESUMO

A Cu-Zn/core-shell Al-MCM-41 catalyst with various Cu and Zn species was investigated for selective catalytic reduction of NO with NH3. The roles of Zn in the NOx adsorption properties and the acidity of the catalysts were studied by temperature-programmed desorption of NOx and in situ Fourier transform infrared spectroscopy of NO+O2 adsorption and NH3 adsorption. The presence of Zn can promote the number of acid sites and improve the NOx adsorption capacity by providing the additional sites for NOx adsorption and subsequent nitrite and nitrate formation. Based on the experimental results, a possible reaction pathway was suggested. Cu-Zn/Al-MCM-41 exhibited higher activity compared with that of Cu/Al-MCM-41, having an average NO conversion of 73%. However, the average NO conversion was increased to 77% when Zn was loaded as ZnO form instead of various Zn species. in situ X-ray adsorption near edge structure during reduction by H2 revealed that there is a higher number of Cu+ in Cu-ZnO/Al-MCM-41 than that in Cu-Zn/Al-MCM-41. Under wet condition, the average NO conversion of Cu-ZnO/core-shell Al-MCM-41 was dropped to 68%. However, activity of Cu-ZnO/core-shell Al-MCM-41 was more stable than that of Cu-Zn/core-shell Al-MCM-41.

15.
ACS Catal ; 8(9): 8630-8641, 2018 Sep 07.
Artigo em Inglês | MEDLINE | ID: mdl-30221030

RESUMO

Cobalt oxide Co3O4 has recently emerged as promising, noble metal-free catalyst for oxidation reactions but a better understanding of the active catalyst under working conditions is required for further development and potential commercialization. An operando approach has been applied, combining near ambient (atmospheric) pressure X-ray photoelectron spectroscopy (NAP-XPS), Fourier transform infrared spectroscopy (FTIR), or X-ray diffraction (XRD) with simultaneous catalytic tests of CO oxidation on Co3O4, enabling one to monitor surface and bulk states under various reaction conditions (steady-state and dynamic conditions switching between CO and O2). On the basis of the surface-specific chemical information a complex network of different reaction pathways unfolded: Mars-van-Krevelen (MvK), CO dissociation followed by carbon oxidation, and formation of carbonates. A possible Langmuir-Hinshelwood (LH) pathway cannot be excluded because of the good activity when no oxygen vacancies were detected. The combined NAP-XPS/FTIR results are in line with a MvK mechanism above 100 °C, involving the Co3+/Co2+ redox couple and oxygen vacancy formation. Under steady state, the Co3O4 surface appeared oxidized and the amount of reduced Co2+ species at/near the surface remained low up to 200 °C. Only in pure CO, about 15% of surface reduction were detected, suggesting that the active sites are a minority species. The operando spectroscopic studies also revealed additional reaction pathways: CO dissociation followed by carbon reoxidation and carbonate formation and its decomposition. However, due to their thermal stability in various atmospheres, the carbonates are rather spectators and also CO dissociation seems a minor route. This study thus highlights the benefits of combining operando surface sensitive techniques to gain insight into catalytically active surfaces.

16.
Dalton Trans ; 46(14): 4554-4570, 2017 Apr 05.
Artigo em Inglês | MEDLINE | ID: mdl-28317954

RESUMO

The surface chemical properties of undoped tetragonal ZrO2 and the gas-phase dependence of the tetragonal-to-monoclinic transformation are studied using a tetragonal ZrO2 polymorph synthesized via a sol-gel method from an alkoxide precursor. The obtained phase-pure tetragonal ZrO2 is defective and strongly hydroxylated with pronounced Lewis acidic and Brønsted basic surface sites. Combined in situ FT-infrared and electrochemical impedance measurements reveal effective blocking of coordinatively unsaturated sites by both CO and CO2, as well as low conductivity. The transformation into monoclinic ZrO2 is suppressed up to temperatures of ∼723 K independent of the gas phase composition, in contrast to at higher temperatures. In inert atmospheres, the persisting structural defectivity leads to a high stability of tetragonal ZrO2, even after a heating-cooling cycle up to 1273 K. Treatments in CO2 and H2 increase the amount of monoclinic ZrO2 upon cooling (>85 wt%) and the associated formation of either Zr-surface-(oxy-)carbide or dissolved hydrogen. The transformation is strongly affected by the sintering/pressing history of the sample, due to significant agglomeration of small crystals on the surface of sintered pellets. Two factors dominate the properties of tetragonal ZrO2: defect chemistry and hydroxylation degree. In particular, moist conditions promote the phase transformation, although at significantly higher temperatures as previously reported for doped tetragonal ZrO2.

17.
Water Sci Technol ; 61(3): 659-69, 2010.
Artigo em Inglês | MEDLINE | ID: mdl-20150702

RESUMO

The main objective of this work was to investigate the filterability of MBR sludge and its mixture with conventional activated sludge (CAS). In addition, the impacts of type and dose of various polyelectrolytes, filter type and sludge properties on the filterability of both MBR and Mixed sludges were determined. Specific cake resistance (SCR) measured by the Buchner funnel filtration test apparatus and the solids content of the resulting sludge cake were used to assess the dewaterability of tested sludges. The type of filter paper used in Buchner tests affected the results of filterability for MBR, CAS and Mixed sludges. SCR values and optimum polyelectrolyte doses increased with increasing MLSS concentrations in the MBR, which suggested that increase in MLSS concentrations accompanied by increases in EPS and SMP concentrations and a shift toward smaller particles caused poorer dewaterability of the MBR sludge. The significant differences observed among the filterability of CAS and MBR sludges suggested that MLSS alone is not a good predictor of sludge dewaterability. Combining CAS and MBR sludges at different proportions generally improved their dewaterability. Combining MBR sludges having typically high MLSS and EPS concentrations with CAS having much lower MLSS concentrations may be an option for full-scale treatment plants experiencing sludge dewaterability problems. Better filterability and higher cake dry solids were achieved with cationic polyelectrolytes compared to anionic and non-ionic ones for all sludge types tested.


Assuntos
Reatores Biológicos , Membranas Artificiais , Esgotos/análise , Ação Capilar , Eletrólitos/isolamento & purificação , Filtração/instrumentação , Filtração/métodos , Análise de Alimentos , Cinética , Eliminação de Resíduos Líquidos/instrumentação , Eliminação de Resíduos Líquidos/métodos , Água/análise , Purificação da Água/instrumentação , Purificação da Água/métodos
18.
Water Res ; 43(3): 822-30, 2009 Feb.
Artigo em Inglês | MEDLINE | ID: mdl-19100595

RESUMO

This paper presents the findings of experimental investigations regarding the influence of 13 different flux enhancing chemicals (FeCl3, polyaluminium chloride, 2 chitosans, 5 synthetic polymers, 2 starches and 2 activated carbons) on respirometric characteristics and nitrification/denitrification performance of membrane bioreactor (MBR) mixed liquor. Flux enhancing chemicals are a promising method to reduce the detrimental effects of fouling phenomena via the modification of mixed liquor characteristics. However, potentially inhibiting effects of these chemicals on mixed liquor biological activity triggered the biokinetic studies (in jar tests) conducted in this work. The tested polyaluminium chloride (PACl) strongly impacted on nitrification (-16%) and denitrification rate (-43%). The biodegradable nature of chitosan was striking in endogenous and exogenous tests. Considering the relatively high costs of this chemical, an application for wastewater treatment does thus not seem to be advisable. Also, addition of one of the tested activated carbons strongly impacted on the oxygen uptake rate (-28%), nitrification (-90%) and denitrification rate (-43%), due to a decrease of pH. Results show that the changes in kLa values were mostly not significant, however, a decrease of 13% in oxygen transfer was found for sludge treated with PACl.


Assuntos
Reatores Biológicos , Respiração Celular , Membranas Artificiais , Compostos Orgânicos/isolamento & purificação , Esgotos , Aerobiose , Biomassa , Concentração de Íons de Hidrogênio , Nitrogênio/metabolismo , Oxigênio/metabolismo , Projetos Piloto , Viscosidade
19.
Water Res ; 39(8): 1652-62, 2005 Apr.
Artigo em Inglês | MEDLINE | ID: mdl-15878038

RESUMO

The main objective of this research was to investigate the oxidative destruction of free cyanide with hydrogen peroxide and copper-impregnated pumice as a heterogeneous catalyst. Original or copper-impregnated pumices added alone were not effective adsorbents of negatively charged cyanide ions due to incompatible surface interactions. Peroxide and original pumices added together were also ineffective in removing cyanide. However, for all of the three natural pumices tested with various particle size fractions, the use of copper-impregnated pumices and peroxide together significantly enhanced both the initial rate and extent of cyanide removal. Although copper-impregnated specific surface area was the major factor affecting the rate and extent of cyanide destruction for a particular pumice source with similar surface chemistries, the type of surface chemistry (i.e., specific functional groups) within different pumice sources also appears to be a very important factor. Lower rates and extents of cyanide removals were observed at pH 11 compared to pH 8 probably because of the negative impacts of alkaline conditions in terms of scavenging peroxide and forming more negatively charged pumice surfaces. Both the initial rate and ultimate extent of cyanide removals were generally higher at a temperature of 20 degrees C compared with those found at 10 degrees C. The use of copper-impregnated pumice as a light, cheap, readily available, natural, and porous heterogeneous catalyst either in completely mixed/suspended or fixed-bed reactor configurations may be an effective treatment technology for cyanide removal from solution. This new approach may minimize downstream metal removal problems experienced in conventional cyanide oxidation technologies.


Assuntos
Cobre/química , Cianetos/química , Peróxido de Hidrogênio/química , Eliminação de Resíduos Líquidos/métodos , Catálise , Concentração de Íons de Hidrogênio , Resíduos Industriais , Oxirredução , Tamanho da Partícula
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