Removal of Hg0 from flue gas using two homogeneous photo‐fenton‐like reactions

Removal of Hg⁰ using two homogeneous Photo‐Fenton‐Like reactions was first investigated in a photochemical reactor. Effects of process parameters on Hg⁰ removal were studied. Free radical and reaction products were analyzed. Removal pathways of Hg⁰ were discussed. Simultaneous removal of Hg⁰, NO, and SO₂ is also studied briefly. The results show that UV power, wavelength, H₂O₂ concentration, and solution pH have great effects on Hg⁰ removal. Hg⁰, and SO₂ concentrations, solution temperature, Fe³⁺, Cu²⁺, , and concentrations also have significant effects on Hg⁰ removal. However, concentrations of CO₂, NO, O₂, Cl^?, , , SiO₂, Al₂O₃, and Fe₂O₃ only have slight effects on Hg⁰ removal. Hg⁰/NO/SO₂ can be simultaneously removed by Photo‐Fenton‐Like reactions. ·OH was captured, and / /Hg²⁺ were also detected. Removals of Hg⁰ by photochemical oxidation and ·OH oxidation play a major role, and removal of Hg⁰ by H₂O₂ oxidation only plays a secondary role in removal of Hg⁰. © 2015 American Institute of Chemical Engineers AIChE J, 61: 1322–1333, 2015     

Effect of pre‐treatments based on UV photocatalysis and photo‐oxidation on toluene biofiltration performance

BACKGROUND: The integration of UV photocatalysis and biofiltration seems to be a promising combination of technologies for the removal of hydrophobic and poorly biodegradable air pollutants. The influence of pre‐treatments based on UV_{254 nm} photocatalysis and photo‐oxidation on the biofiltration of toluene as a target compound was evaluated in a controlled long‐term experimental study using different system configurations: a standalone biofilter, a combined UV photocatalytic reactor‐biofilter, and a combined UV photo‐oxidation reactor (without catalyst)‐biofilter. RESULTS: Under the operational conditions used (residence time of 2.7 s and toluene concentrations 600–1200 mg C m^?3), relatively low removal efficiencies (6–3%) were reached in the photocatalytic reactor and no degradation of toluene was found when the photo‐oxidation reactor was operated without catalyst. A noticeable improvement in the performance of the biofilter combined with a photocatalytic reactor was observed, and the elimination capacity of the biological process increased by more than 12 g C h^?1 m^?3 at the inlet loads studied of 50–100 g C h^?1 m^?3. No positive effect on toluene removal was observed for the combination of UV photoreactor and biofilter. CONCLUSIONS: Biofilter pre‐treatment based on UV_{254 nm} photocatalysis showed promising results for the removal of hydrophobic and recalcitrant air pollutants, providing synergistic improvement in the removal of toluene. Copyright © 2011 Society of Chemical Industry     

Prediction of dispersed phase holdup in a modified multi‐stage bubble column scrubber

This paper reports on the experimental investigation carried out to evaluate fractional dispersed phase holdup for a gas‐liquid mixture in a modified multi‐stage bubble column (with contraction and expansion disks), which has been conceived, designed and fabricated as a wet scrubber for control of air pollution; in addition it has versatile use as a gas‐liquid contactor in chemical process industries. A correlation developed for predicting fractional dispersed phase holdup has been found to be encouraging and highly significant from statistical analysis.     

Bubble size and radial gas hold‐up distributions in a slurry bubble column using ultrafast electron beam X‐ray tomography

Gas hold‐up and bubble size distribution in a slurry bubble column (SBC) were measured using the advanced noninvasive ultrafast electron beam X‐ray tomography technique. Experiments have been performed in a cylindrical column (D_T = 0.07 m) with air and water as the gas and liquid phase and spherical glass particles (d_P = 100 μm) as solids. The effects of solid concentration (0 ≤ C_s ≤ 0.36) and superficial gas velocity (0.02 ≤ U_G ≤ 0.05 m/s) on the flow structure, radial gas hold‐up profile and approximate bubble size distribution at different column heights in a SBC were studied. Bubble coalescence regime was observed with addition of solid particles; however, at higher solid concentrations, larger bubble slugs were found to break‐up. The approximate bubble size distribution and radial gas hold‐up was found to be dependent on U_G and C_s. The average bubble diameter calculated from the approximate bubble size distribution was increasing with increase of U_G. The average gas hold‐up was calculated as a function of U_G and agrees satisfactorily with previously published findings. The average gas hold‐up was also predicted as a function of C_s and agrees well for low C_s and disagrees for high C_s with findings of previous literature. © 2012 American Institute of Chemical Engineers AIChE J, 59: 1709–1722, 2013     

The effect of gas‐liquid counter‐current operation on gas hold‐up in bubble columns using electrical resistance tomography

BACKGROUND: In order to improve the performance of a counter‐current bubble column, radial variations of the gas hold‐ups and mean hold‐ups were investigated in a 0.160 m i.d. bubble column using electrical resistance tomography with two axial locations (Plane 1 and Plane 2). In all experiments the liquid phase was tap water and the gas phase air. The superficial gas velocity was varied from 0.02 to 0.25 m s^?1, and the liquid velocity varied from 0 to 0.01 m s^?1. The effect of liquid velocity on the distribution of mean hold‐ups and radial gas hold‐ups is discussed. RESULTS: The gas hold‐up profile in a gas–liquid counter‐current bubble column was determined by electrical resistance tomography. The liquid velocity slightly influences the mean hold‐up and radial hold‐up distribution under the selected operating conditions and the liquid flow improves the transition gas velocity from a homogeneous regime to a heterogeneous regime. Meanwhile, the radial gas hold‐up profiles are steeper at the central region of the column with increasing gas velocity. Moreover, the gas hold‐up in the centre of the column becomes steeper with increasing liquid velocity. CONCLUSIONS: The value of mean gas hold‐ups slightly increases with increasing downward liquid velocity, and more than mean gas hold‐ups in batch and co‐current operation. According to the experimental results, an empirical correlation for the centreline gas hold‐up is obtained based on the effects of gas velocity, liquid velocity, and ratio of axial height to column diameter. The values calculated in this way are in close agreement with experimental data, and compare with literature data on gas hold‐ups at the centre of the column. Copyright © 2010 Society of Chemical Industry     

Enhanced production of lovastatin in a bubble column by Aspergillus terreus using a two‐stage feeding strategy

A two‐stage feeding strategy is shown to improve the rate of production of lovastatin by Aspergillus terreus when compared with conventional batch fermentation. The feeding strategy consisted of an initial batch/fed‐batch phase and a semi‐continuous culture dilution phase with retention of pelleted biomass in a slurry bubble column reactor. The batch phase served only to build up the biomass for producing lovastatin, a secondary metabolite that inhibits its own synthesis in the producing microfungus. The semi‐continuous dilution phase provided nutrients to sustain the fungus, but prevented biomass growth by limiting the supply of essential nitrogen. (Synthesis of lovastatin does not require nitrogen.) The preferred pelleted growth morphology that favors lovastatin synthesis was readily obtained and maintained in the 20 L bubble column used. In contrast, a stirred tank fermentation had a substantially lower production of lovastatin because mechanical agitation damaged the fungal pellets. The two‐stage feeding method increased lovastatin production rate by more than 50% in comparison with the conventional batch operation. Rheological data for the fungal broth are presented. Copyright © 2007 Society of Chemical Industry     

Unified correlation for overall gas hold‐up in bubble column reactors for various gas–liquid systems using hybrid genetic algorithm‐support vector regression technique

The objective of this study is to collect the data on overall gas hold‐up (∈_G) for bubble column reactors handling various gas–liquid systems and further develop a unified data‐driven model for the estimation of the same. In this work, around 3300 experimental points for ∈_G have been collected from 85 open sources spanning the years 1963–2008. The data‐driven model for overall gas hold‐up has been established using hybrid Genetic Algorithm‐Support Vector Regression (GA‐SVR)‐based methodology. In the present study, GA has been used for nonlinear rescaling of the parameters. These exponentially scaled parameters are subsequently subjected for SVR training. The technique is an extension of conventional SVR technique, showing relatively enhanced results. The proposed hybrid model is based on various prominent design and operating parameters (15 in number) which includes superficial gas velocity, superficial liquid velocity, gas density, molecular weight of gas, sparger type, sparger hole diameter, number of sparger holes, liquid viscosity, liquid density, liquid surface tension, ionic strength of liquid, operating temperature, operating pressure, liquid height, and the column diameter. The estimations made by the SVR‐based unified model for ∈_G shows an excellent agreement with actual values with estimation accuracy of 98.5% and % AARE of 9.32%. For ease in applicability and ready reference of the practicing engineers, the hybrid GA‐SVR‐based model in the form of software and the entire database for ∈_G has been uploaded on the link http://www.esnips.com/web/UICT‐NCL .     

Prediction of gas hold‐up in a bubble column filled with pure and binary liquids

A dimensionless correlation for gas hold‐up in a bubble column filled with pure liquids and binary mixtures has been developed. The criteria of bubble coalescence in pure liquids and foamability of binary mixtures have been included successfully in the proposed correlation. For the first time, comprehensive data of gas hold‐up with respect to concentration in four binary systems are presented. The often‐reported enhancement of gas hold‐up in aqueous alcohol mixtures has been observed experimentally. The proposed correlation is able to predict successfully the trend of gas hold‐up enhancement with respect to concentration. The estimated values are found to be within 7% of the measured values.     

Advanced Oxidative Removal of Nitric Oxide from Flue Gas by Homogeneous Photo‐Fenton in a Photochemical Reactor

In this work, advanced oxidation removal of nitric oxide (NO) from flue gas by homogeneous Photo‐Fenton was investigated in a photochemical reactor and the effects of several influencing factors on NO removal were evaluated. The gas‐liquid reaction products were determined. The reaction pathways of NO removal are also preliminarily discussed. It was found that with the increase of Fe²⁺ concentration, NO removal efficiency first increased and then decreased. Increasing H₂O₂ concentration and UV radiation intensity greatly increased NO removal efficiency, but the growth rates gradually became smaller. NO removal efficiency greatly reduced with the increase of gas flow and NO concentration, and only slightly decreased with the increase of solution temperature, but significantly increased with the increase of initial solution pH value. The main anion product in the liquid phase was NO₃^–. With respect to removal of NO using homogeneous Photo‐Fenton, ·OH oxidation was the main reaction pathway, and H₂O₂ oxidation was the secondary reaction pathway.     

Advanced oxidation processes for the degradation of p‐hydroxybenzoic acid 2: Photo‐assisted Fenton oxidation

Oxidation of p‐hydroxybenzoic acid in aqueous solution by the photo‐assisted Fenton reaction (Fe²⁺ + H₂O₂ + UV) has been studied. The effects of ferrous ion concentration (0.05, 0.14 and 0.29 mmol dm^?3), temperature (10, 20, 30 and 40 °C), and initial hydrogen peroxide concentration (0.7, 1.4, 2.2 and 2.9 mmol dm^?3) on the p‐hydroxybenzoic acid conversion were established. Experimental results indicate that the kinetics of this oxidation process fits pseudo‐first‐order kinetics well. The overall kinetic rate constant was split into two components: direct oxidation by UV radiation (photolysis) and oxidation by free radicals (mainly OH·) generated in the system. The importance of these two reaction paths for each specific value of ferrous ion concentration, temperature and initial hydrogen peroxide concentration was evaluated. A semi‐empirical expression is proposed for the overall reaction rate which takes into account both oxidation pathways and is a function of operating variables. © 2001 Society of Chemical Industry     

Mineralisation of the antibiotic amoxicillin in pure and surface waters by artificial UVA‐ and sunlight‐induced Fenton oxidation

BACKGROUND: The degradation and mineralisation of the antibiotic amoxicillin by photo‐Fenton reactions, mediated by artificial UVA or solar irradiation, were investigated. Experiments were conducted with 30 mg L^?1 amoxicillin solutions prepared with deionised or surface water at Fe²⁺ and H₂O₂ concentrations in the range 0.0179–0.0895 and 1–10 mmol L^?1, respectively. Black‐light irradiation at 365 nm was provided by a 13 W m^?2 lamp, while samples were exposed to sunlight at 20 W m^?2 for solar experiments. RESULTS: In all cases, quantitative amoxicillin degradation occurred within 5 min and this was accompanied by lower mineralisation rates. Mineralisation followed first‐order kinetics with respect to organic carbon content and it was not affected by the water matrix with either type of illumination. Solar‐induced reactions were only marginally faster than artificial irradiation. Increasing the H₂O₂ to Fe²⁺ concentration ratio increases the extent of mineralisation up to a point beyond which degradation is impeded due to radical scavenging associated with the high concentrations of the Fenton reagents. CONCLUSION: Amoxicillin is readily degradable by homogeneous photocatalysis, being converted to more stable intermediates as indicated by lower mineralisation rates. The process can be driven by solar irradiation, thus providing a sustainable treatment technology. Copyright © 2009 Society of Chemical Industry     

Formation of needle‐like lepidocrocite fine particles by oxidation of an aqueous suspension of ferrous hydroxide in a bubble column

Fine particles of needle‐like lepidocrocite (γ‐FeOOH) were synthesized by the oxidation of aqueous suspensions of ferrous hydroxide using a bubble column with draft tube at a constant temperature ranging from 20°C to 30°C. The oxidation steps leading to green rust (an intermediate) and lepidocrocite (final product), termed Step I and II, respectively, could be described apparently as first order, with respect to oxygen, and zero order, with respect to total ferrous species. When the concentration of oxygen in the feed stream was varied under a constant gas velocity, the mean size based on the major axis of needle‐like particle decreased from 0.60 to 0.35 μm with increasing oxidation rate. When the gas velocity was varied under a constant oxygen concentration, the particle size was almost independent of the oxidation rate and was equal to ca. 0.6 μm. By the addition of a small amount of sodium dihydrogenphosphate (NaH₂PO₄), the major axis could be reduced to 0.2 μm with the minor axis and the oxidation rate almost unchanged.     

Modeling the ultrasonic cavitation‐enhanced removal of nitrogen oxide in a bubble column reactor

A model study of the sonochemical removal of nitric oxide (NO) in a bubble column reactor is presented. The detailed model is developed to investigate the actual cavitation phenomena taking place during the absorption of NO. The expansion and subsequent collapse of cavitation bubble according to the theory of cavity collapse—initially developed by Lord Rayleigh and then improved on by coupling the energy balance equation of the bubble and the chemical reactions taking place inside the cavity to calculate the composition of different species formed during the collapse—are modeled. The model takes into consideration (1) cavitation bubble dynamics, (2) generation and transfer of oxidizing species from bubble collapse through reaction kinetics, (3) transfer of NO from gas to liquid, and (4) chemical reactions of oxidizing species with dissolved NO. The results of the simulations surprisingly indicate that the chemistry induced by ultrasonic cavitation cannot explain the absorption of NO beyond about 30% of the inlet concentration if the mass transfer is assumed to be the same as that in the bubble column without ultrasound. When experimental values of mass‐transfer coefficients, calculated in the studies by other researchers (which are in the range of about five times the physical mass‐transfer coefficient in a bubble column), are used, absorption up to 80% are calculated in the simulations consistent with experimental results obtained from the sonochemical bubble column reactor. The present model provides a framework on which more robust and rigorous models can be developed for the complex gas‐liquid sonochemical systems and reactors. © 2011 American Institute of Chemical Engineers AIChE J, 58: 2397–2411, 2012     

Statistical analysis of effects of experimental variables on mass transfer coefficient in a novel hybrid bubble column using Box–Behnken design

Statistical analysis of effects of experimental variables on volumetric mass transfer coefficient in a novel hybrid rotating and reciprocating perforated plate bubble column is studied. The novel bubble column is designed indigenously using bevel gear arrangement. Agitation level, superficial gas velocity, superficial liquid velocity, perforation diameter and plate spacing are the experimental variables. Air–sodium sulphite solution system is used in this investigation. The Box–Behnken design in response surface methodology is employed for statistical analysis. The relationship between experimental variables and the desired response of volumetric mass transfer coefficient is established for this novel hybrid column. The linear, quadratic and interactive effects of experimental variables are found to be significant on the desired response of volumetric mass transfer coefficient. Results show that the data adequately fit into the second‐order polynomial model. An F‐test and P‐value show the significance of parameters on volumetric mass transfer coefficient. © 2012 Canadian Society for Chemical Engineering