Hydrogen sulfide gas treatment by a chemical-biological process: chemical absorption and biological oxidation steps

In order to remove high concentrations of hydrogen sulfide (H2S) gas from anaerobic wastewater treatments in livestock farming, a novel process was evaluated for H2S gas abatement involving the combination of chemical absorption and biological oxidation processes. In this study, the extensive experiments evaluating the removal efficiency, capacity, and removal characteristics of H2S gas by the chemical absorption reactor were conducted in a continuous operation. In addition, the effects of initial Fe2+ concentrations, pH, and glucose concentrations on Fe2+ oxidation by Thiobacillus ferrooxidans CP9 were also examined. The results showed that the chemical process exhibited high removal efficiencies with H2S concentrations up to 300 ppm, and nearly no acclimation time was required. The limitation of mass-transfer was verified as the rate-determining step in the chemical reaction through model validation. The Fe2+ production rate was clearly affected by the inlet gas concentration as well as flow rate and a prediction equation of ferrous production was established. The optimal operating conditions for the biological oxidation process were below pH 2.3 and 35 degrees C in which more than 90% Fe3+ formation ratio was achieved. Interestingly, the optimal glucose concentration in the medium was 0.1%, which favored Fe2+ oxidation and the growth of T. ferrooxidans CP9.     

Removal of nitric oxide in a biotrickling filter under thermophilic condition using Chelatococcus daeguensis

The development of a thermophilic biotrickling ?lter (BTF) system to inoculate a newly isolated strain of Chelatococcus daeguensis TAD1 for the effective treatment of nitric oxide (NO) is described. A bench-scale BTF was run under high concentrations of NO and 8% O₂ in thermophilic aerobic environment. A novel aerobic denitrifier Chelatococcus daeguensis TAD1 was isolated from the biofilm of an on-site biotrickling filter and it showed a denitrifying capability of 96.1% nitrate removal rate in a 24 h period in aerobic environment at 50 °C, with no nitrite accumulation. The inlet NO concentration fluctuated between approximately 133.9 and 669.6 mg m-3 and kept on a steady NOx removal rate above 80% in an oxygen stream of 8%. The BTF system was able to consistently remove 80–93.7% NO when the inlet NO was 535.7 mg m-3 in an oxygen stream of 2–20%. The biological removal efficiency of NO at 50 °C is higher than that at 25 °C, suggesting that the aerobic denitri?er TAD1 display well denitrification performance under thermophilic condition. Starvation for 2, 4 and 8 days resulted in the re-acclimation times of Chelatococcus daeguensis TAD1 ranging between 4 and 16 hours. A longer recovery time than that for weekend shutdown will be required when a longer starvation occurs. The results presented here demonstrate the feasibility of biotrickling ?lter for the thermophilic removal of NOx from gas streams.

Implications A novel denitrifier Chelatococcus daeguensis TAD1 was isolated from an on-site biotrickling filter in aerobic environment at 50 °C. To date, C. daeguensis has not been previously reported to be an aerobic denitrifier. In this study, a thermophilic biotrickling ?lter system inoculated with Chelatococcus daeguensis TAD1 for treatment of nitric oxide is developed. In coal-fired power plants, influent flue gas stream for nitrogen oxides (NO_x) removal typically exhibit temperatures between 50 and 60 °C. Traditionally, cooling gases to below 40 °C prior to biological treatment is inevitable, which is costly. Therefore, the application of thermophilic microorganisms for the removal of nitric oxide (NO) at this temperature range would offer great savings and would greatly extend the applicability of biofilters and biotrickling filters. Until now there has not been any study published about thermophilic biological treatment of NO under aerobic condition.     

Removal of ammonia solutions used in catalytic wet oxidation processes

Ammonia (NH(3)) is an important product used in the chemical industry, and is common place in industrial wastewater. Industrial wastewater containing ammonia is generally either toxic or has concentrations or temperatures such that direct biological treatment is unfeasible. This investigation used aqueous solutions containing more of ammonia for catalytic liquid-phase oxidation in a trickle-bed reactor (TBR) based on Cu/La/Ce composite catalysts, prepared by co-precipitation of Cu(NO(3))(2), La(NO(3))(2), and Ce(NO(3))(3) at 7:2:1 molar concentrations. The experimental results indicated that the ammonia conversion of the wet oxidation in the presence of the Cu/La/Ce composite catalysts was determined by the Cu/La/Ce catalyst. Minimal ammonia was removed from the solution by the wet oxidation in the absence of any catalyst, while approximately 91% ammonia removal was achieved by wet oxidation over the Cu/La/Ce catalyst at 230 degrees C with oxygen partial pressure of 2.0 MPa. Furthermore, the effluent streams were conducted at a liquid hourly space velocity of under 9 h(-1) in the wet catalytic processes, and a reaction pathway was found linking the oxidizing ammonia to nitric oxide, nitrogen and water. The solution contained by-products, including nitrates and nitrites. Nitrite selectivity was minimized and ammonia removal maximized when the feed ammonia solution had a pH of around 12.0.     

Removal of nitric oxide in a biotrickling filter under thermophilic condition using Chelatococcus daeguensis

The development of a thermophilic biotrickling filter (BTF) system to inoculate a newly isolated strain of Chelatococcus daeguensis TAD1 for the effective treatment of nitric oxide (NO) is described. A bench-scale BTF was run under high concentrations of NO and 8% O2 in thermophilic aerobic environment. A novel aerobic denitrifier Chelatococcus daeguensis TAD1 was isolated from the biofilm of an on-site biotrickling filter and it showed a denitrifying capability of 96.1% nitrate removal rate in a 24 h period in aerobic environment at 50 degrees C, with no nitrite accumulation. The inlet NO concentration fluctuated between approximately 133.9 and 669.6 mg m-3 and kept on a steady NOx removal rate above 80% in an oxygen stream of 8%. The BTF system was able to consistently remove 80-93.7% NO when the inlet NO was 535.7 mg m-3 in an oxygen stream of 2-20%. The biological removal efficiency of NO at 50 degrees C is higher than that at 25 degrees C, suggesting that the aerobic denitrifier TAD1 display well denitrification performance under thermophilic condition. Starvation for 2, 4 and 8 days resulted in the re-acclimation times of Chelatococcus daeguensis TAD1 ranging between 4 and 16 hours. A longer recovery time than that for weekend shutdown will be required when a longer starvation occurs. The results presented here demonstrate the feasibility of biotrickling filter for the thermophilic removal of NOx from gas streams. Implications: A novel denitrifier Chelatococcus daeguensis TAD1 was isolated from an on-site biotrickling filter in aerobic environment at 50 degrees C. To date, C. daeguensis has not been previously reported to be an aerobic denitrifier. In this study, a thermophilic biotrickling filter system inoculated with Chelatococcus daeguensis TADI for treatment of nitric oxide is developed. In coal-fired power plants, influent flue gas stream for nitrogen oxides (NOx) removal typically exhibit temperatures between 50 and 60 degrees C. Traditionally, cooling gases to below 40 degrees C prior to biological treatment is inevitable, which is costly. Therefore, the application ofthermophilic microorganisms for the removal of nitric oxide (NO) at this temperature range would offer great savings and would greatly extend the applicability ofbiofilters and biotrickling filters. Until now there has not been any study published about thermophilic biological treatment of NO under aerobic condition.     

Hydrogen Sulfide Gas Treatment by a Chemical‐Biological Process: Chemical Absorption and Biological Oxidation Steps

In order to remove high concentrations of hydrogen sulfide (H₂S) gas from anaerobic wastewater treatments in livestock farming, a novel process was evaluated for H₂S gas abatement involving the combination of chemical absorption and biological oxidation processes. In this study, the extensive experiments evaluating the removal efficiency, capacity, and removal characteristics of H₂S gas by the chemical absorption reactor were conducted in a continuous operation. In addition, the effects of initial Fe^2 + concentrations, pH, and glucose concentrations on Fe^2 + oxidation by Thiobacillus ferrooxidans CP9 were also examined. The results showed that the chemical process exhibited high removal efficiencies with H₂S concentrations up to 300 ppm, and nearly no acclimation time was required. The limitation of mass‐transfer was verified as the rate‐determining step in the chemical reaction through model validation. The Fe^2 + production rate was clearly affected by the inlet gas concentration as well as flow rate and a prediction equation of ferrous production was established. The optimal operating conditions for the biological oxidation process were below pH 2.3 and 35°C in which more than 90% Fe^3 + formation ratio was achieved. Interestingly, the optimal glucose concentration in the medium was 0.1%, which favored Fe^2 + oxidation and the growth of T. ferrooxidans CP9.     

Ultrafine particle emission from incinerators: the role of the fabric filter

Incinerators are claimed to be responsible of particle and gaseous emissions: to this purpose Best Available Techniques (BAT) are used in the flue-gas treatment sections leading to pollutant emission lower than established threshold limit values. As regard particle emission, only a mass-based threshold limit is required by the regulatory authorities. However; in the last years the attention of medical experts moved from coarse and fine particles towards ultrafine particles (UFPs; diameter less than 0.1 microm), mainly emitted by combustion processes. According to toxicological and epidemiological studies, ultrafine particles could represent a risk for health and environment. Therefore, it is necessary to quantify particle emissions from incinerators also to perform an exposure assessment for the human populations living in their surrounding areas. A further topic to be stressed in the UFP emission from incinerators is the particle filtration efficiency as function of different flue-gas treatment sections. In fact, it could be somehow important to know which particle filtration method is able to assure high abatement efficiency also in terms of UFPs. To this purpose, in the present work experimental results in terms of ultrafine particle emissions from several incineration plants are reported. Experimental campaigns were carried out in the period 2007-2010 by measuring UFP number distributions and total concentrations at the stack of five plants through condensation particle counters and mobility particle sizer spectrometers. Average total particle number concentrations ranging from 0.4 x 10(3) to 6.0 x 10(3) particles cm(-3) were measured at the stack of the analyzed plants. Further experimental campaigns were performed to characterize particle levels before the fabric filters in two of the analyzed plants in order to deepen their particle reduction effect; particle concentrations higher than 1 x 10(7) particles cm(-3) were measured, leading to filtration efficiency greater than 99.99%.     

非平衡等离子体技术对有害气体污染物的降解研究进展

由于非平衡等离子体化学过程在增强氧化能力、促进分子离解以及加速化学反应等方面具有很高的效率 ,因此 ,近年来利用非平衡等离子技术对气体污染物的破坏分解研究受到了广泛的关注。本文简述了非平衡等离子体技术对气体污染物的降解原理 ,综述了国内外利用这一技术破坏各种气体污染物的最新进展 ,讨论了放电功率、停留时间、催化剂、化合物结构等因素对放电反应效率的影响 ,并展望了其应用前景     

Optimization of the coating layer for the measurement of ammonia by diffusion denuders

The performance of citric acid, oxalic acid and phosphorous acid as denuder coating layers for the determination of atmospheric ammonia have been studied by means of laboratory and field tests. The parameters evaluated during the study include: collection efficiency, selectivity of the coating layer, stability of the reaction product, operative capacity and stability of the coating layer. The results of this study show that phosphorous acid is a suitable coating layer for a denuder line intended to determine both gaseous ammonia and particulate ammonium in the atmosphere. It has been found that the citric acid coating suffers from an insufficient strength of the bond between collected ammonia and the coating layer, which causes a release of the collected ammonia both towards the air flow and towards the active sites of the denuder glass. The performance of oxalic acid was very good in the determination of gaseous ammonia, but this coating showed to be unsuitable for denuder sampling lines which are intended also for the determination of atmospheric ammonium. The volatilisation of oxalic from the denuder surface, in fact, causes a displacement of nitrate from the Teflon filter and an excess of nitrate ion on the back-up filter.Phosphorous acid-coated denuders were added to the sampling line employed in the EMEP station of Montelibretti. Reliable and interesting results were obtained, which allowed us to detect the presence of gaseous ammonia adsorbed on atmospheric particles.     

Combined effect of adsorption and biodegradation of biological activated carbon on H2S biotrickling filtration

In order to evaluate the combined effect of adsorption and biodegradation of H(2)S on activated carbon surface in biotrickling filtration, four laboratory-scale biofiltration columns were operated simultaneously for 120h to investigate the mechanisms involved in treating synthetic H(2)S streams using biological activated carbon (BAC). The first three columns (A, B, C) contained a mixture of activated carbon and glass beads, with the carbons (BAC or virgin activated carbon (VAC)) and conditions (with or without liquid medium recirculation) differentiated. The last column (D) used 100% glass beads with liquid medium recirculation. Air streams containing 45ppmv H(2)S were passed through the columns at 4s of gas retention time (GRT) and liquid flow rate was set at 0.71mlmin(-1). Column D got its breakthrough in 3min of operation, indicating a negligible contribution of glass beads to the adsorption of H(2)S. The removal efficiency (RE) of Columns B and C using VAC dropped quickly to 30% within the first 8h, and afterwards continued to drop further but slowly. Column A using BAC stayed at 25% of RE throughout the operation time. A thorough investigation of the H(2)S oxidation products, i.e., various S species in both aqueous (recirculation media) and solid phases (BAC and VAC), was conducted using ICP-OES, IC, XRF, and CHNS elemental analyzer. BAC demonstrated a better performance than columns with adsorption only. Water film was found to enhance H(2)S removal. The percentage of sulphate in the total sulphur of the BAC system improved to twice of that of VAC system, indicating sulphate is the main product of H(2)S biofiltration. The observed pH drop in BAC system double confirmed that the presence of biodegradation in the biofilm over carbon surface did profound effect on the oxidation of H(2)S, compare to the systems with adsorption only.     

Abiotic and biological mechanisms of nitric oxide removal from waste air in biotrickling filters

Nitric oxide (NO) may participate in the ozone layer depletion and forming of nitric acid. Abiotic and biological mechanisms of NO removal from waste gases were studied in a biotrickling filter. The abiotic NO removal rate in the biotrickling filter was estimated by a review of the literature. The abiotic and biological removals were also verified in the biotrickling filter. The result has shown that chemical oxidation and bionitrification were both involved in the NO removal. It was found that the NO removal in high concentration (approximately 1000 ppm or higher) was in large measure the result of abiotic removal in both gas-phase and liquid-phase reactions. When NO concentration is low (less than approximately 100 ppm), bionitrification was the main process in the NO removal process in the biotrickling filter.     

The treatment of waste air containing phenol vapors in biotrickling filter

This research aimed at investigating the biodegradation of phenol contaminated-air streams in biotrickling filter. The effect of inlet concentration (200-1000 ppmv) and empty bed contact time (EBCT) (15-60 s) were investigated under steady state, transient and shock loading, and shutdown periods. Upon rapid start up operation, inlet phenol concentrations of up to 1000 ppmv did not significantly affect the performance of the biotrickling filter at EBCT of 60 s, so that removal efficiency was well greater than 99%. In addition, the EBCT as low as 30 s did not have detrimental effects on the efficiency of the bioreactor and phenol removal was greater than 99%. Decreasing the EBCT to 15s reduced the removal efficiency to around 92%. The maximum elimination capacity obtained in the biotrickling filter was 642 g(phenol) m(-3) h(-1), where the removal efficiency was only 57%. Results from the transient loading experiments revealed that the biotrickling filter could effectively handle the variations of the inlet loads without the phenol removal capacity being significantly affected.     

Urea removal coupled with enhanced electricity generation in single-chambered microbial fuel cells

High concentration of total ammonia nitrogen (TAN) in the form of urea is known to inhibit the performance of many biological wastewater treatment processes. Microbial fuel cells (MFCs) have great potential for TAN removal due to its unique oxic/anoxic environment. In this study, we demonstrated that increased urea (TAN) concentration up to 3940 mg/L did not inhibit power output of single-chambered MFCs, but enhanced power generation by 67% and improved coulombic efficiency by 78% compared to those obtained at 80 mg/L of TAN. Over 80% of nitrogen removal was achieved at TAN concentration of 2630 mg/L. The increased nitrogen removal coupled with significantly enhanced coulombic efficiency, which was observed for the first time, indicates the possibility of a new electricity generation mechanism in MFCs: direct oxidation of ammonia for power generation. This study also demonstrates the great potential of using one MFC reactor to achieve simultaneous electricity generation and urea removal from wastewater.

     

Treatment of 1,3-Butadiene in an Air Stream by a Biotrickling Filter and a Biofilter

ABSTRACT

This paper presents results obtained from a performance study on the biotreatment of 1,3-butadiene in an air stream using a reactor that consisted of a two-stage, in-series biotrickling filter connected with a three-stage, in-series biofilter. Slags and pig manure-based media were used as packing materials for the biotrickling filter and the biofilter, respectively. Experimental results indicated that, for the biotrickling filter portion, the butadiene elimination capacities were below 5 g/m³/hr for loadings of less than 25 g/m³/hr, and the butadiene removal efficiency was only around 17%. For the biofilter portion, the elimination capacities ranged from 10 to 107 g/m³/hr for loadings of less than 148 g/m³/hr. The average butadiene removal efficiency was 75–84% for superficial gas velocities of 53–142 m/hr and a loading range of 10–120 g/m³/hr. The elimination capacity approached a maximum of 108 g/m³/hr for a loading of 150 g/m³/hr. The elimination rates of butadiene in both the biotrickling filter and biofilter were mass-transfer controlled for influent butadiene concentrations below about 600 ppm for superficial gas velocities of 29–142 m/hr. The elimination capacity was significantly higher in the biofilter than in the biotrickling filter. This discrepancy may be attributed to the higher mass-transfer coefficient and gas-solid interfacial area offered for transferring the gaseous butadiene in the biofilter.     

Advanced oxidation processes for the treatment of olive-oil mills wastewater

In this work, the treatment of an actual industrial waste with three advanced oxidation processes (AOP) has been studied: conductive-diamond electrooxidation (CDEO), ozonation and Fenton oxidation. The wastewater comes from olive-oil mills (OMW) and contains a COD of nearly 3000 mg dm(-3). CDEO allowed achieving the complete mineralization of the waste with high current efficiencies. Likewise, both ozonation and Fenton oxidation were able to treat the wastes, but they obtained very different results in terms of efficiency and mineralization. The accumulation of oxidation-refractory compounds as final products excludes the use of ozonation and Fenton oxidation as a sole treatment technology. This confirms that besides the hydroxyl-radical mediated oxidation, CDEO combines other important oxidation processes such as the direct electro-oxidation on the diamond surface and the oxidation mediated by other electrochemically formed compounds generated on this electrode.     

Co-treatment of hydrogen sulfide and methanol in a single-stage biotrickling filter under acidic conditions

Biofiltration of waste gases is cost-effective and environment-friendly compared to the conventional techniques for treating large flow rates of gas streams with low concentrations of pollutants. Pulp and paper industry off-gases usually contain reduced sulfur compounds, such as hydrogen sulfide and a wide range of volatile organic compounds (VOCs), e.g., methanol. It is desirable to eliminate both of these groups of compounds. Since the co-treatment of inorganic sulfur compounds and VOCs in biotrickling filters is a relatively unexplored area, the simultaneous biotreatment of H2S and methanol as the model VOC was investigated. The results showed that, after adaptation, the elimination capacity of methanol could reach around 236 g m(-3) h(-1) with the simultaneous complete removal (100%) of 12 ppm H2S when the empty bed residence time is 24 s. The pH of the system was around 2. Methanol removal was hardly affected by the presence of hydrogen sulfide, despite the low pH. Conversely, the presence of the VOC in the waste gas reduced the efficiency of H2S biodegradation. The maximal methanol removal decreased somewhat when increasing the gas flow rate. This is the first report on the degradation of methanol at such low pH in a biotrickling filter and on the co-treatment of H2S and VOCs under such conditions.     

Construction and Economics of a Pilot/Full-Scale Biological Trickling Filter Reactor for the Removal of Volatile Organic Compounds from Polluted Air

ABSTRACT

The design and the construction of an actual 8.7-m³ pilot/ full-scale biotrickling filter for waste air treatment is described and compared with a previous conceptual scale-up of a laboratory reactor. The reactor construction costs are detailed and show that about one-half of the total reactor costs ($97,000 out of $178,000) was for personnel and engineering time, whereas ~20% was for monitoring and control equipment. A detailed treatment cost analysis demonstrated that, for an empty bed contact time of 90 sec, the overall treatment costs (including capital charges) were as low as $8.7/1000 m³ _air in the case where a nonchlorinated volatile organic compound (VOC) was treated, and $14/ 1000 m³ _air for chlorinated compounds such as CH₂Cl₂. Comparison of these costs with conventional air pollution control techniques demonstrates excellent perspectives for more field applications of biotrickling filters. As the specific costs of building and operating biotrickling filter reactors decrease with increasing size of the reactor, the cost benefit of biotrickling filtration is expected to increase for full technical-scale bioreactors.     

沿面放电氧化液相亚硫酸铵

为了解决湿式氨法烟气脱硫生成不稳定亚硫酸铵（（NH4）2SO3）副产物的问题,设计了以不锈钢弹簧和溶液分别作为高压和低压电极的沿面放电系统,对液相（NH4）2SO3的氧化进行了研究。空气从反应器上方进入后经放电区域形成活性物质,再由底部的曝气头鼓入溶液并与（NH4）2SO3发生反应。比较了沿面放电处理与传统曝气处理的氧化效率,考察了放电电压、载气气量和初始浓度等因素对（NH4）2SO3氧化的影响。结果表明,沿面放电对（NH4）2SO3有显著的氧化效果;优化条件下的（NH4）2SO3氧化率接近100%;溶液中（NH4）2SO4与（NH4）2SO3的浓度比小于1时有利于（NH4）2SO3的氧化。     

Combination of ozonation with conventional aerobic oxidation for distillery wastewater treatment

Laboratory-scale experiments were conducted in order to investigate the effect of ozone as pre-aerobic treatment and post-aerobic treatment for the treatment of the distillery wastewater. The degradation of the pollutants present in distillery spent wash was carried out by ozonation, aerobic biological degradation processes alone and by using the combinations of these two processes to investigate the synergism between the two modes of wastewater treatment and with the aim of reducing the overall treatment costs. Pollutant removal efficiency was followed by means of global parameters directly related to the concentration of organic compounds in those effluents: chemical oxygen demand (COD) and the color removal efficiency in terms of absorbance of the sample at 254 nm. Ozone was found to be effective in bringing down the COD (up to 27%) during the pretreatment step itself. In the combined process, pretreatment of the effluent led to enhanced rates of subsequent biological oxidation step, almost 2.5 times increase in the initial oxidation rate has been observed. Post-aerobic treatment with ozone led to further removal of COD along with the complete discoloration of the effluent. The integrated process (ozone-aerobic oxidation-ozone) achieved approximately 79% COD reduction along with discoloration of the effluent sample as compared to 34.9% COD reduction for non-ozonated sample, over a similar treatment period.     

Air Pollution Abatement in the Ceramic Industry

Air pollution abatement has been a constant concern for the ceramic indudry over the last four decades. The multiplicity of materials involved, numbering in the hundreds of fluxes and refractories for the manufacture of many different types of glasses, results in gaseous as well as particulate reaction products. Methods of abatement through various means have been developed and are in use in the United States and world-wide today.     

Scrubbing intensification for sulphur and ammonia compounds removal

Operating conditions were optimised in a new compact scrubber in order to remove odorous sulphur (H(2)S and CH(3)SH) and ammonia compounds. The influence of the superficial gas and liquid velocities, pH, contactor length, inlet concentrations (sulphur compounds, ammonia, chlorine), and the mixing effects was characterised. Whereas abatement increased with velocities, pH and the chlorine concentration, an increase of inlet CH(3)SH concentration drove to a worse efficiency of process. Moreover, the contactor length and the presence of another pollutant in the gas phase only played a role on the methylmercaptan removal. Finally, the reactive consumptions were estimated at the outlet of the reactor. The chlorination by-product quantification permitted to understand the under-stoichiometry.