Toward better understanding and feasibility of controlling greenhouse gas emissions from treatment of industrial wastewater with activated sludge

Wastewater treatment plants (WWTPs) have been recognized as important sources for anthropogenic greenhouse gas (GHG) emission. The objective of the study was to thoroughly investigate a typical industrial WWTP in southern Taiwan in winter and summer which possesses the emission factors close to those reported values, with the analyses of emission factors, mass fluxes, fugacity, lab-scale in situ experiments, and impact assessment. The activated sludge was the important source in winter and summer, and nitrous oxide (N₂O) was the main contributor (e.g., 57 to 91 % of total GHG emission in a unit of kg carbon dioxide-equivalent/kg chemical oxygen demand). Albeit important for the GHGs in the atmosphere, the fractional contribution of the GHG emission to the carbon or nitrogen removal in wastewater treatment was negligible (e.g., less than 1.5 %). In comparison with the sludge concentration or retention time, adjusting the aeration rate was more effective to diminish the GHG emission in the activated sludge without significantly affecting the treated water quality. When the aeration rate in the activated sludge simulation was reduced by 75 %, the mass flux of N₂O could be diminished by up to 53 % (from 9.6 to 4.5 mg/m²-day). The total emission in the WWTP (including carbon dioxide, methane, and N₂O) would decrease by 46 % (from 0.67 to 0.36 kg CO₂-equiv/kg COD). However, the more important benefit of changing the aeration rate was lowering the energy consumption in operation of the WWTP, as the fractional contribution of pumping to the total emission from the WWTP ranged from 46 to 93 % within the range of the aeration rate tested. Under the circumstance in which reducing the burden of climate change is a global campaign, the findings provide insight regarding the GHG emission from treatment of industrial wastewater and the associated impact on the treatment performance and possible mitigation strategies by operational modifications.

     

Seasonal variation and spatial distribution of atmospheric mercury and its gas-particulate partition in the vicinity of a semiconductor manufacturing complex

This study investigated the tempospatial variation of atmospheric mercury and its gas-particulate partition in the vicinity of a semiconductor manufacturing complex, where a plenty of flat-monitor manufacturing plants using elemental mercury as a light-initiating medium to produce backlight fluorescence tubes and may fugitively emit mercury-containing air pollutants to the atmosphere. Atmospheric mercury speciation, concentration, and the partition of total gaseous mercury (TGM) and particulate mercury (Hg_p) were measured at four sites surrounding the semiconductor manufacturing intensive district/complex. One-year field measurement showed that the seasonal averaged concentrations of TGM and Hg_p were in the range of 3.30–6.89 and 0.06–0.14 ng/m³, respectively, whereas the highest 24-h TGM and Hg_p concentrations were 10.33 and 0.26 ng/m³, respectively. Atmospheric mercury apportioned as 92.59–99.01 % TGM and 0.99–7.41 % Hg_p. As a whole, the highest and lowest concentrations of TGM were observed in the winter and summer sampling periods, respectively, whereas the concentration of Hg_p did not vary much seasonally. The highest TGM concentrations were always observed at the downwind sites, indicating that the semiconductor manufacturing complex was a hot spot of mercury emission source, which caused severe atmospheric mercury contamination over the investigation region.     

Enhanced mercuric chloride adsorption onto sulfur-modified activated carbons derived from waste tires

A number of activated carbons derived from waste tires were further impregnated by gaseous elemental sulfur at temperatures of 400 and 650 degrees C, with a carbon and sulfur mass ratio of 1:3. The capabilities of sulfur diffusing into the micropores of the activated carbons were significantly different between 400 and 650 degrees C, resulting in obvious dissimilarities in the sulfur content of the activated carbons. The sulfur-impregnated activated carbons were examined for the adsorptive capacity of gas-phase mercuric chloride (HgC1) by thermogravimetric analysis (TGA). The analytical precision of TGA was up to 10(-6) g at the inlet HgCl2 concentrations of 100, 300, and 500 microg/m3, for an adsorption time of 3 hr and an adsorption temperature of 150 degrees C, simulating the flue gas emitted from municipal solid waste (MSW) incinerators. Experimental results showed that sulfur modification can slightly reduce the specific surface area of activated carbons. High-surface-area activated carbons after sulfur modification had abundant mesopores and micropores, whereas low-surface-area activated carbons had abundant macropores and mesopores. Sulfur molecules were evenly distributed on the surface of the inner pores after sulfur modification, and the sulfur content of the activated carbons increased from 2-2.5% to 5-11%. After sulfur modification, the adsorptive capacity of HgCl2 for high-surface-area sulfurized activated carbons reached 1.557 mg/g (22 times higher than the virgin activated carbons). The injection of activated carbons was followed by fabric filtration, which is commonly used to remove HgCl2 from MSW incinerators. The residence time of activated carbons collected in the fabric filter is commonly about 1 hr, but the time required to achieve equilibrium is less than 10 min. Consequently, it is worthwhile to compare the adsorption rates of HgCl2 in the time intervals of < 10 and 10-60 min.     

Comparative assessments of VOC emission rates and associated health risks from wastewater treatment processes

With the growing concern regarding emission of volatile organic compounds (VOCs) from wastewater treatment plants (WWTPs), the relationship between the VOC emission rates and the associated public health risks has been rarely discussed. The objective of this study was to examine and compare the VOC emission rates and cancer and non-cancer risks by inhalation intake, using a municipal WWTP in China as an example, with respect to the effects of treatment technologies, VOC species, and seasonal variation. Given the treatment technology considered, the emission rates of VOCs in this study were estimated by means of mass balance or calculated on the molecular level. From the viewpoints of both emission rates and cancer and non-cancer risks, sedimentation was the treatment technology with the highest health risks to the workers. Slightly lower VOC emission rates and health risks than those for sedimentation were observed in anaerobic treatment. Although the aeration significantly enhanced the VOC emission rates in the aerobic treatment process, the associated health risks were limited due to the low VOC concentrations in the gas phase, which were likely attributed to the strong mixing and dilution with fresh air by aeration. Amongst the VOCs investigated, benzene was the VOC with both a relatively high emission rate and health risk, while trichloroethylene possessed a high emission rate but the lowest health risk. Without strong interfacial aeration and turbulence between the water and atmosphere, the effects of treatment technology and seasonal variation on the health risks might be connected to the VOC emission rates, while the effect of VOC species depended considerably on the respective cancer slope factors and reference concentrations; the employment of aeration provided a different conclusion in which the emission rates were enhanced without a significant increase in the related cancer risks. These findings can provide insight into future health risk management and reduction strategies for workers in WWTPs.     

Surface functional characteristics (C, O, S) of waste tire-derived carbon black before and after steam activation

The effects of steam activation on the surface functional characteristics of waste tire-derived carbon black were investigated. Two carbon-based materials, powdered carbon black (PCB) and PCB-derived powdered activated carbon (PCB-PAC), were selected for this study. A stainless steel tubular oven was used to activate the PCB at an activation temperature of 900 degrees C and 1 atm using steam as an activating reagent. X-ray photoelectron spectroscopy (XPS) was adopted to measure the surface composition and chemical structure of carbon surface. Various elemental spectra (C, O, and S) of each carbon sample were further deconvoluted by peak synthesis. Results showed that the surfaces of PCB and PCB-PAC consisted mainly of C-C and C-O. The PCB-PAC surface had a higher percentage of oxygenated functional groups (C=O and O-C=O) than PCB. The O1s spectra show that the oxygen detected on the PCB surface was mainly bonded to carbon (C-O), whereas the oxygen on the PCB-PAC surface could be bonded to hydrogen (O-H) and carbon (C-O). Sulfur on the surface of PCB consisted of 58.9 wt% zinc sulfide (ZnS) and 41.1 wt% S=C=S, whereas that on the surfaces of PCB-PAC consisted mainly of S=C=S. Furthermore, the increase of oxygen content from 9.6% (PCB) to 11.9% (PCB-PAC) resulted in the increase of the pH values of PCB-PAC after steam activation.     

Preparation of sulfurized powdered activated carbon from waste tires using an innovative compositive impregnation process

The objective of this study is to develop an innovative compositive impregnation process for preparing sulfurized powdered activated carbon (PAC) from waste tires. An experimental apparatus, including a pyrolysis and activation system and a sulfur (S) impregnation system, was designed and applied to produce sulfurized PAC with a high specific surface area. Experimental tests involved the pyrolysis, activation, and sulfurization of waste tires. Waste-tire-derived PAC (WPAC) was initially produced in the pyrolysis and activation system. Experimental results indicated that the Brunauer-Emmett-Teller (BET) surface area of WPAC increased, and the average pore radius of WPAC decreased, as water feed rate and activation time increased. In this study, a conventional direct impregnation process was used to prepare the sulfurized PAC by impregnating WPAC with sodium sulfide (Na2S) solution. Furthermore, an innovative compositive impregnation process was developed and then compared with the conventional direct impregnation process. Experimental results showed that the compositive impregnation process produced the sulfurized WPAC with high BET surface area and a high S content. A maximum BET surface area of 886 m2/g and the S content of 2.61% by mass were obtained at 900 degrees C and at the S feed ratio of 2160 mg Na2S/g C. However, the direct impregnation process led to a BET surface area of sulfurized WPAC that decreased significantly as the S content increased.     

Effects of aerosol species on atmospheric visibility in Kaohsiung City, Taiwan

Visibility data collected from Kaohsiung City, Taiwan, for the past two decades indicated that the air pollutants have significantly degraded visibility in recent years. During our study period, the seasonal mean visibilities in spring, summer, fall, and winter were only 5.4, 9.1, 8.2, and 3.4 km, respectively. To ascertain how urban aerosols influence the visibility, we conducted concurrent visibility monitoring and aerosol sampling in 1999 to identify the principal causes of visibility impairments in the region. In this study, ambient aerosols were sampled and analyzed for 11 constituents, including water-soluble ions and carbon materials, to investigate the chemical composition of Kaohsiung aerosols. Stepwise regression method was used to correlate the impact of aerosol species on visibility impairments. Both seasonal and diurnal variation patterns were found from the monitoring of visibility. Our results showed that light scattering was attributed primarily to aerosols with sizes that range from 0.26 to 0.90 pm, corresponding with the wavelength region of visible light, which accounted for approximately 72% of the light scattering coefficient. Sulfate was a dominant component that affected both the light scattering coefficient and the visibility in the region. On average, (NH4)2SO4, NH4NO3, total carbon, and fine particulate matter (PM2.5)-remainder contributed 53%, 17%, 16%, and 14% to total light scattering, respectively. An empirical regression model of visibility based on sulfate, elemental carbon, and humidity was developed, and the comparison indicated that visibility in an urban area could be properly simulated by the equation derived herein.     

Preparation of Sulfurized Powdered Activated Carbon from Waste Tires Using an Innovative Compositive Impregnation Process

Abstract

The objective of this study is to develop an innovative compositive impregnation process for preparing sulfurized powdered activated carbon (PAC) from waste tires. An experimental apparatus, including a pyrolysis and activation system and a sulfur (S) impregnation system, was designed and applied to produce sulfurized PAC with a high specific surface area. Experimental tests involved the pyrolysis, activation, and sulfurization of waste tires. Waste-tire-derived PAC (WPAC) was initially produced in the pyrolysis and activation system. Experimental results indicated that the Brunauer-Emmett-Teller (BET) surface area of WPAC increased, and the average pore radius of WPAC decreased, as water feed rate and activation time increased. In this study, a conventional direct impregnation process was used to prepare the sulfurized PAC by impregnating WPAC with sodium sulfide (Na₂S) solution. Furthermore, an innovative compositive impregnation process was developed and then compared with the conventional direct impregnation process. Experimental results showed that the compositive impregnation process produced the sulfurized WPAC with high BET surface area and a high S content. A maximum BET surface area of 886 m²/g and the S content of 2.61% by mass were obtained at 900°C and at the S feed ratio of 2160 mg Na₂S/g C. However, the direct impregnation process led to a BET surface area of sulfurized WPAC that decreased significantly as the S content increased.     

The adsorptive capacity of vapor-phase mercury chloride onto powdered activated carbon derived from waste tires

Injection of powdered activated carbon (PAC) upstream of particulate removal devices (such as electrostatic precipitator and baghouses) has been used effectively to remove hazardous air pollutants, particularly mercury-containing pollutants, emitted from combustors and incinerators. Compared with commercial PACs (CPACs), an alternative PAC derived from waste tires (WPAC) was prepared for this study. The equilibrium adsorptive capacity of mercury chloride (HgCl2) vapor onto the WPAC was further evaluated with a self-designed bench-scale adsorption column system. The adsorption temperatures investigated in the adsorption column were controlled at 25 and 150 degrees C. The superficial velocity and residence time of the flow were 0.01 m/sec and 4 sec, respectively. The adsorption column tests were run under nitrogen gas flow. Experimental results showed that WPAC with higher Brunauer-Emmett-Teller (BET) surface area could adsorb more HgCl2 at room temperature. The equilibrium adsorptive capacity of HgCl2 for WPAC measured in this study was 1.49 x 10(-1) mg HgCl2/g PAC at 25 degrees C with an initial HgCI2 concentration of 25 microg/m3. With the increase of adsorption temperature < or = 150 degrees C, the equilibrium adsorptive capacity of HgCl2 for WPAC was decreased to 1.34 x 10(-1) mg HgCl2/g PAC. Furthermore, WPAC with higher sulfur contents could adsorb even more HgCl2 because of the reactions between sulfur and Hg2+ at 150 degrees C. It was demonstrated that the mechanisms for adsorbing HgCl2 onto WPAC were physical adsorption and chemisorption at 25 and 150 degrees C, respectively. Experimental results also indicated that the apparent overall driving force model appeared to have the good correlation with correlation coefficients (r) > 0.998 for HgCl2 adsorption at 25 and 150 degrees C. Moreover, the equilibrium adsorptive capacity of HgCl2 for virgin WPAC was similar to that for CPAC at 25 degrees C, whereas it was slightly higher for sulfurized WPAC than for CPAC at 150 degrees C.     

Nitrogen isotope composition of ammonium in PM2.5 in the Xiamen,China: impact of non-agricultural ammonia

Environmental Science and Pollution Research - Since NH3 is a significant precursor to ammonium in PM2.5 and contributes significantly to atmospheric nitrogen deposition but largely remains...