Abstract This study investigated the use of thermogravimetric analysis (TGA) to determine the adsorptive capacity and adsorption isotherm of vapor-phase mercury chloride on powdered activated carbon (PAC). The technique is commonly applied to remove mercury-containing air pollutants from gas streams emitted from municipal solid waste incinerators. An alternative form of powdered activated carbon derived from a pyrolyzed tire char was prepared for use herein. The capacity of waste tire-derived PAC to adsorb vapor-phase HgCl2 was successfully measured using a self-designed TGA adsorption system. Experimental results showed that the maximum adsorptive capacities of HgCl2 were 1.75, 0.688, and 0.230 mg of HgCl2 per gram of powdered activated carbon derived from carbon black at 30, 70, and 150 °C for 500 µg/m3 of HgCl2, respectively. Four adsorption isotherms obtained using the Langmuir, Freundlich, Redlich-Peterson, and Brunauer–Emmett–Teller (BET) models were used to simulate the adsorption of HgCl2. The comparison of experimental data associated with the four adsorption isotherms indicated that BET fit the experimental results better than did the other isotherms at 30 °C, whereas the Freundlich isotherm fit the experimental results better at 70 and 150 °C. Furthermore, the calculations of the parameters associated with Langmuir and Freundlich isotherms revealed that the adsorption of HgCl2 by PAC-derived carbon black favored adsorption at various HgCl2 concentrations and temperatures. 相似文献
Abstract 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 °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 × 10?1 mg HgCl2/g PAC at 25 °C with an initial HgCl2 concentration of 25 μg/m3. With the increase of adsorption temperature ≤150 °C, the equilibrium adsorptive capacity of HgCl2 for WPAC was decreased to 1.×34 10?1 mg HgCl2/g PA≤C. Furthermore,WPAC with higher sulfur contents could adsorb even more HgCl2 because of the reactions between sulfur and Hg2+ at 150 °C. It was demonstrated that the mechanisms for adsorbing HgCl2 onto WPAC were physical adsorption and chemisorption at 25 and 150 °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 °C. Moreover, the equilibrium adsorptive capacity of HgCl2 for virgin WPAC was similar to that for CPAC at 25 °C, whereas it was slightly higher for sulfurized WPAC than for CPAC at 150 °C. 相似文献
Some metal etching operations emit limited flow rates of waste gases with reddish-brown NO2 fume, which may cause visual and acidic-odor complaints, as well as negative health effects. In this study, tests were performed by passing caustic-treated waste gases vented from Al-etching operations through columns packed either with virgin or regenerated granular activated carbon (GAC) to test their adsorptive conversion performance of NO2 in the gases. The gases contained 5–55 ppm NO2 and acetic and nitric acids of below 3 ppm. Exhausted carbon was regenerated by scrubbing it with caustic solution and water, and dried for further adsorption tests. Results indicate that with an (empty bed residence time (EBRT) of 0.15 sec for the gas through the GAC-packed space, around 60% of the influent NO2 of 54 ppm could be removed, and 47% of the removed NO2 was converted by and desorbed from the carbon as NO. GAC used in the present study could be regenerated at least twice to restore its capacity for NO2 adsorption. Within EBRTs of 0.076–0.18 sec, the adsorptive conversion capacity was linearly varied with EBRT. In practice, with an EBRT of 0.20 sec, a conversion capacity of 0.80 kg NO2 (kg GAC)?1 with an influent NO2 of 40 ppm can be used as a basis for system design.Implications: Some metal etching operations emit waste gases with reddish-brown (yellow when diluted) NO2 fume which may cause visual and acidic-odor complaints, as well as negative health effects. This study provides a simple process for the adsorptive conversion of NO2 in caustic-treated waste gases vented from metal-etching operations through a GAC column. With an EBRT of 0.20 sec, a conversion capacity of 0.80 kg NO2 (kg GAC)?1 with an influent NO2 of 40 ppm can be used as a basis for system design. Saturated GAC can be regenerated at least twice by simply scrubbing it with aqueous caustic solution. 相似文献
ABSTRACT The capture of elemental mercury (Hg0) and mercuric chloride (HgCl2) by three types of calcium (Ca)-based sor-bents was examined in this bench-scale study under conditions prevalent in coal-fired utilities. Ca-based sorbent performances were compared with that of an activated carbon. Hg0 capture of about 40% (nearly half that of the activated carbon) was achieved by two of the Ca-based sorbents. The presence of sulfur dioxide (SO2) in the simulated coal combustion flue gas enhanced the Hg0 capture from about 10 to 40%. Increasing the temperature in the range of 65-100 °C also caused an increase in the Hg0 capture by the two Ca-based sorbents. Mercuric chloride (HgCl2) capture exhibited a totally different pattern. The presence of SO2 inhibited the HgCl2 capture by Ca-based sorbents from about 25 to less than 10%. Increasing the temperature in the studied range also caused a decrease in HgCl2 capture. Upon further pilot-scale confirmations, the results obtained in this bench-scale study can be used to design and manufacture more cost-effective mercury sorbents to replace conventional sorbents already in use in mercury control. 相似文献
Activated carbon was one of the main adsorptions utilized in elemental mercury (Hg0) removal from coal combustion flue gas. However, the high cost and low physical adsorption efficiency of activated carbon injection (ACI) limited its application. In this study, an ultra-high efficiency (nearly 100%) catalyst sorbent-Sex/Activated carbon (Sex/AC) was synthesized and applied to remove Hg0 in the simulated flue gas, which exhibited 120 times outstanding adsorption performance versus the conventional activated carbon. The Sex/AC reached 17.98 mg/g Hg0 adsorption capacity at 160 °C under the pure nitrogen atmosphere. Moreover, it maintained an excellent mercury adsorption tolerance, reaching the efficiency of Hg0 removal above 85% at the NO and SO2 conditions in a bench-scale fixed-bed reactor. Characterized by the multiple methods, including BET, XRD, XPS, kinetic and thermodynamic analysis, and the DFT calculation, we demonstrated that the ultrahigh mercury removal performance originated from the activated Se species in Sex/AC. Chemical adsorption plays a dominant role in Hg0 removal: Selenium anchored on the surface of AC would capture Hg0 in the flue gas to form an extremely stable substance-HgSe, avoiding subsequent Hg0 released. Additionally, the oxygen-containing functional groups in AC and the higher BET areas promote the conversion of Hg0 to HgO. This work provided a novel and highly efficient carbon-based sorbent -Sex/AC to capture the mercury in coal combustion flue gas.
An activated carbon commercially available named HGR, produced by Calgon-Carbon Group, was used to adsorbe metallic mercury. The work is part of a wider research activity by the same group focused on the removal of metallic and divalent mercury from combustion flue gas. With respect to previously published papers, this one is aimed at studying in depth thermodynamic equilibria of metallic mercury adsorption onto a commercial activated carbon. The innovativeness lies in the wider operative conditions explored (temperature and mercury concentrations) and in the evaluation of kinetic and thermodynamic data for a commercially available adsorbing material. In detail, experimental runs were carried out on a laboratory-scale plant, in which Hg° vapors were supplied in a nitrogen gas stream at different temperature and mercury concentration. The gas phase was flowed through a fixed bed of adsorbent material. Adsorbate loading curves for different Hg° concentrations together with adsorption isotherms were achieved as a function of temperature (120, 150, 200°C) and Hg° concentrations (1.0?7.0 mg/m3). Experimental runs demonstrated satisfying results of the adsorption process, while Langmuir parameters were evaluated with gas–solid equilibrium data. Especially, they confirmed that adsorption capacity is a favored process in case of lower temperature and they showed that the adsorption heat was –20 kJ/mol. Furthermore, a numerical integration of differential equations that model the adsorption process was proposed. Scanning electron microscopy (SEM) investigation was an useful tool to investigate about fresh and saturated carbon areas. The comparison between them allowed identification of surface sites where mercury is adsorbed; these spots correspond to carbon areas where sulfur concentration is greater.Implications: Mercury compounds can cause severe harm to human health and to the ecosystem. There are a lot of sources that emit mercury species to the atmosphere; the main ones are exhaust gases from coal combustion and municipal solid waste incineration. Furthermore, certain CO2 capture processes, particularly oxyfuel combustion in a pulverized fuel coal-fired power station, produce a raw CO2 product containing several contaminants, mainly water vapor, oxygen, and nitrogen but also mercury, that have to be almost completely removed; otherwise these would represent a strong drawback to the success of the process. 相似文献