Shoujun Yuan

Removal of Congo Red from aqueous solution by cattail root

In this study, cattail root was used to remove Congo Red (CR) from aqueous solution. The effects of operation variables, such as cattail root dosage, contact time, initial pH, ionic strength and temperature on the removal of CR were investigated using batch adsorption technique. Removal efficiency increased with increase of cattail root dosage and ionic strength, but decreased with increase of temperature. The equilibrium data fitted well to the Langmuir model (R(2)>0.98) and the adsorption kinetic followed the pseudo-second-order equation (R(2)>0.99). Thermodynamics parameters such as standard free energy change (Delta G degrees), standard enthalpy change (Delta H degrees), and standard entropy change (DeltaS degrees ) were analyzed. The values of Delta G degrees were between -7.871 and -4.702 kJ mol(-1), of Delta H degrees was -54.116 kJ mol(-1), and of DeltaS degrees was -0.157 kJ mol(-1)K(-1), revealing that the removal of CR from aqueous solution by cattail root was a spontaneous and exothermic adsorption process. The maximum adsorption capacities of CR on cattail root were 38.79, 34.59 and 30.61 mg g(-1) at 20, 30 and 40 degrees C, respectively. These results suggest that cattail root is a potential low-cost adsorbent for the dye removal from industrial wastewater.

Electrochemical Stimulation of Microbial Roxarsone Degradation under Anaerobic Conditions

Roxarsone (4-hydroxy-3-nitrophenylarsonic acid) has been commonly used in animal feed as an organoarsenic additive, most of which is excreted in manure. Roxarsone is easily biodegraded to 4-hydroxy-3-aminophenylarsonic acid (HAPA) under anaerobic conditions, but HAPA persists for long periods in the environment, increasing the risk of arsenic contamination through diffusion. We investigated the electrochemical stimulation of the microbial degradation of roxarsone under anaerobic conditions. After the carbon sources in the substrate were depleted, HAPA was slowly degraded to form arsenite under anaerobic conditions. The degradation rate of HAPA was significantly increased when 0.5 V was applied without adding a carbon source. The two-cell membrane reactor assays reveal that the HAPA was degraded in the anode chambers, confirming that the anode enhanced the electron transfer process by acting as an electron acceptor. The degradation product formed with electrochemical stimulation was arsenate, which facilitates the removal of arsenic from wastewater. Based on the high performance liquid chromatography-ultraviolet-hydride generation-atomic fluorescence spectrometry (HPLC-UV-HG-AFS) and gas chromatography-mass spectrometry (GC-MS) data, the pathway for the biodegradation of roxarsone and the mechanisms for the electrochemically stimulated degradation are proposed. This method provides a potential solution for the removal of arsenic from organoarsenic-contaminated wastewater.

Biodegradation and speciation of roxarsone in an anaerobic granular sludge system and its impacts

Roxarsone (3-nitro-4-hydroxy benzene arsenic acid) is an organoarsenic feed additive and has been widely used in the poultry industry to prevent coccidiosis and improve feed efficiency. The presence of roxarsone and its degradation products results in the instability of the anaerobic methanogenic process. This study investigated the degradation and speciation of roxarsone in an anaerobic granular sludge (AGS) system and the impacts of roxarsone and its degradation products on the structure of AGS. Roxarsone inhibited methane production, and the added roxarsone was rapidly degraded into 3-amino-4-hydroxyphenylarsonic acid (HAPA). After 240 days of incubation, the distribution of arsenic differed between the aqueous solution and the AGS in the assays of 20 and 350mg/L roxarsone. Species analysis indicated that HAPA was completely degraded in all of the assays with roxarsone addition after 240 days of incubation. Species distribution was affected by the phases and the initial concentration of roxarsone added. The concentration of As(III) was higher than that of As(V) in both the aqueous solution and the AGS in all assays with roxarsone addition. The toxicity of roxarsone and its degradation products resulted in changes in the structure and the microorganism species in the AGS.

Adsorption and photocatalytic decomposition of roxarsone by TiO2 and its mechanism

Roxarsone (3-nitro-4-hydroxyphenylarsonic acid) has been widely used as organic arsenic additive in animal industry. In this study, the adsorption of roxarsone on TiO2 under dark conditions, the photocatalytic decomposition of roxarsone under UV/TiO2, and the possible photocatalytic pathway were investigated. At the initial concentration of 5–35xa0mg/L, the adsorption of roxarsone fitted well with the pseudo-second-order kinetics. The isotherms analysis showed that the Langmuir model was better than the Freundlich and Dubinin–Radushkevich models for describing the adsorption process. After 7xa0h of photocatalytic decomposition, a complete disappearance of roxarsone was achieved. The pH value has a significant effect on both adsorption and photocatalytic decomposition of roxarsone. The results of high-performance liquid chromatography-hydride generation-atomic fluorescence spectrometry (HPLC-HG-AFS) and gas chromatography-mass spectrometry (GC/MS) analyses proved the cleavage of the As-C bond during the photocatalytic decomposition process by TiO2 and the intermediates of the decomposition. Based on the results, a possible photocatalytic decomposition pathway was proposed.

Degradation of aqueous 3,4-dichloroaniline by a novel dielectric barrier discharge plasma reactor.

Degradation of aqueous 3,4-dichloroaniline (3,4-DCA) was conducted in a novel dielectric barrier discharge (DBD) plasma reactor. The factors affecting the degradation efficiency of 3,4-DCA and the degradation mechanism of 3,4-DCA were investigated. The experimental results indicated that the degradation efficiency of 3,4-DCA increased with increasing input power intensity, and the degradation of 3,4-DCA by the novel DBD plasma reactor fitted pseudo-first-order kinetics. Higher degradation efficiency of 3,4-DCA was observed in acidic conditions. The degradation efficiency of 3,4-DCA, the removal rate of total organic carbon (TOC), and the detected Cl− increased dramatically with adding Fe2+ or Fe3+. Degradation of 3,4-DCA could be accelerated or inhibited in the presence of H2O2 depending on the dosage. Several degradation intermediates of 3,4-DCA such as 1,2-dichlorobenzene, 2-chloro-1,4-benzoquinone, 3,4-dichlorophenyl isocyanate, 2-chlorohydroquinone, 3,4-dichloronitrobenzene, and 3,4-dichlorophenol were identified by gas chromatography mass spectrometry (GC-MS) analysis. Based on the identification of aromatic intermediates, acetic acid, formic acid, oxalic acid, and Cl− released, a possible mineralization pathway of 3,4-DCA was proposed.

Potential impact of methyl isobutyl ketone (MIBK) on phenols degradation in an UASB reactor and its degradation properties

Methyl isobutyl ketone (MIBK) as a solvent is extensively used for the phenols extraction from the wastewater, so it is unavoidable to expose in the effluent due to the solubility and leakage problem. The present study evaluated the impact of MIBK on phenols degradation in an UASB reactor and analyzed its degradation properties. The results indicated that the continuous dosing (0.1gL-1) and impact (10gL-1) of MIBK had limited effect on phenols removal (1-2% reduction) in the UASB reactor, but the specific methanogenic activity (SMA) values of sludge decreased by 45-75% after MIBK exposure. Anaerobic degradation rate of MIBK fitted well to a pseudo-first-order kinetic equation with respect to the initial concentration of 35mgL-1 (k=0.0115h-1, R2=0.9664). Furthermore, the relative methane generation rate constants of MIBK were 0.00816, 0.00613, 0.00273, and 0.00207d-1 at the initial concentrations of 0.1, 0.5, 5, and 10gL-1, respectively. MIBK showed higher inhibitory effect on the methanogenesis than on phenols degradation. This study pointed out that the industrial installations should consider the influence of solvent on anaerobic treatment of phenolic wastewater.

Impact of roxarsone on the UASB reactor performance and its degradation

Roxarsone (3-nitro-4-hydroxyphenylarsonic acid, ROX) has been widely used for decades as an organoarsenic feed additive to control intestinal parasites and improve feed efficiency in animal production. However, most of the ROX is excreted into the manure, causing arsenic contamination in wastewater. The arsenic compounds are toxic to microorganisms, but the influence of continuous ROX loading on upflow anaerobic sludge blanket (UASB) reactor is still unknown. In this study, the impact of ROX and its degradation products on the performance of the UASB reactor and the degradation and speciation of ROX in the reactor were investigated. The UASB reactor (hydraulic retention time: 1.75 d) was operated using synthetic wastewater supplemented with ROX for a period of 260 days. With continuous ROX addition at 25.0 mg·L–1, severe inhibition to methanogenic activity occurred after 87 days operation accompanied with an accumulation of volatile fatty acids (VFAs) and a decline in pH. The decrease of added ROX concentration to 13.2 mg·L–1 did not mediate the inhibition. As(III), As (V), MMA(V), DMA(V), HAPA and an unknown arsenic compound were detected in the reactor, and a possible biotransformation pathway of ROX was proposed. Mass balance analysis of arsenic indicated that 60%–70% of the arsenic was discharged into the effluent, and 30%–40% was precipitated in the reactor. The results from this study suggest that we need to pay attention to the stability in the UASB reactors treating organoarsenic-contaminated manure and wastewater, and the effluent and sludge from the reactor to avoid diffusion of arsenic contamination.

Removal of roxarsone from aqueous solution by Fe/La-modified montmorillonite

AbstractRoxarsone is an organoarsenical compound widely used as a feed additive in animal husbandry and might result in the contamination of inorganic arsenic in aquatic environment. Montmorillonite is an economical adsorbent with many advantages. In this study, Fe/La-modified montmorillonite (Fe/La-Mt) was prepared, characterized, and investigated for the removal of roxarsone from aqueous solutions. Brunauer–Emmett–Teller (BET) analysis confirmed the increase in specific surface area and pore volume of montmorillonite after modification. FESEM analysis showed that Fe/La-Mt formed flake structure and the structure was collapsed after being calcined (C-Fe/La-Mt). The adsorption results indicated that the adsorption capacity of Fe/La-Mt onto roxarsone is higher than that of C-Fe/La-Mt. The adsorption process of roxarsone onto Fe/La-Mt and C-Fe/La-Mt can be well described using pseudo-second-order model and interpreted using the Langmuir isotherm. Thermodynamic analysis indicated that the adsorption was a sp...

Precipitation of organic arsenic compounds and their degradation products during struvite formation

Roxarsone (ROX) and arsanilic acid (ASA) have been extensively used as organoarsenic animal feed additives. Organic arsenic compounds and their degradation products, arsenate (As(V)) and arsenite (As(III)), exist in the effluent from anaerobic reactors treating animal manure contaminated by ROX or ASA with ammonium (NH4(+)-N) and phosphate (PO4(3-)-P) together. Therefore, arsenic species in the effluent might be involved in the struvite formation process. In this study, the involvement of organic arsenic compounds and their degradation products As(V) and As(III) in the struvite crystallization was investigated. The results demonstrated that arsenic compounds did not substantially affect the PO4(3-)-P recovery, but confirmed the precipitation of arsenic during struvite formation. The precipitation of arsenic compounds in struvite was considerably affected by a solution pH from 9.0 to 11.0. With an increase in pH, the content of ASA and ROX in the precipitation decreased, but the contents of As(III) and As(V) increased. In addition, the arsenic content of As(V) in the struvite was higher than that of As(III), ASA and ROX. The results indicated that the struvite could be contaminated when the solution contains arsenic species, but that could be minimized by controlling the solution pH and maintaining anaerobic conditions during struvite formation.

Adsorption characteristics of 4-hydroxy-3-aminophenylarsonic acid (HAPA) onto anaerobic granular sludge

AbstractFour-hydroxy-3-aminophenylarsonic acid (HAPA) is the degradation product of 3-nitro-4-hydroxyphenylarsonic acid (roxarsone, a widely used organoarsenic additive in animal feed) under anaerobic conditions. HAPA is highly water soluble and resistant to degradation by anaerobic micro-organisms. In this study, the effect of initial concentration, temperature, pH, ionic strength, and interferential ions on the adsorption of HAPA onto anaerobic granular sludge (AGS) was investigated using batch adsorption experiments. The results showed that equilibrium state of the adsorption was reached at about 10xa0h. The kinetics analysis indicated that the adsorption process followed a pseudo-second-order model and intra-particle diffusion was the rate-limiting step. The adsorption mechanisms could be explained by the Freundlich and D–R isotherm models. The maximum adsorption capacity of HAPA onto AGS was 12.57, 25.05, and 26.31xa0mg/g at 15, 25, and 35°C, respectively. pH, ionic strength, and phosphate ions had obvio...