Arsenic contamination caused by roxarsone transformation with spatiotemporal variation of microbial community structure in a column experiment

Arsenic contamination from roxarsone in livestock manure is common,and livestock manure continuously accumulates in the open environment.Evaluations of the environmental processes of As mobilization and transformation are critical for predicting the fate of As compounds after roxarsone degradation.In this study,spatiotemporal variations in As species and microbial community structure were characterized using laboratory column experiments with background soil collected from Yanggu County(northern Shandong Plain,China),a region of intense poultry production.Organic and inorganic arsenic were detected by high-performance liquid chromatography(HPLC)and HPLC with hydride generation atomic fluorescence spectrometry(HPLC-HG-AFS),respectively.High-throughput sequencing technology was used to describe microbial diversity.Results showed that roxarsone was transformed completely within 7 days,and A_(s)(Ⅲ)and As(Ⅴ)were the major degradation products.The concentration of A_(s)(Ⅲ)was much lower than that of As(Ⅴ).The A_(s)(Ⅲ)concentration increased significantly after Day 14,whereas the A_(s)(Ⅴ)concentration increased significantly after Day 84,indicating that A_(s)(Ⅲ)was initially produced.The microbial community structure changed significantly as roxarsone transformed into various As compounds.A critical and dominant bacterial strain,norank_f__Family_XVⅢ,was found to be related to the degradation of roxarsone into As(Ⅲ).This study improves our understanding of the fate of As species released from poultry litter to soil and groundwater,which is a threat to human health and environment.

Research Progress on the Mechanism of Groundwater Arsenic Contamination Caused by Animal Feed Additives with Roxarsone

Firstly, the general situation of arsenic pollution caused by livestock and poultry industry at home and abroad was introduced, and then the transformation and adsorption of roxarsone in the environment were analyzed, finally the control measures of roxarsone pollution was discussed,

Adsorption removal of roxarsone, arsenite(Ⅲ),and arsenate(Ⅴ) using iron-modified sorghum straw biochar and its kinetics

Arsenic(As)contamination in groundwater is a major problem in many countries,which causes serious health issues.In this paper,a novel method has been developed for the simultaneous removal of ROX and As(Ⅲ/Ⅴ)using the modified sorghum straw biochar(MSSB).The MSSB was characterized by X-ray diffraction,scanning electron microscopy,Fourier Transform Infrared,and Brunauer–Emmet–Teller(BET)surface area.The removal performance of MSSB for ROX,arsenite[As(Ⅲ)],and arsenate(As(Ⅴ))was investigated using batch experiments.At pH of 5,the arsenic concentration of 1.0 mg/L,adsorbent dose of 1.0 g/L,the maximum adsorptioncapacities of ROX,As(Ⅲ),and As(Ⅴ)were 12.4,5.3,and 23.0 mg/g,respectively.The adsorption behaviors were fit well with the Langmuir and the pseudo-second-order rate model.The results showed that MSSB acted as a highly effective adsorbent to simultaneously remove the composite pollution system consisted of ROX and As(Ⅲ/Ⅴ)in aqueous solutions,providing a promising method in environmental restoration applications.

Permeation of roxarsone and its metabolites increases caco-2 cell proliferation

The benzenearsonate, Roxarsone, has been used since 1944 as an antimicrobial, growth-promoting poultry feed additive. USGS and EPA report that Roxarsone (4-hydroxy-3-nitrobenzenearsonate) and metabolites, including AHBA (3-amino-4-hydroxybenzenearsonate), contaminate waterways at greater than 1100 tons annually. To assess human impact of these organic arsenic water contaminants, it was important to study their potential absorption. The human adenocarcinoma cell line, Caco-2, is a model for intestinal absorption. We found proliferative effects on Caco-2 cells at micromolar levels of these compounds, as monitored by [3H]-thymidine incorporation into DNA. Flow cytometry cell cycle analysis confirmed accumulation in S phase from 21% (control) to 36% (24 hour exposure to 10 μM AHBA). Confluent Caco-2 cells grown on collagen-coated Transwell plates were dosed on the apical side. After exposure, media from apical and basolateral sides were collected separately. Following removal of FBS by 30K centrifugal filtration, the benzenearsonates in the collected media were analyzed by HPLC. Analyses were at wavelengths in the ultraviolet/visible range where the absorbance values were linear with respect to concentration. Concentrations were calculated by comparison with analytically-prepared commercial standards. Results from cells dosed at 10 μM for 24 hours with AHBA, Roxarsone, or Acetarsone indicated 6%-29% permeation occurring from apical to basolateral side, modeling absorption across intestinal epithelium to the circulatory system. Benzenearsonate feed additives are frequently applied in combination with antibiotics, raising additional health concerns. We conclude that micromolar levels of these benzenearsonates are adequate to stimulate Caco-2 cell proliferation.

The role of organic and inorganic substituents of roxarsone determines its binding behavior and mechanisms onto nano-ferrihydrite colloidal particles

The retention and fate of Roxarsone(ROX)onto typical reactive soil minerals were crucial for evaluating its potential environmental risk.However,the behavior and molecular-level reaction mechanism of ROX and its substituents with iron(hydr)oxides remains unclear.Herein,the binding behavior of ROX on ferrihydrite(Fh)was investigated through batch experiments and in-situ ATR-FTIR techniques.Our results demonstrated that Fh is an effective geo-sorbent for the retention of ROX.The pseudo-second-order kinetic and the Langmuir model successfully described the sorption process.The driving force for the binding of ROX on Fh was ascribed to the chemical adsorption,and the rate-limiting step is simultaneously dominated by intraparticle and film diffusion.Isotherms results revealed that the sorption of ROX onto Fh appeared in uniformly distributed monolayer adsorption sites.The twodimensional correlation spectroscopy and XPS results implied that the nitro,hydroxyl,and arsenate moiety of ROX molecules have participated in binding ROX onto Fh,signifying that the predominated mechanisms were attributed to the hydrogen bonding and surface complexation.Our results can help to better understand the ROX-mineral interactions at the molecular level and lay the foundation for exploring the degradation,transformation,and remediation technologies of ROX and structural analog pollutants in the environment.

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.

Livestock Antibiotic Effects on Nitrification, Denitrification, and Microbial Community Composition in Soils

The broiler (Gallus gallus domesticus) industry in the United States and several other countries routinely includes subtherapeutic levels of antibiotics such as roxarsone, virginiamycin, and bacitracin in the feed to improve bird growth yields. Large fractions of the antibiotics fed to the birds are excreted in manure (litter), which is often applied to soils to improve fertility. Some concerns with this practice are antibiotic-induced alterations in microbially-mediated nutrient cycling, which could influence plant productivity and environmental quality. To investigate this possibility, a series of lab experiments were conducted to determine the effects of increasing levels of the three livestock antibiotics on nitrification, denitrification, and microbial community composition (fatty acid methyl ester profiles) of soils collected along a catena. Roxarsone and virginiamycin significantly influenced microbial community composition and inhibited nitrification in the soils, but only at levels that were several-fold higher than expected in poultry litter-applied soils. Bacitracin did not affect microbial growth, microbial community composition, or nitrification at any concentration tested (up to 500 mg·kg-1). None of the antibiotics influenced denitrification at environmentally-relevant concentrations. Amounts of antibiotics in soil solution were greatly reduced by sorption, which followed Freundlich models in the concentration range of 1 -?500 mg·L-1. Results from this study indicated that addition of roxarsone, virginiamycin, or bacitracin to these soils at environmentally-relevant concentrations would not likely impact microbial community composition, nitrification or denitrification due to intrinsic resistance/insensitivity of microorganisms to these antibiotics and reductions in the bioavailable amounts due to sorption by soil surfaces.

Structural Study of Cellulose-Iron Oxide Composite Materials

There are limited structural studies of iron oxide coated cellulose materials despite their use as adsorbents for the removal of waterborne arsenic species. This study reports on the structural characterization of cellulose-iron oxide composites at variable iron oxide content using spectroscopy methods (Raman, solids 13C NMR, powder X-ray diffraction (pXRD)) and thermal gravi-metric analysis (TGA). Iron oxide was supported onto cellulose (ca. 25 wt.%) without significant loss in the Fe coating efficiency, where the accessibility of the biopolymer -OH groups affect the coating efficiency and yield of the iron oxide-cellulose composite. Isotherm adsorption studies for cellulose, iron oxide species and the cellulose composite materials with roxarsone (3-nitro- 4-hydroxyphenylarsonic acid) were studied to characterize the surface chemical properties of these potential adsorbent materials.