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Ball milled biochar effectively removes sulfamethoxazole and sulfapyridine antibiotics from water and wastewater
2020
Wong, Kam Sing | Zimmerman, Andrew R. | Chen, Hao | Gao, Bin
Release of antibiotics into the environment, which often occurs downstream of wastewater treatment plants, poses a human health threat due to the potential development of bacterial antibiotic resistance. In this study, laboratory experiments were conducted to evaluate the performance of ball milled biochar on the removal of two sulfonamide antibiotics, sulfamethoxazole (SMX) and sulfapyridine (SPY) from water and wastewater. Aqueous batch sorption experiment using both pristine and ball milled biochar derived from bagasse (BG), bamboo (BB) and hickory chips (HC), made at three pyrolysis temperatures (300, 450, 600 °C), showed that ball milling greatly enhanced the SMX and SPY adsorption. The 450 °C ball milled HC biochar and BB biochar exhibited the best removal efficiency for SMX (83.3%) and SPY (89.6%), respectively. A range of functional groups were produced by ball milling, leading to the conclusion that the adsorption of sulfonamides on the biochars was controlled by multiple mechanisms including hydrophobic interaction, π–π interaction, hydrogen bonding, and electrostatic interaction. Due to the importance of electrostatic interaction, SMX and SPY adsorption was pH dependent. In laboratory water solutions, the Langmuir maximum adsorption capacities of SMX and SPY reached 100.3 mg/g and 57.9 mg/g, respectively. When tested in real wastewater solution, the 450 °C ball milled biochar still performed well, especially in the removal of SPY. The maximum adsorption capacities of SMX and SPY in wastewater were 25.7 mg/g and 58.6 mg/g, respectively. Thus, ball milled biochar has great potential for SMX and SPY removal from aqueous solutions including wastewater.
Show more [+] Less [-]Activation of percarbonate by water treatment sludge–derived biochar for the remediation of PAH-contaminated sediments
2020
Hung, Chang-Mao | Huang, Jinbao | Chen, Chiu-Wen | Wu, Chung-Hsin | Lin, Yi-Li | Dong, Cheng-Di
Sludge from a groundwater treatment plant was used to prepare biochar by pyrolysis. The Fe–Mn rich biochar was used to activate percarbonate for the remediation of polycyclic aromatic hydrocarbons (PAHs) contaminated aquatic sediments. Results showed that the sludge–derived biochar (SBC) produced at a pyrolysis temperature of 700 °C was the most effective in activating percarbonate, which exhibited significant oxidative removal of PAHs. PAHs degradation took place via a Fenton-like oxidation manners, contributed from the Fe³⁺/Fe²⁺ and Mn³⁺/Mn²⁺ redox pairs, and achieved the highest degradation efficiency of 87% at pH₀ 6.0. Reactions between oxygenated functional groups of biochar and H₂O₂ generated of O₂•– and HO• radicals in abundance under neutral and alkaline pH was responsible for the catalytic degradation of PAHs. Our results provided new insights into the environmental applications of SBC for the green sustainable remediation of organics-contaminated sediments and aided in reduction of associated environmental and health risk.
Show more [+] Less [-]Fe1-xS/biochar combined with thiobacillus enhancing lead phytoavailability in contaminated soil: Preparation of biochar, enrichment of thiobacillus and their function on soil lead
2020
Ye, Junpei | Liao, Wenmin | Zhang, Panyue | Li, Juan | Nabi, Mohammad | Wang, Siqi | Cai, Yajing | Li, Fan
Properly increasing mobility of heavy metals could promote phytoremediation of contaminated soil. Fe₁₋ₓS/biochar was successfully prepared from sawdust with loading pyrrhotite (Fe₁₋ₓS) at a pyrolysis temperature of 550 °C. Thiobacillus were successfully adsorbed and enriched on the surface of Fe₁₋ₓS/biochar. Microbial growth for 36 d supported by bio-oxidization of Fe₁₋ₓS decreased the system pH from 4.32 to 3.50, increased the ORP from 298 to 487 mV, and the Fe³⁺ release reached 25.48 mg/g, enhancing the oxidation and leaching of soil Pb. Finally, Fe₁₋ₓS/biochar and Thiobacillus were simultaneously applied into Pb-contaminated soil for 60 d, the soil pH decreased from 7.83 to 6.72, and the exchangeable fraction of soil Pb increased from 22.86% to 37.19%. Ryegrass planting for 60 d in Pb-contaminated soil with Fe₁₋ₓS/biochar and Thiobacillus showed that the Pb content in shoot and root of ryegrass increased by 55.65% and 73.43%, respectively, confirming an obvious increase of phytoavailability of soil Pb. The relative abundance of Thiobacillus in remediated soil significantly increased from 0.06% to 34.55% due to the addition of Fe₁₋ₓS/biochar and Thiobacillus. This study provides a novel approach for regulating the Pb phytoavailability for phytoremediation of Pb-contaminated soil.
Show more [+] Less [-]Mechanistic insights and multiple characterizations of cadmium binding to animal-derived biochar
2020
Lei, Sicong | Zhu, Ling | Xue, Cong | Hong, Chengyi | Wang, Junliang | Che, Lei | Hu, Yongfeng | Qiu, Yuping
Cattle-derived biochar (CB), which is derived from industrial pyrolysis of cattle carcasses in harmless treatment plants, is a naturally occurring mineral form of carbonate-bearing hydroxyapatite (CHAP) with a small amount of elemental carbon. CB has 4.02% of carbonate content, which falls under the B-type substitution of CHAP. In this work, the Cd(II) sorption capacity of CB was determined to be 0.82 mmol/g, with 97.6% of the Cd(II) uptake contributing to CHAP and only 2.36% of the Cd(II) uptake contributing to the elemental carbon component. The calculation and linear combination fitting (LCF) of Cd L₃-edge X-ray absorption near-edge structure (XANES) analysis indicated that the contributions of Cd(II) species to CB presented the following order: ion exchange (57.6%–61.0%) > precipitation (24.4%–29.9%) > surface complexation (12.5%–13.4%). The depth dependent X-ray photoelectron spectroscopy (XPS) showed the presence of ion exchange, which is accompanied by intraparticle diffusion. LCF of XANES and Rietveld analysis of X-ray diffraction (XRD) demonstrated that Cd(II) was precipitated in the form of Cd₅H₂(PO₄)₄·4H₂O on the CB surface. Furthermore, the precipitate was directly observed and identified by scanning electron microscopy with energy-dispersive spectroscopy (SEM-EDS). Consequently, we revealed the intricate binding mechanism of Cd(II) to CHAP-rich CB and confirmed the importance of surface precipitation.
Show more [+] Less [-]Simultaneous removal of arsenic, cadmium, and lead from soil by iron-modified magnetic biochar
2020
Wan, Xiaoming | Li, Chongyang | Parikh, Sanjai J.
Effective and economically viable method to remove elevated metal(loid)s from farm and industrial lands remains a major challenge. In this study, magnetic biochar-based adsorbents with Fe₃O₄ particles embedded in a porous biochar matrix was synthesized via iron (Fe) treated biochar or thermal pyrolysis of Fe treated cedar sawdust. Application and separation of the adsorbent to a multi-contaminated soil slurry simultaneously removed 20–30% of arsenic, cadmium and lead within 24 h. Fast removal of multi-metal(loid)s result from the decrease in all operationally defined fractions of metal(loid)s, not limited to the exchangeable fraction. The direct removal of arsenic-enriched soil particles was observed via micro X-ray fluorescence maps. Furthermore, through comparison of biochars with different production methods, it has been found that magnetization after pyrolysis treatment leads to stronger metals/metalloids adsorption with a higher qₑ (bound sorbate) than other treatments but pyrolysis after magnetization stabilized Fe oxides on the biochar surface, indicating a higher biochar recovery rate (∼65%), and thus a higher metal(loid)s removal efficiency. The stability of Fe oxides on the surface of biochar is the determining factor for the removal efficiency of metal(loid)s from soil.
Show more [+] Less [-]Environmental forensics of complexly contaminated sites: A complimentary fingerprinting approach
2020
Kruge, Michael A. | Lara-Gonzalo, Azucena | Gallego, José Luis R.
The environmental forensics approach is most often applied in petroleum and fuel spill incidents, for which sophisticated chemical fingerprinting procedures have evolved. In cases in which pollutant discharges occur in settings with prior contamination, more care must be taken in source discrimination, requiring further advances in methodology. Additional obstacles can arise if the spill is an atypical industrial discharge. This would necessitate painstaking characterization of unfamiliar substances lying outside of existing regulatory regimes and thus overlooked by mandated analytical protocols (i.e., contaminants of emerging concern). Towards these ends, this paper presents a systematic, multi-faceted GC-MS approach using the saturated, aromatic, and resin fractions of contaminated soil extracts, alongside soil thermal desorption and analytical pyrolysis of the soil and its asphaltene fraction. This complimentary “extract + thermal” approach is applied to a typical fuel oil spill, sediments of a severely-impacted urban river, and brownfield soils from coke, petrochemical, and Hg-As pyrometallurgical plants. The insights thus attained can serve to better inform brownfield remediation planning in the public interest.
Show more [+] Less [-]Nitrogen and sulfur co-doped biochar derived from peanut shell with enhanced adsorption capacity for diethyl phthalate
2020
Guo, Ruishui | Yan, Lili | Rao, Pinhua | Wang, Runkai | Guo, Xin
Doping of nitrogen and sulfur on biochar (NS-B) was investigated by a novel and improved method for diethyl phthalate (DEP) removal. The preparation parameters including pyrolysis temperature and size of peanut shell biochar as well as thiourea/biochar mass ratio were selected as independent variables at three levels by applying the Box-Behnken design. The ANOVA results indicated that thiourea/biochar mass ratio exhibited the most significant effect. The comprehensive effects of the three factors on DEP removal efficiency were further elaborated, combining with the characterization results of the obtained NS-B materials. The formation of the pyridinic N and oxidized S groups examined by XPS was responsible for enhancing the DEP removal efficiency. The adsorption kinetic model fitting illustrated that large micropores and numerous adsorption sites improved the adsorption capacity of NS-B. According to the adsorption isotherm model fitting, NS-B (temperature 375 °C, size 300 mesh and thiourea/biochar mass ratio 0.1) possessed much higher maximum adsorption capacity for DEP (14.34 mg g⁻¹) than biochar (6.57 mg g⁻¹). NS-B exhibited excellent reusability towards DEP removal after five times recycling. Moreover, NS-B also had the potential in peroxydisulfate activation. These findings provide new insights into the environmental implications of NS-B.
Show more [+] Less [-]Effect of pyrolysis conditions on bone char characterization and its ability for arsenic and fluoride removal
2020
Alkurdi, Susan S.A. | Al-Juboori, Raed A. | Bundschuh, Jochen | Bowtell, Les | McKnight, Stafford
This study examined arsenite [As(III)], arsenate [As(V)] and fluoride (F⁻) removal potential of bone char produced from sheep (Ovis aries) bone waste. Pyrolysis conditions tested were in the 500 °C–900 °C range, for a holding time of 1 or 2 h, with or without N₂ gas purging. Previous bone char studies mainly focused on either low or high temperature range with limited information provided on As(III) removal. This study aims to address these gaps and provide insights into the effect of pyrolysis conditions on bone char sorption capacity. A range of advanced chemical analyses were employed to track the change in bone char properties. As pyrolysis temperature and holding time increased, the resulting pH, surface charge, surface roughness, crystallinity, pore size and CEC all increased, accompanied by a decrease in the acidic functional groups and surface area. Pyrolysis temperature was a key parameter, showing improvement in the removal of both As(III) and As(V) as pyrolysis temperature was increased, while As(V) removal was higher than As(III) removal overall. F⁻ removal displayed an inverse relationship with increasing pyrolysis temperature. Bone char prepared at 500 °C released significantly more dissolved organic carbon (DOC) then those prepared at a higher temperature. The bone protein is believed to be a major factor. The predominant removal mechanisms for As were surface complexation, precipitation and interaction with nitrogenous functional groups. Whereas F⁻ removal was mainly influenced by interaction with oxygen functional groups and electrostatic interaction. This study recommends that the bone char pyrolysis temperature used for As and F⁻ removal are 900 °C and 650 °C, respectively.
Show more [+] Less [-]In-situ biodegradation of harmful pollutants in landfill by sludge modified biochar used as biocover
2020
Qin, Linbo | Huang, Xinming | Xue, Qiang | Liu, Lei | Wan, Yong
MSW landfill releases a lot of harmful pollutants such as H₂S, NH₃, and VOCs. In this study, two laboratory-scale biocovers such as biochar (BC) derived from agricultural & forestry wastes (AFW) pyrolysis, and sludge modified the biochar (SBC) were designed and used to remove the harmful pollutants. In order to understand in-situ biodegradation mechanism of the harmful pollutants by the SBC, the removal performances of the harmful pollutants together with the bacterial community in the BC and SBC were investigated in simulated landfill systems for 60 days comparing with the contrast experiment of a landfill cover soil (LCS). Meanwhile, the adsorption capacities of representative harmful pollutants (hydrogen sulfide, toluene, acetone and chlorobenzene) in the LCS, BC, and SBC were also tested in a fixed bed reactor. The removal efficiencies of the harmful pollutants by the SBC ranged from 95.43% to 100.00%, which was much higher than that of the LCS. The adsorption capacities of the harmful pollutants in the SBC were 4 times higher than that of the LCS since the SBC exhibited higher BET surface and N-containing functional groups. Meanwhile, the biodegradation rates of the harmful pollutants in the SBC were also much higher than that of the LCS since the populations of the bacterial community in the SBC were more abundant due to its facilitating the growth and activity of microorganisms in the porous structure of the SBC. In addition, a synergistic combination of adsorption and biodegradation in the SBC that enhanced the reproduction rate of microorganisms by consuming the absorbed-pollutants as carbon sources, which also contributed to enhance the biodegradation rates of the harmful pollutants.
Show more [+] Less [-]Peat burning – An important source of pyridines in the earth atmosphere
2020
Kosyakov, Dmitry S. | Ul’yanovskii, Nikolay V. | Latkin, Tomas B. | Pokryshkin, Sergey A. | Berzhonskis, Valeria R. | Polyakova, Olga V. | Lebedev, Albert T.
Studies of the chemical composition of atmospheric aerosols, rain water and snow in various regions of the globe quite often show the presence of pyridine and a number of its low mass derivatives. Nevertheless, the sources of those compounds in the environment have not yet been established and definitely require elucidation, supported by reliable experimental results. In the present work the chemical composition of peat combustion products as one of the important sources of atmospheric aerosol emission is studied by two-dimensional gas chromatography – high-resolution mass spectrometry with a focus on the detection of pyridine derivatives. Twenty-five compounds of this class were reliably identified and quantified in laboratory experiments on peat burning. Among them 3-hydroxypyridine predominates, while the rest analytes are mostly represented by alkyl derivatives: pyridine, 2-methylpyridine, 3-methylpyridine, 2,5-dimethylpyridine, 2,6-dimethylpyridine, 2-ethylpyridine, lutidines (in order of decreasing concentration). The distribution of these combustion products coincides with that obtained earlier in environmental studies carried out in Arctic, Central Russia and France. The experiments on peat thermal decomposition by pyrolysis GC-MS demonstrated that the maximum concentrations as well as the number of detected analytes were found under conditions of oxygen lack and a temperature of about 500 °C, i.e. characteristic conditions of peat wildfires. The observed levels of pyridines’ emission recalculated on the peat dry weight exceeded 200 mg kg⁻¹. Considering hundreds of millions tons of peat burning in megafires over 20,000 tons of pyridines penetrate the Earth atmosphere annually. The obtained results allow concluding that peat burning may be the major and still underestimated source of pyridine and lower alkylpyridines in the Earth atmosphere.
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