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Removal of heavy metal Cu(II) in simulated aquaculture wastewater by modified palygorskite
2016
Cao, Jia-Shun | Wang, Cheng | Fang, Fang | Lin, Jun-Xiong
Palygorskite (PAL) is a good heavy metal adsorbent due to its high surface area, low cost, and environmentally compatibility. But the natural PAL has limited its adsorption capacity and selectivity. In this study, a cost-effective and readily-generated absorbent, l-threonine-modified palygorskite (L-PAL), was used and its performance for Cu(II) removal in simulated aquaculture wastewater was evaluated. After preparation, L-PAL was characterized by using Fourier transform infrared spectroscopy, scanning electron microscope, energy dispersive X-ray spectroscopy, X-ray diffractometer, X-ray photoelectron spectroscopy, transmission electron microscopy and thermogravimetric analysis. The impacts of pH, adsorbent dosage, contact time, and initial Cu(II) concentration on the adsorption capacity of L-PAL were examined. The Cu(II) adsorption capacity on L-PAL was enhanced almost 10 times than that of raw PAL. The adsorption isotherms of Cu(II) fit the Langmuir isotherms, and the adsorption kinetics was dominated by the pseudo-second-order model. The thermodynamic parameters at four temperatures were calculated, which indicated that the adsorption was spontaneous and endothermic. The adsorption mechanism involves complexation, chelation, electrostatic attraction, and micro-precipitation. Furthermore, L-PAL is shown to have a high regeneration capacity. These results indicate that L-PAL is a cheap and promising absorbent for Cu(II) removal and hold potential to be used for aquaculture wastewater treatment.
Show more [+] Less [-]Sorption affinities of sulfamethoxazole and carbamazepine to two sorbents under co-sorption systems
2014
Wang, Chi | Li, Hao | Liao, Shaohua | Zhang, Di | Wu, Min | Pan, Bo | Xing, Baoshan
The Kd of sulfamethoxazole (SMX) on activated carbon (AC) was larger than that of SMX on single-walled carbon nanotubes (SC), but the competition of SMX with carbamazepine (CBZ) for adsorption sites was weaker on AC than SC. Thus, a large Kd value does not necessarily reflect a high affinity. The analysis of the apparent sorption, competition, desorption hysteresis, and the sorption thermodynamics for SMX and CBZ did not provide sufficient information to distinguish their sorption affinities. The release of the adsorbed CBZ was not altered with SMX as the competitor, but SMX release increased significantly after CBZ addition. The higher sorption affinity of CBZ may be explained by the interactions of the CBZ benzene rings with the aromatic structures of the adsorbents. Although the thermodynamic meaning cannot be described, the release ratio of the adsorbed pollutants provides useful information for understanding pollutant sorption strength and associated risks.
Show more [+] Less [-]Adsorption mechanism of two pesticides on polyethylene and polypropylene microplastics: DFT calculations and particle size effects
2021
Mo, Qiming | Yang, Xingjian | Wang, Jinjin | Xu, Huijuan | Li, Wenyan | Fan, Qi | Gao, Shuang | Yang, Wenyi | Gao, Chengzhen | Liao, Dehua | Li, Yongtao | Zhang, Yulong
Polyethylene (PE) and polypropylene (PP) microplastics (MPs), as carriers, can bind with pesticides, which propose harmful impacts to aqueous ecosystems. Meanwhile, carbofuran and carbendazim (CBD), two widely used carbamate pesticides, are toxic to humans because of the inhibition of acetylcholinesterase activity. The interaction between two MPs and two pesticides could start in farmland and be maintained during transportation to the ocean. Herein, the adsorption behavior and mechanism of carbofuran and carbendazim (CBD) by PE and PP MPs were investigated via characterization and density functional theory (DFT) simulation. The adsorption kinetic and thermodynamic data were best described by pseudo-second-order kinetics and the Freundlich models. The adsorption behaviors of individual carbofuran/CBD on both MPs were very similar. The CBD adsorption rate and capacity of PE and PP MPs were higher than those of carbofuran. This phenomenon explained the lower negative effects of DOM (oxalic acid, glycine (Gly)) on CBD adsorption relative to those of carbofuran. The presence of oxalic acid and Gly decreased the PE adsorption by 20.40–48.02% and the PP adsorption by 19.27–42.11%, respectively. It indicated the significance of DOM in carbofuran cycling. The adsorption capacities were negatively correlated with MPs size, indicating the importance of specific surficial area. Fourier transformation infrared spectroscopy before and after adsorption suggested that the adsorption process did not produce any new covalent bond. Instead, intermolecular van der Waals forces were one of the primary adsorption mechanisms of carbofuran and CBD by MPs, as evidenced by DFT calculations. Based on the zeta potential, the electrostatic interaction explained the higher adsorption CBD by MPs than carbofuran.
Show more [+] Less [-]Competitive adsorption of pharmaceuticals in lake water and wastewater effluent by pristine and NaOH-activated biochars from spent coffee wastes: Contribution of hydrophobic and π-π interactions
2021
Shin, Jaegwan | Kwak, Jinwoo | Lee, Yong-Gu | Kim, Sangwon | Choi, Minhee | Bae, Sungjun | Lee, Sang-Ho | Park, Yongeun | Chon, Kangmin
This study investigated the competitive adsorption mechanisms of pharmaceuticals (i.e., naproxen, diclofenac, and ibuprofen) toward the pristine and NaOH-activated biochars from spent coffee wastes (SCW) in lake water and wastewater effluent. The kinetic and isotherm studies revealed that the improved physicochemical characteristics and physically homogenized surfaces of the pristine SCW biochar through the chemical activation with NaOH were beneficial to the adsorption of pharmaceuticals (competitive equilibrium adsorption capacity (Qₑ, ₑₓₚ): NaOH-activated SCW biochar (61.25–192.07 μmol/g) > pristine SCW biochar (14.81–20.65 μmol/g)). The adsorptive removal of naproxen (Qₑ, ₑₓₚ = 14.81–18.81 μmol/g), diclofenac (Qₑ, ₑₓₚ = 15.73–20.00 μmol/g), and ibuprofen (Qₑ, ₑₓₚ = 16.20–20.65 μmol/g) for the pristine SCW biochar showed linear correlations with their hydrophobicity (log D at pH 7.0: ibuprofen (1.71) > diclofenac (1.37) > naproxen (0.25)). However, their Qₑ, ₑₓₚ values for the NaOH-activated SCW biochar (naproxen (176.39–192.07 μmol/g) > diclofenac (78.44–98.74 μmol/g) > ibuprofen (61.25–80.02 μmol/g)) were inversely correlated to the order of their log D values. These results suggest that the reinforced aromatic structure of the NaOH-activated SCW biochar facilitated the π-π interaction. The calculated thermodynamic parameters demonstrated that the competitive adsorption of pharmaceuticals on the NaOH-activated SCW biochar compared to pristine SCW biochar occurred more spontaneously over the entire pH (5.0–11.0) and ionic strength (NaCl: 0–0.125 M) ranges. These observations imply that the NaOH-activated SCW biochar might be potentially applicable for the removal of pharmaceuticals in lake water and wastewater effluent.
Show more [+] Less [-]Efficient removal of Cd(II) from aqueous solution by pinecone biochar: Sorption performance and governing mechanisms
2020
Teng, Dongye | Zhang, Bingbing | Xu, Guomin | Wang, Bing | Mao, Gang | Wang, Jianxu | Sun, Jing | Feng, Xinbin | Yang, Zhugen | Zhang, Hua
Cadmium (Cd) is one of the most harmful and widespread environmental pollutants. Despite decades-long research efforts, the remediation of water contaminated by Cd has remained a significant challenge. A novel carbon material, pinecone biochar, was previously hypothesized to be a promising adsorbent for Cd, while so far, it has received little attention. This study evaluated the sorption capacity of pinecone biochar through isotherm experiments. Based on Langmuir model, the adsorption maximum for Cd(II) was up to 92.7 mg g⁻¹. The mechanism of Cd(II) adsorption on pinecone biochar was also explored through both thermodynamic and kinetics adsorption experiments, as well as both solution and solid-phase microstructure characterization. The solid-solution partitioning behaviour of Cd(II) fitted best with the Tόth model while the adsorption process followed a pseudo-second-order rate, suggesting that the Cd(II) adsorption on the pinecone biochar was mainly a chemisorption process. Microstructure characteristics and mechanism analysis further suggested that coprecipitation and surface complexation were the main mechanisms of Cd adsorption by biochar. Coprecipitation occurred mainly through the forms of Cd(OH)₂ and CdCO₃. Our results demonstrated that pinecone biochar was an efficient adsorbent which holds a huge potential for Cd(II) removal from aqueous solution.
Show more [+] Less [-]Experimental and theoretical insight into hydroxyl and sulfate radicals-mediated degradation of carbamazepine
2020
Xiao, Ruiyang | Ma, Junye | Luo, Zonghao | Zeng, Weizhi | Wei, Zongsu | Spinney, Richard | Hu, Wei‒Ping | Dionysiou, Dionysios D.
Carbamazepine (CBZ), a widely detected pharmaceutical in wastewaters, cannot currently be treated by conventional activated sludge technologies, as it is highly resistant to biodegradation. In this study, the degradation kinetics and reaction mechanisms of CBZ by hydroxyl radical (OH) and sulfate radical (▪)–based advanced oxidation processes (AOPs) were investigated with a combined experimental/theoretical approach. We first measured the UV absorption spectrum of CBZ and compared it to the theoretical spectrum. The agreement of two spectra reveals an extended π–conjugation system on CBZ molecular structure. The second–order rate constants of OH and ▪ with CBZ, measured by competition kinetics method, were (4.63 ± 0.01) × 10⁹ M⁻¹ s⁻¹ and (8.27 ± 0.01) × 10⁸ M⁻¹ s⁻¹, respectively at pH 3. The energetics of the initial steps of CBZ reaction with OH and ▪ were also calculated by density functional theory (DFT) at SMD/M05–2X/6–311++G**//M05–2X/6–31 + G**level. Our results reveal that radical addition is the dominant pathway for both OH and ▪. Further, compared to the positive ΔGR0 value for the single electron transfer (SET) reaction pathway between CBZ and OH, the ΔGR0 value for SET reaction between CBZ and ▪ is negative, showing that this reaction route is thermodynamically favorable. Our results demonstrated the remarkable advantages of AOPs for the removal of refractory organic contaminants during wastewater treatment processes. The elucidation of the pathways for the reaction of OH and ▪ with CBZ are beneficial to predict byproducts formation and assess associated ecotoxicity, providing an evaluation mean for the feasibility of AOPs application.
Show more [+] Less [-]Single and competitive sorption of sulfadiazine and chlortetracycline on loess soil from Northwest China☆
2020
Jiang, Yufeng | Zhang, Qian | Deng, Xueru | Nan, Zhijiang | Liang, Xinru | Wen, Hong | Huang, Kui | Wu, Yingqin
The fate of veterinary antibiotics (VAs) in soil environment is determined by the hydrophilic performance and solubility of VAs and the type of soil. In this study, sulfadiazine (SDZ) and chlortetracycline (CTC) were selected as target pollutants, and a batch sorption method was used to find out the single and sorption competitive behavior and mechanism of the target pollutants on loess soil. Kinetic studies showed the apparent sorption equilibrium was reached 0–6 h for CTC and 0–12 h for SDZ. The sorption kinetics of VAs on loess soil were fitted well with a pseudo-second order kinetic model. Sorption thermodynamic data indicated the isotherm sorption of both SDZ and CTC on loess soil was fitted well with Freundlich isothermal (R², 0.960–0.975) and linear models (R², 0.908–0.976). The sorption affinity of CTC (Kd, 290–1620 L/kg for CTC) was much greater than that of SDZ (Kd, 0.6–4.9 L/kg for SDZ). The results also suggest that SDZ may be easily mobilized or leached from loess soil at neutral and alkaline pH, while CTC may be easily mobilized or leached at neutral pH. The sorption of each single target pollutant on the outer layer complex decreased with increasing ionic strength. Higher initial concentrations resulted in greater sorption capacity of target pollutants on loess soil increased. The sorption capacities of CTC and SDZ in the mixed system were lower than the sorption capacity of each single system, showing a competitive sorption behavior of CTC and SDZ during the sorption process. Overall, CTC showed the highest sorption potential in loess soil, whereas SDZ showed a high leaching risk in loess soil. These findings contribute to understanding the fate of different VAs in loess in the natural environment.
Show more [+] Less [-]Phosphorus-rich biochar produced through bean-worm skin waste pyrolysis enhances the adsorption of aqueous lead
2020
Yan, Yubo | Sarkar, Binoy | Zhou, Lei | Zhang, Ling | Li, Qiao | Yang, Jianjun | Bolan, Nanthi
In China, more than 10,000 tons of bean-worm, which is rich in protein (68.5%) and essential amino acids (52.8%), is consumed annually. Thus, a large amount of bean-worm skin waste is generated, and is often indiscriminately disposed of, potentially causing environment problems. In this study, bean-worm skin (BWS) waste was pyrolyzed at 500 °C to produce biochar (BWS-BC), and the surface properties of BWS and BWS-BC were characterized using various spectroscopic techniques. Pb(II) adsorption properties of BWS and the corresponding biochar as a function of solution pH, contact time, and equilibrium concentration of Pb(II) were examined using adsorption isotherm, kinetics and thermodynamics studies. The maximum Pb(II) adsorption capacities based on the Langmuir isotherm model were calculated as 45 and 62 mg g⁻¹ for BWS and BWS-BC, respectively, which were comparable to the values obtained for biochars derived from other agro-wastes. The adsorption feasibility, favorability and spontaneity of Pb(II), as derived from the thermodynamic parameters, indicated that chemisorption and precipitation (e.g., hydroxypyromorphite) were the main adsorption mechanism in case of BWS and BWS-BC, respectively. Thus, conversion of BWS to biochar for Pb(II) adsorption can be considered as a feasible, promising and high value-added approach for BWS recycling.
Show more [+] Less [-]Co-combustion of anthracite coal and wood pellets: Thermodynamic analysis, combustion efficiency, pollutant emissions and ash slagging
2018
Guo, Feihong | Zhong, Zhaoping
This work presents studies on the co-combustion of anthracite coal and wood pellets in fluidized bed. Prior to the fluidized bed combustion, thermogravimetric analysis are performed to investigate the thermodynamic behavior of coal and wood pellets. The results show that the thermal decomposition of blends is divided into four stages. The co-firing of coal and wood pellets can promote the combustion reaction and reduce the emission of gaseous pollutants, such as SO₂ and NO. It is important to choose the proportion of wood pellets during co-combustion due to the low combustion efficiency caused by large pellets with poor fluidization. Wood pellets can inhibit the volatilization of trace elements, especially for Cr, Ni and V. In addition, the slagging ratio of wood pellets ash is reduced by co-firing with coal. The research on combustion of coal and wood pellets is of great significance in engineering.
Show more [+] Less [-]Rapidly probing the interaction between sulfamethazine antibiotics and fulvic acids
2018
Xu, Juan | Hu, Yan-Yun | Li, Xiu-Yan | Chen, Jie-Jie | Sheng, Guo-Ping
Antibiotics residuals in the environments receive wide concerns due to the high risk of generating antibiotic resistance. Natural organic matters (NOM) existed in the environments are considered to have the capacity of binding with organic contaminants, consequently influencing their speciation and transformation in the natural environments. To assess the migration of antibiotics in the environments, it is crucial to understand the binding mechanisms between NOM and antibiotics, which is still unclear due to the limit of available research methods. In this study, the interaction between fulvic acids (FA), one of the main components of NOM, and sulfamethazine (SMZ) was characterized by nuclear magnetic resonance (NMR) combined with surface plasmon resonance (SPR) and isothermal titration calorimetry (ITC) technology. The parameters related to kinetics and thermodynamics of the interaction were determined, and the possible mechanisms driving the interaction were also proposed. In addition, density functional theory (DFT) was used to predict the binding mode between FA and SMZ to reveal the interaction mechanism. Results indicate that FA can effectively bound with SMZ to form a stable complex with a binding constant at the level of 10³ L/mol. The kinetic parameters including association and dissociation constants were 29.4 L/mol/s and 6.64 × 10⁻³ 1/s, respectively. Hydrophobic interaction might play significant roles in the binding interaction with ancillary contribution of π-π conjunction arising from the aromatic rings stacking of FA and SMZ.
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