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Opposite impact of DOM on ROS generation and photoaging of aromatic and aliphatic nano- and micro-plastic particles
2022
Cao, Runzi | Liu, Xinna | Duan, Jiajun | Gao, Bowen | He, Xiaosong | Nanthi Bolan, | Li, Yang
Dissolved organic matter (DOM) plays a significant role in the photochemical behavior of nano- and micro-plastic particles (NPs/MPs). We investigated the influence of DOM on the mechanism on the photoaging of NPs/MPs with different molecular structures under UV₃₆₅ irradiation in water. DOM components used in this study are mainly humic acid and fulvic acid. The results showed that DOM promoted the weathering of aliphatic NPs/MPs (polypropylene (PP)), but inhibited or had only a minor effect on the photoaging of aromatic NPs/MPs (polystyrene (PS) NPs/MPs, carboxyl-modified PS NPs, amino-modified PS NPs, and polycarbonate MPs). NPs with a large surface area may adsorb sufficient DOM on the particle surfaces through π-π interactions, which competes with NPs for photon absorption sites, thus, can delay the photoaging of PS NPs. Aromatic MPs may release phenolic compounds that quench •OH, thereby weakening the photoaging process. For aliphatic MPs, the detection of peracid, aldehyde, and ketone groups on the polymer surface indicated that DOM promoted weathering of PP MPs, which was primarily because the generation of •OH due to DOM photolysis may attack the polymer by C–C bond cleavage and hydrogen extraction reactions. This study provides insight into the UV irradiation weathering process of NPs/MPs of various compositions and structures, which are globally distributed in water.
Afficher plus [+] Moins [-]Effects of composite environmental materials on the passivation and biochemical effectiveness of Pb and Cd in soil: Analyses at the ex-planta of the Pak-choi root and leave
2022
Wang, An | Wang, Yao | Zhao, Peng | Huang, Zhanbin
Passivation of soil heavy metals using environmental materials is an important method or important in situ remediation measure. There are more studies on inorganic environmental materials for heavy metal passivation, but not enough studies on organic and their composite environmental materials with inorganic ones. In order to reveal the passivation effect of coal-based ammoniated humic acid (CAHA), biochemical humic acid (BHA), biochar (BC) and other organic types and inorganic environmental materials such as zeolites (ZL) on soil heavy metals and their biological effectiveness. The microstructures of these materials were analyzed by Scanning electron microscope (SEM). The main components of the environmental materials were analyzed by Energy dispersive spectrometer (EDS), Fourier transforms infrared spectroscopy (FT-IR) and X-ray diffraction spectrum (XRD) to elucidate the mechanism of passivation of heavy metals in soil by these environmental materials. The study was conducted to investigate the effects of different types of environmental materials and their combinations on the passivation effect and biological effectiveness of Pb and Cd complex contamination in soil by means of soil incubation and pot experiments using single-factor and multifactor multilevel orthogonal experimental designs. Soil incubation experiments proved that the effective state of soil Pb and Cd in T₇ was reduced by 13.40% and 11.07%, respectively. The extreme difference analysis determined the optimized formulation of soil lead and cadmium passivation as BHA: CAHA: BC: ZL = 3.5:5:20:10. The pot experiment proved that the application of composite environmental materials led to the reduction of lead and cadmium content and increase of biomass of Pak-choi, and the optimal dosage of optimized composite environmental materials was 23.1 g/kg.
Afficher plus [+] Moins [-]Insights into phenol monomers in response to electron transfer capacity of humic acid during corn straw composting process
2022
Zhao, Xinyu | Zhang, Chuanyan | Dang, Qiuling | Xi, Beidou
Quinone is the important redox functional group for electron transfer capacity (ETC) of humic acid (HA). Lignin, as major component in corn straw, can be decomposed into phenol monomers, then oxidation into quinones for synthesis of HA during composting process. However, it is still unclear that the effects of type and variation characteristics of phenol monomers on redox characteristics of HA during straw composting process. In this study, p-hydroxybenzoic acid (P1), vanillic acid (P2), syringic acid (P3), p-hydroxy benzaldehyde (P4), 4-coumaric acid (P5), 4-hydroxyacetophenone (P6), ferulic acid (P7) and 4-hydroxy-3-methylacetophenone (P8) were recognized and clustered into three groups. The concentration of polyphenol presented a significant downward trend during the straw composting process. Based on the relationships among phenol monomers to ETC, electron donating capacity (EDC), electron accepting capacity (EAC) and quinone, we found that P1, P2, P3, P5 and P7 were significantly related to ETC, EDC and EAC of HA (P < 0.05). Furthermore, NH₄⁺-N and NO₃⁻-N were the main micro-environmental factors linking to ETC-related phenol monomers and redox characteristics of HA in straw composts (P < 0.05). Finally, two groups of core microflora that promoting the ETC-related phenol monomers and NH₄⁺-N, and ETC-related phenol monomers and NO₃⁻-N were identified by Mantel test, respectively. This study contributes a new insight for polyphenol way for redox capacity of HA in traditional composting and utilization of straw compost in contaminated environments.
Afficher plus [+] Moins [-]Exposure to nanoplastic induces cell damage and nitrogen inhibition of activated sludge: Evidence from bacterial individuals and groups
2022
Tang, Sijing | Qian, Jin | Wang, Peifang | Lu, Bianhe | He, Yuxuan | Yi, Ziyang | Zhang, Yuhang
Wastewater treatment plants (WWTPs) are almost the only place where plastic fragments are artificially removed, resulting in mass accumulation of nanoplastics (NPs). In this research, four different concentrations (0 mg/L, 0.1 mg/L, 1 mg/L, 10 mg/L) of polystyrene nanoplastics (PS-NPs) were used to investigate the cell damage and nitrogen inhibition of activated sludge, exposed in a self-assembled SBR reactor for 30 days. Intracellular reactive oxides (ROS) and extracellular lactate dehydrogenase (LDH) increased with the rise of exposure concentration, and morphological analysis disclosed the creases, collapse, and even rupture of cell membranes. However, exposure damage (PS-NPs ≤ 1 mg/L) appeared to be reversible, attributed to that extracellular polymeric substances (EPS) secretion can thicken the three protective layers outside the membrane. PS-NPs did not disrupt the EPS chemical structure, but increased humic acid content. Prolonged exposure time (from 15 to 30 days) was directly related to the nitrogen inhibition. Due to the habitat changes under PS-NPs exposure, abundance and diversity of microorganisms in the original activated sludge decreased significantly, and the dominant phylum was occupied by Patescibacteria (PS-NPs = 10 mg/L). Changes in enzyme activities of AMO, NR, NIR, and NOR with exposure concentration may explain the conversion of nitrogen in SBR. This research broadens our horizons to understand the response mechanism of activated sludge bacteria to PS-NPs exposure individually and collectively.
Afficher plus [+] Moins [-]Nanoanalysis of the leaching process simulation of Pb in agricultural soil
2022
Liu, Shuyu | Min, Xin | Xiang, Minghui | Wang, Jiangli | Tang, Lei | Liu, Li
Using the Spectral characteristics of gold nanorods to investigate heavy metals Pb in agricultural soils. Studied included: (1) The effects of humic acid on Pb transformation and its formation changing were explored. The laboratory model was established to simulate Pb leaching process in the soil and investigated the change of total Pb content at different layers. (2) The migration and transformation of different forms Pb were studied by the nano system. The effect of humic acid and pH were analyzed based on the nano-analysis method. (3) The relationship between various forms Pb irons were analyzed. (4) The data showed that ion exchange state and iron-manganese oxidation state Pb were more likely to enriched at 0 cm depth, and organic bound state was more likely to enriched at 10 cm depth. Humic acid increased the solidify ability of different forms of Pb in agricultural soil, and the analysis system was efficient to supply the exactly transition process.
Afficher plus [+] Moins [-]Transport and retention of microplastics in saturated porous media with peanut shell biochar (PSB) and MgO-PSB amendment: Co-effects of cations and humic acid
2022
Wang, Xiaoxia | Dan, Yitong | Diao, Yinzhu | Liu, Feihong | Wang, Huan | Sang, Wenjing
Biochar particles are extensively used in soil remediation and interact with microplastics (MPs), especially metal oxide-modified biochar may have stronger interactions with MPs. The mechanism of interactions between humic acid (HA) and different valence cations is different and the co-effect on the transport of MPs is not clear. In this study, the co-effects of HA and cations (Na⁺, Ca²⁺) on the transport and retention of MPs in saturated porous media with peanut shell biochar (PSB) and MgO-modified PSB (MgO-PSB) were systematically investigated. Breakthrough curves (BTCs) of MPs were fitted by the two-site kinetic retention model for analysis. In the absence of HA, the addition of PSB and MgO-PSB significantly hindered the transport of MPs in saturated porous media, and the retention of MPs increased from 34.2% to 59.1% and 75.5%, respectively. In Na⁺ solutions, the HA concentration played a dominant role in controlling MPs transport, compared to the minor role of Na⁺. The transport capacity of MPs always increased gradually with the increase of HA concentration. Whereas, in Ca²⁺ solutions, Ca²⁺ concentrations had a stronger effect than HA. The transport ability of MPs was instead greater than that in Na⁺ solutions as the HA concentration increased at low ionic strength (1 mM). However, the transport capacity of MPs was significantly reduced with increasing HA concentrations at higher ionic strength (10, 100 mM). The two-site kinetic retention model indicated that chemical attachment and physical straining are the main mechanisms of MPs retention in the saturated porous media.
Afficher plus [+] Moins [-]Biochar composite derived from cellulase hydrolysis apple branch for quinolone antibiotics enhanced removal: Precursor pyrolysis performance, functional group introduction and adsorption mechanisms
2022
Zou, Mengyuan | Tian, Weijun | Chu, Meile | Gao, Huizi | Zhang, Dantong
In this study, magnetic biochar (MAB) and humic acid (HA)-coated magnetic biochar produced from apple branches without and after cellulase hydrolysis (HMAB and CHMAB, respectively) were prepared and tested as adsorbents of enrofloxacin (ENR) and moxifloxacin (MFX) in aqueous solution. Compared with MAB and HMAB, novel adsorbent CHMAB possessed a superior mesoporous structure, greater graphitization degree and abundant functional groups. When antibiotic solutions ranged from 2 to 20 mg L⁻¹, the theoretical maximum adsorption capacities of CHMAB for ENR and MFX were 48.3 and 61.5 mg g⁻¹ at 35 °C with adsorbent dosage of 0.4 g L⁻¹, respectively, while those of MAB and HMAB were 39.6 and 54.4 mg g⁻¹, and 44.7 and 59.0 mg g⁻¹, respectively. The pseudo-second-order kinetic model and Langmuir model presented a better fitting to the spontaneous and endothermic adsorption process. The maximum adsorption capacity of ENR and MFX onto CHMAB was achieved at initial pH values of 5 and 8, respectively. Additionally, the adsorption capacity of ENR and MFX decreased with increasing concentrations of K⁺ and Ca²⁺ (0.02–0.1 mol L⁻¹). Synergism between the pore-filling effect, π-π electron-donor-acceptor interactions, regular and negative charge-assisted H-bonding, surface complexation, electrostatic interactions and hydrophobic interactions may dominate the adsorption process. This study demonstrated that a novel magnetic biochar composite prepared through pyrolysis of agricultural waste lignocellulose hydrolyzed by cellulase in combination with HA coating was a promising adsorbent for eliminating quinolone antibiotics from aqueous media.
Afficher plus [+] Moins [-]Enhanced propagation of intracellular and extracellular antibiotic resistance genes in municipal wastewater by microplastics
2022
Cheng, Yuan | Lu, Jiarui | Fu, Shusen | Wang, Shangjie | Senehi, Naomi | Yuan, Qingbin
Microplastics (MPs) are an emerging global concern as they are abundant in the environment and can act as vectors of various contaminants. However, whether and how MPs can be vectors of antibiotic resistance genes (ARGs), especially extracellular ARGs (eARGs), remains far from explicit. This study addresses the adsorption of both intracellular ARGs (iARGs) and eARGs by four types of MPs in municipal wastewater, and then explores the potential horizontal gene transfer of iARGs and eARGs exposed to MPs. Results indicate that though MPs significantly adsorbed both iARGs and eARGs, eARGs were adsorbed with a significantly higher fold enrichment (2.0–5.0 log versus 2.0–3.3 log) and rate (0.0056 min⁻¹ versus 0.0037 min⁻¹) than iARGs. While all four types of MPs adsorbed ARGs, polypropylene MPs showed the highest adsorption capacity for ARGs. Background constituents such as humic acid and antibiotics significantly inhibited adsorption of iARGs, but not eARGs on MPs. The presence of sodium chloride didn't significantly affect adsorption of iARGs or eARGs. The adsorption of ARGs was well explained by the extended Derjaguin–Landau–Verwey–Overbeek (XDLVO) interaction energy profile. Higher eARG adsorption was attributed to a lower energy barrier between MPs and eARGs than that between MPs and iARGs. Exposure to MPs enhanced horizontal gene transfer of both iARGs and eARGs by 1.5 and 2.0 times, respectively. The improved contact potential between donors and recipients, as well as the increased cell permeability of recipients induced the improved horizontal gene transfer by MPs. This study underscores the need to address ARG propagation through adsorption to MPs.
Afficher plus [+] Moins [-]Hexachloroethane dechlorination in sulfide-containing aqueous solutions catalyzed by nitrogen-doped carbon materials
2021
Liu, Na | Hu, Qing | Wang, Chao | Tong, Lizhi | Weng, Chih-Huang | Ding, Longzhen
This study demonstrated that nitrogen-doped carbon materials (NCMs) could effectively catalyze the chlorine elimination process in hexachloroethane (HCA) declorination in sulfide-containing environments for the first time. The kₒbₛ values of HCA dechlorination by sulfide in the presence of 10 mg/L NCMs were higher than that of no mediator at pH 7.3 by one or two orders of magnitude. The catalytic capabilities of NCMs on HCA dechlorination were evident in common ranges of natural pH (5.3–8.9) and it could be accelerated by the increase of pH but be suppressed by the presence of dissolved humic acid. Moreover, NCMs exhibited much better catalytic capability on HCA dechlorination compared to the carbon materials, mainly owing to the combined contributions of pyridine N, including enhanced nucleophilic attack to HCA molecule by generating newborn C–S–S and activation of HCA molecule by elongating C–Cl bonds. The functions of pyridine N in micron-sized NCMs with mesopores were better than in nano-sized NCMs on HCA dechlorination. These findings displayed the potential of NCMs, when released into sulfide-containing environments, may significantly increase the dechlorination of chlorinated aliphatic hydrocarbons.
Afficher plus [+] Moins [-]Water-induced release of recalcitrant polycyclic aromatic hydrocarbons from soil organic matter during microwave-assisted solvent extraction
2021
Wang, Wei | Zhang, Yanyan | Du, Wei | Tao, Shu
Polycyclic aromatic hydrocarbons (PAHs) in soil can be recalcitrant to solvent extraction after aging. We showed in this study that mixing a small amount of water in the extracting solvent during microwave-assisted extraction (MAE) can release recalcitrant PAHs, resulting in significant improvement in the analyzed concentrations. The improvement factor (F) for the total of 16 priority PAHs (∑PAH16) listed by the United States Environmental Protection Agency was 1.44–1.55 for field soils. By comparing the F values for different soil organic components, we demonstrated that the recalcitrant PAHs were primarily associated with biochar, humic acid (HA), and humin (HM), with the F values for ∑PAH16 of 1.94, 6.62, and 4.59, respectively. The results showed that the recalcitrant PAHs comprised a sequestered fraction and a desorption-limited fraction. NMR spectra showed that water worked alone at elevated temperature to promote hydrolysis of biochar and destroy the macromolecular structure, thus causing the release of the otherwise sequestered PAHs during MAE. The substantial reduction in F values for HA and HM after demineralization indicated sequestration of PAHs in organic-mineral complexes, which can be destroyed by hot water treatment. The release of the sequestered fraction was nonselective and independent of compound hydrophobicity. In comparison, the release of the desorption-limited fraction was positively affected by the hydrophobicity of PAHs and was facilitated by the presence of water in the extracting solvent. The results of this study provide important insights into the sequestration and release of recalcitrant PAHs in soil.
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