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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.
Show more [+] Less [-]Multi-spectroscopic investigation of the molecular weight distribution and copper binding ability of dissolved organic matter in Dongping Lake, China
2022
Fan, Tuantuan | Yao, Xin | Ren, Haoyu | Ma, Feiyang | Liu, Li | Huo, Xiaojia | Lin, Tong | Zhu, Haiyan | Zhang, Yinghao
The properties and metal-binding abilities of dissolved organic matter (DOM) rely on its molecular weight (MW) structure. In this study, the spatial differences of DOM in compositions, MW structures, and binding mechanisms with copper (Cu²⁺) in Dongping Lake were investigated by applying excitation-emission matrix combining parallel factor analysis (EEM-PARAFAC), synchronous fluorescence (SF) spectra, two-dimensional correlation spectra (2D-COS), and Fourier transform infrared (FTIR) spectra. The EDOM for the entrance of the Dawen River and PDOM for the macrophyte-dominated region were divided from DOM of Dongping Lake based on hierarchical clustering analysis (HCA) and principal component analysis (PCA) and were size-fractioned into MW < 500 kDa and <100 kDa fractions. According to EEM-PARAFAC, Dongping Lake was dominated by tryptophan-like substances with MW < 500 kDa. The concentration of PDOM was higher than that of EDOM (p < 0.05). 2D-COS showed that protein-like components preceded humic-like components binding to Cu²⁺ regardless of sample type (215 nm > 285 nm > 310–360 nm). The Cu²⁺ binding capacity of DOM exhibited specific differences in space, components, and molecular weights. The humic-like component 1 (C1) and tryptophan-like component 4 (C4) of PDOM showed stronger binding abilities than those of EDOM. Endogenous tryptophan-like component 4 (C4) had a higher binding affinity for Cu²⁺ than humic-like components (logKₐ: C4 > C1 > C2) in PDOM irrespective of MW. Humic-like components with MW < 500 kDa displayed higher binding potentials for Cu²⁺. FTIR spectra showed that the main participants of DOM-Cu complexation included aromatic hydrocarbons, aliphatic groups, amide Ⅰ bands, and carboxyl functional groups. This study provides spatial-scale insights into the molecular weight structure of DOM in influencing the behavior, fate, and bioavailability of heavy metals in lakes.
Show more [+] Less [-]Inhibition of methylmercury uptake by freshwater phytoplankton in presence of algae-derived organic matter
2022
Li, Zhike | Chi, Jie | Shao, Bo | Wu, Zhengyu | He, Wei | Liu, Yiwen | Sun, Peizhe | Lin, Huiming | Wang, Xuejun | Zhao, Yingxin | Chen, Long | Tong, Yindong
As the first step of methylmercury (MeHg) entry into the aquatic food webs, MeHg uptake by phytoplankton is crucial in determining the final human MeHg exposure risks. MeHg availability to plankton is regulated by dissolved organic matter (DOM) in the water, while the extent of the impacts can vary largely based on the sources of DOM. Here, we investigated impacts of DOM sources on MeHg bioconcentration by three freshwater phytoplankton species (i.e. S. quadricauda, Chlorella sp., Microcystis elabens) in the laboratory system. We found that algae-derived DOM would prohibited the cellular MeHg bioconcentration by a percent up to 77–93%, while the soil-derived DOM didn't show similar inhibition effects. DOM characterization by the excitation‒emission matrices, Fourier transform infrared spectrum, ultra‒high performance liquid chromatography‒tandem quadrupole time of flight mass spectrometry shown that the molecular size of S-containing compound, rather than thiol concentration, has played a crucial role in regulating the MeHg uptake by phytoplankton. Climate change and increasing nutrient loadings from human activities may affect plankton growth in the freshwater, ultimately changing the DOM compositions. Impacts of these changes on cellular MeHg uptakes by phytoplankton should be emphasized when exploring the aquatic Hg cycling and evaluating their risks to human beings and wild life.
Show more [+] Less [-]Correlative distribution of DOM and heavy metals in the soils of the Zhangxi watershed in Ningbo city, East of China
2022
Wang, Zhe | Han, Ruixia | Muhammad, Azeem | Guan, Dong-Xing | Zama, Eric | Li, Gang
In peri-urban critical zones, soil ecosystems are highly affected by increasing urbanization, causing probably an intense interaction between dissolved organic matter (DOM) and heavy metals in soil. Such interaction is critical for understanding the biogeochemical cycles of both organic matter and heavy metals in these zones. However, limited research has reported the correlative distribution of DOM and heavy metals at high seasonal and spatial resolutions in peri-urban critical zones. In this study, 160 soil samples were collected from the farmland and forestland of Zhangxi watershed, in Ningbo, eastern China during spring, summer, fall and winter four seasons. UV–visible absorption and fluorescent spectroscopy were used to explore the optical characteristics of DOM. The results indicated a mixture of exogenous and autogenous sources of DOM in the Zhangxi watershed, while DOM in farmland exhibited a higher degree of aromaticity and humification than that in forestland. Fluorescent results showed that humic acid-like, fulvic acid-like and microbial-derived humic-like fractions were mostly affected by seasons. The distribution of heavy metals was affected mainly by land-use changes and seasons. Correlation analysis between heavy metals and DOM characteristics and components suggested that aromatic and humic substances were more favorable in binding with EDTA extractable Ni, Cu, Zn and Cd. The bioavailable Cd and Pb decreased due to binding with humic fractions, indicating its great effects on the bioavailability of Cd and Pb. Overall, these findings provide an insight into the correlative distributions of DOM and heavy metals in peri-urban areas, thereby highlighting their biogeochemical cycling in the soil environment.
Show more [+] Less [-]Effect of fulvic acid concentration levels on the cleavage of piperazinyl and defluorination of ciprofloxacin photodegradation in ice
2022
Li, Zhuojuan | Dong, Deming | Zhang, Liwen | Li, Yanchun | Guo, Zhiyong
Ice is an important physical and chemical sink for various pollutants in cold regions. The photodegradation of emerging fluoroquinolone (FQ) antibiotic contaminants with dissolved organic matter (DOM) in ice remains poorly understood. Here, the photodegradation of ciprofloxacin (CIP) and fulvic acid (FA) in different proportions as representative FQ and DOM in ice were investigated. Results suggested that the photodegradation rate constant of CIP in ice was 1.9 times higher than that in water. When CFA/CCIP ≤ 60, promotion was caused by FA sensitization. FA increased the formation rate of cleavage in the piperazine ring and defluorination products. When 60 < CFA/CCIP < 650, the effect of FA on CIP changed from promoting to inhibiting. When 650 ≤ CFA/CCIP ≤ 2600, inhibition was caused by both quenching effects of 143.9%–51.3% and light screening effects of 0%–48.7%. FA inhibited cleavage in the piperazine ring for CIP by the scavenging reaction intermediate of aniline radical cation in ice. When CFA/CCIP > 2600, the light screening effect was greater than the quenching effect. This work provides new insights into how DOM affects the FQ photodegradation with different concentration proportions, which is beneficial for understanding the environmental behaviors of fluorinated pharmaceuticals in cold regions.
Show more [+] Less [-]Insights into variations on dissolved organic matter of bauxite residue during soil-formation processes following 2-year column simulation
2022
Xue, Shengguo | Liu, Zheng | Fan, Jiarong | Xue, Rui | Guo, Ying | Chen, Wei | Hartley, William | Zhu, Feng
Bauxite residue, an industrial alkaline solid waste, has a low organic carbon content which hinders plant growth. Dissolved organic matter (DOM) drives many biogeochemical processes including carbon storage and soil formation in soils. Input of exogenous organic materials may provide organic carbon and accelerate soil formation processes in bauxite residue. However, the potential effects of ameliorants on the quantity and quality of DOM in bauxite residue are still poorly understood. Here, the integration of ultraviolet–visible (UV–Vis) spectra, fluorescence spectra, and parallel factor (PARAFAC) analysis were used to investigate the vertical characteristics of DOM in bauxite residue treated by PV (the combined addition of 2% phosphogypsum and 4% vermicompost, w/w) and BS (6% w/w including 4% bagasse and 2% bran) with 2-year column experiments. The content of DOM in untreated residues ranged from 0.064 to 0.096 g/kg, whilst higher contents of DOM were observed in PV (0.13 g/kg) and BS (0.26 g/kg) treatment. Meanwhile, with the increase of residue depth, the aromaticity and hydrophobic components of DOM in residue decreased, which indicated that the degree of humification of the treated residues in the upper layer was higher than that in the lower layer. Compared with BR, BS and PV treatment accumulated the related content of fulvic acid-like substance from 36.14% to 71.33% and 74.86%, respectively. The incorporation of vermicompost and biosolids increased the content of humic-like substances, whilst decreasing the content of protein-like substances in the surface layer, which may be due to the enrichment of the microbial community. During soil formation processes, the application of organic amendments reduced both salinity and alkalinity, enhanced microbial community diversity, and changed the quantity and quality of DOM in bauxite residue. These findings improve our understanding of the dynamics of DOM and response of DOM to soil formation processes in bauxite residue.
Show more [+] Less [-]Properties of sediment dissolved organic matter respond to eutrophication and interact with bacterial communities in a plateau lake
2022
Li, Shuaidong | Fang, Jie | Zhu, Xinshu | Spencer, Robert G.M. | Álvarez -Salgado, Xosé Antón | Deng, Yongcui | Huang, Tao | Yang, Hao | Huang, Changchun
Sediment dissolved organic matter (DOM) in inland waters is commonly affected by environmental changes. However, knowledge about how sediment DOM responds to eutrophication and the associations between sediment DOM and bacterial communities requires further investigation. We selected a sediment core from Dianchi Lake (China) that was dated from 1864 to 2019 by the activity of radionuclides (²¹⁰Pb and ¹³⁷Cs). δ¹³CDOC changes fit well with the historical record that heavy eutrophic status in Dianchi Lake were observed since 1980s. Large amounts of dissolved organic carbon (DOC), chromophoric (CDOM) and fluorescent (FDOM) DOM accumulated at the top of the sediments during the eutrophication period (1982-present). The additional algae sources with a higher degradation rate altered the composition, aromaticity and humification of DOM. After long-term mineralization, the remaining DOM became more and more recalcitrant and kept a relatively stable level at older sediments. A co-occurrence network analysis revealed that Proteobacteria, Chloroflexi, Acidobacteriota, Bacteroidota and Desulfobacterota were the most abundant species at the phylum level and clustered into three primary modules. Different microbes shared unique preferences for niches, causing a heterogeneous bacterial distribution at different depths. We conducted Spearman's correlation and redundancy analysis (RDA) to explore potential interactions between bacterial community and sediment DOM. The richness and diversity of bacterial communities were positively related to DOM content, suggesting abundant DOM can produce more available resources for bacteria. RDA results showed some specific species might modify DOM composition and structure. This study suggests that sediment DOM properties were regulated by source transformation during eutrophication, and emphasizes the importance of microbial role on sediment biogeochemical process.
Show more [+] Less [-]Characteristics of oxytetracycline stress-sensitive microbe-dissolved organic matter component interactions during composting
2022
Zhang, Xu | Zhang, Xinlin | Cui, Hongyang | Zhao, Ran | Zhao, Meiyang | Wei, Zimin
Dissolved organic matter (DOM) has important impacts on the transportation of antibiotics through chemical and biological processes in composting. The interaction between DOM and antibiotics is reciprocal. The interaction between DOM ligands and antibiotics could be characterized based on a technique combining parallel factor analysis (PARAFAC) and microbial community structure analysis. However, PARAFAC cannot reveal the dynamic changes in each DOM peak in one PARAFAC component under antibiotic stress. In this study, two-dimensional correlation spectroscopy (2DCOS) combined with PARAFAC and bacterial community diversity analyses were employed to reveal the effects of oxytetracycline (OTC) stress and the key microorganisms on the transformation of different fluorescent peaks from DOM PARAFAC components during chicken manure composting. The results showed that OTC inhibits the transformation between DOM PARAFAC components by inhibiting the core microbial activities involved in the transformation of DOM components. Protein-like components (C1 and C2) were more sensitive to OTC residue, and components with a high humification degree promoted the degradation of OTC. The interaction between special DOM PARAFAC components and certain bacteria affects the degradation of OTC. The DOM PARAFAC components A2(C1), B1(C2), B2(C2) and Z1(C4) enhanced OTC degradation by stimulating the genera Pseudomonas, Glycomyces and Hyphomicrobium. With these promising results, the true effect of DOM PARAFAC components on the degradation of OTC can be revealed, which is helpful for addressing antibiotic contamination to improve the bioavailability of compost products.
Show more [+] Less [-]Microbial metabolism changes molecular compositions of riverine dissolved organic matter as regulated by temperature
2022
Tang, Gang | Zheng, Xing | Hu, Shiwen | Li, Binrui | Chen, Shuling | Liu, Tong | Zhang, Bowei | Liu, Chongxuan
This study investigated the control of dissolved organic matter (DOM) molecular compositions by microbial community shifts under temperature regulation (range from 5 to 35 °C), using riverine DOM and in situ microorganisms as examples. The functioning of different microbial metabolisms, including the utilization and generation processes, was comprehensively analyzed. Though the overall quantity of DOM was less temperature-affected, more molecules were identified at moderate temperatures (e.g., 15 and 25 °C) and their accumulated mass peak intensities increased with the temperature. The results were ascribed to 1) the microbial production of macromolecular (m/z > 600) CHO, CHON, and CHONS species was stimulated at higher temperatures; 2) the microorganisms consumed more DOM molecules at both higher and lower temperatures; and 3) the simultaneously decreased utilization and increased generation of recalcitrant CHO and CHON molecules with m/z < 600 at higher temperatures. The strong correlations among the temperature, community structures, and DOM chemodiversity suggested that temperature promoted the community evenness to increase the DOM generation. In addition, the higher temperature decreased the abundance of microorganisms that utilized more recalcitrant molecules and produced fewer new molecules (e.g., Proteobacteria, Acinetobacter, and Erythrobacter) while increased others that functioned the opposite (e.g., Verrucomicrobia, Bacteroidetes, and Flavobacterium) to increase the DOM production. The constructed temperature-community-DOM chemistry relationship deepened the molecular-level understanding of DOM variations and provided implications for the warming future.
Show more [+] Less [-]Activation of peroxydisulfate by ball-milled α-FeOOH/biochar composite for phenol removal: Component contribution and internal mechanisms
2022
Zhao, Ling | Zhang, Hui | Zhao, Beibei | Lyu, Honghong
Persulfate-based advanced oxidation process is considered as a promising technology for the degradation of phenol, where efficient, cost effective, and green methods with high peroxydisulfate (PS) activation capacity is of increasing demand. In this work, an in-situ liquid phase precipitation combined with ball milling method was applied for the synthesized of α-FeOOH/biochar, as be the PS activator for phenol degradation. Results showed that the ball-milled α-FeOOH and red pine wood biochar prepared at 700 °C (BM-α-FeOOH/PBC700) exhibited the highest catalytic property with PS for phenol oxidation (a phenol removal rate of 100%), compared with the BM-α-FeOOH (16.0%) and BMPBC700 (66.3%). The presence of intermediate products such as hydroquinone and catechol, and total organic carbon (TOC) removal rate (88.9%) proved the oxidation of phenol in the BM-α-FeOOH/PBC700+PS system. The characterization results showed that the functional groups (e.g., CO, C–O, Fe–O, and Si–O), the dissolved organic matter (DOM) in biochar, the loading of Fe element, and higher degree of graphitization and defect structures, contributed to the activation of PS to form free radicals (i.e., SO₄·⁻, ·OH, ·O₂⁻, and hVB⁺) for phenol oxidation, of which, SO₄·⁻ and ·OH account for 72.1% of the phenol removal rate. The specific contribution to the PS activation for phenol oxidation by each part of the materials was calculated based on the “whole to part” experiment. The contribution of DOM, acid-soluble substance, and carbon matrix and basal part in BM-α-FeOOH/PBC700 were 6.0%, 40.9%, and 53.1%, respectively. The reusability experiments of BM-α-FeOOH/PBC700 demonstrated that the composite was relatively stable after four cycles of reuse. Among three co-existing anions (NO₃⁻, Cl⁻, and HCO₃⁻), HCO₃⁻ played the most significant inhibition effects on phenol removal through reducing the phenol removal rate from 89.6% to 77.9%. This work provides guidance for the design of high active and stable carbon materials that activate PS to remove phenol.
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