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EEM-PARAFAC
SCIENCE OF THE TOTAL ENVIRONMENT · 2019 · IF 5.589

Limited Cu(II) binding to biochar DOM: Evidence from C K-edge NEXAFS and EEM-PARAFAC combined with two-dimensional correlation analysis

Jing Wei,Chen Tu,Guodong Yuan,Yongqiang Zhou,Hailong Wang,Jian Lu

Multiple spectroscopic technologies and chemometric analyses were combined to explore the compositional characteristics and Cu binding performance of biochar-derived dissolved organic matter (DOM). The DOM samples were extracted from biochars produced from lignocellulose-rich rapeseed cake (RSC) by pyrolysis at 300, 500, and 700 °C (i.e., RSC300, RSC500, RSC700). Fourier transform infrared spectroscopy (FTIR) and carbon K-edge near-edge X-ray absorption fine structure spectroscopy (NEXAFS) analyses were combined to elucidate the molecular-level C species in the DOM. With the increasing pyrolysis temperature, DOM aromaticity increased, whereas the proportion of metal complexing sites (e.g., carboxyl and phenolic groups) decreased. Fluorescence excitation-emission matrix (EEM) spectroscopy with parallel factor analysis (PARAFAC) indicated that biochar DOM, irrespective of pyrolysis temperature, was mostly composed of three types of humic-like components (C1–C3), and a small amount of a protein-like component (C4). As charring temperature increased, DOM concentrations decreased substantially, but the humic-like C3 with abundant aromatic structures became predominant. Fluorescence quenching experiment and two-dimensional correlation spectroscopy (2D-COS) analysis suggested that the preferential Cu(II) binding fractions of the DOM were the humic-like substances. Moreover, the quenching curve fitting results for individual components indicated that despite the Cu(II) binding affinity was slightly enhanced as the pyrolysis temperature increased, the binding capacities of the four components decreased. In general, the DOM components from RSC biochar exhibited limited Cu(II) binding capacities (2.18–17.7 μmol L −1 ). Results from this study improved understanding of the mechanisms by which biochar DOM interacts with Cu, and provided tools for fast screening of biochars to reduce their environmental risks.

研究领域: 环境科学 · 土壤化学
✓ 已验证 DOI PubMed 高影响因子
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SCIENCE OF THE TOTAL ENVIRONMENT · 2019 · IF 5.589

A comparison of dissolved organic matter transformation in low pressure ultraviolet (LPUV) and ultraviolet light-emitting diode (UV-LED)/chlorine processes

Ze-Chen Gao,Yi-Li Lin,Bin Xu,Ying Xia,Chen-Yan Hu,Tian-Yang Zhang,Tong-Cheng Cao,Yang Pan,Nai-Yun Gao

This study compared the degradation of dissolved organic matter (DOM) by UV/chlorine advanced oxidation processes (AOPs) with emerging ultraviolet light-emitting diode (UV-LED, 275 nm) and traditional low pressure UV (LPUV, 254 nm) as UV sources. Excitation emission matrix-parallel factor (EEM-PARAFAC) analysis and two-dimensional (2D) correlation gel permeation chromatograph were applied to explore the evolutions of DOM during oxidation processes. The degradation behaviors of DOM indicated by UV absorbance at 254 nm (UV 254 ), dissolved organic carbon (DOC), and fluorophores fitted the pseudo-first-order kinetics well. The removal efficiency of DOM was similar under UV-LED and LPUV irradiation alone. However, UV-LED exhibited much higher degradation rates (increased by 29–160%) than LPUV regardless of the tracking variables during UV/chlorine processes. For three PARAFAC components, humic-like fluorescences were preferentially degraded by UV/chlorine oxidation compared with protein-like fluorescence potentially due to the differences of electronic moieties and molecular weight (MW). The decline in UV 254 , DOC, and fluorophores increased with increasing chlorine dosage; linear correlations between those indicators were observed during the two AOPs. Moreover, UV-LED/chlorine could achieve greater extents of MW change. Our study demonstrated that UV-LED could be a superior alternative for the future selection of UV source in the UV/chlorine process.

CAS / MDL: 1330-43-4
研究领域: 环境科学 · 水处理 · 化学工程
✓ 已验证 产品关联 DOI PubMed 高影响因子
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JOURNAL OF HAZARDOUS MATERIALS · 2023 · IF 13.6

Molecular insight into DOM fate using EEM-PARAFAC and FT-ICR MS and concomitant heavy metal behaviors in biologically treated landfill leachate during coagulation: Al speciation dependence

Libing Liu,Lei Du,Sen Lu,Bo Yang,Xu Zhao,Deli Wu,Xunchang Fei,Hongping He,Dongsheng Wang

Various combined processes with pre-coagulation have been developed for biologically treated landfill leachate , but the microscopic-level processes occurring during coagulation remain largely unknown. Herein, dissolved organic matter (DOM) fate using fluorescence excitation emission matrix spectroscopy combined with parallel factor analysis and electrospray ionization coupled Fourier transform-ion cyclotron resonance mass spectrometry and concomitant heavy metal (HM) behaviors were explored at the molecular level. In addition, AlCl 3 and two polyaluminum chloride (PACl) species (dominated by [AlO 4 Al 12 (OH) 24 (H 2 O) 12 ] 7+ and [(AlO 4 ) 2 Al 28 (OH) 56 (H 2 O) 26 ] 18+ , respectively) were used. The results show that all coagulants are efficient at removing DOM. PACl was found to be advantageous over AlCl 3 in overcoming pH fluctuation, which is ascribed to the different dominant mechanisms, namely, entrapment and sweep flocculation for AlCl 3 and charge neutralization for PACl. Consequently, PACl was more effective at removing humic substances , usually high-molecular-weight, oxygen-rich and unsaturated, than protein substances. For HM removal, PACl was likewise better and more stable, where As, Cu, Ni, Co and Hg were removed predominantly via adsorption, and Cr, Zn, Pb, Cd and Mn were removed via coprecipitation . Correlation analysis showed that humic substances tended to complex with HMs and be removed synergistically due to the ubiquitous occurrences of aromatic structures and oxygen-containing functional groups.

研究领域: 环境科学 · 分析化学
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SCIENCE OF THE TOTAL ENVIRONMENT · 2020 · IF 6.551

Photo-ammonification of low molecular weight dissolved organic nitrogen by direct and indirect photolysis

Yutong Zhang,Ruochun Zhang,Si-Liang Li,Khan M.G. Mostofa,Xiaoli Fu,Haodong Ji,Wen Liu,Peizhe Sun

The photo-ammonification process plays a crucial role in the transformation of dissolved organic nitrogen (DON) to dissolved inorganic nitrogen (DIN). However, previous studies have primarily focused on DON biotransformation than on abiotic processes. This study investigated the photo-ammonification process of nine model low molecular weight (LMW) DON molecules (e.g., amino acids, nucleotides, and urea) under the influence of different light sources. The results showed that photo-ammonification of model DON was mainly induced by UV light, while negligible contribution by visible light was found. Depending on their molecular structures, amino acids yielded different ammonia amounts, whereas negligible photo-ammonification was observed for nucleotides and urea. As for the reactive species, OH promoted ammonia yields of all the model amino acids; 3 CDOM ⁎ contributed to the photo-ammonification of six amino acids; 1 O 2 only had a positive impact on ammonification of tryptophan, histidine, and tyrosine; and CO 3 − accelerated ammonia generation from histidine and methionine. In natural water samples, tryptophan, tyrosine, histidine, and methionine generated significant ammonia. OH and 1 O 2 were speculated as the contributing reactive species based on kinetic studies as well as significant fluorescent humic-like and tyrosine-like substances degradation in irradiated samples compared to the raw samples characterized by the EEM-PARAFAC analysis. The negative linear correlations between photo-ammonification rates and the E LUMO –E HOMO of the amino acids emphasized the importance of the role of the molecular structure. Overall, these results revealed the LMW DON photo-ammonification mechanism in sunlit surface waters and highlighted its significance in the nitrogen biogeochemical cycle as well as water quality management.

CAS / MDL: 7722-84-1
研究领域: 环境科学 · 水化学 · 光化学 · 水质
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