Marine dissolved organic matter(DOM) is one of the largest dynamic pools of organic carbon in the global carbon cycle, yet DOM is still chemically poorly characterized. To better understand the origin, composition, an...Marine dissolved organic matter(DOM) is one of the largest dynamic pools of organic carbon in the global carbon cycle, yet DOM is still chemically poorly characterized. To better understand the origin, composition, and cycling of DOM in the China marginal sea, dissolved humic substances(DHS) were isolated from seawaters in two locations in the Southern Yellow Sea. The DHS were subdivided into fulvic acids(FAs), humic acids(HAs) and the XAD-4 fractions. Complementary analytical approaches were used to characterize the isolated DHS samples including stable carbon isotopic composition, Fourier transform infrared spectroscopy(FTIR), ^(13) C cross polarization magic angle spinning(CP/MAS) nuclear magnetic resonance(NMR), and pyrolysis gas chromatography-mass spectrometry(Py-GC/MS). The results demonstrated that both DHS samples encountered the influences from marine source, indicating that algal and microbial-derived materials are the predominant precursors for the studied samples. The three fractions of DHS showed diff erent properties. FAs presented more aromatic features, whereas HAs contained more aliphatic lipids and proteinaceous materials. The XAD-4 fractions were enriched in ^(13) C and contained more carbohydrates but less aromatic compounds. The lower molecular weight and higher heteroatom content and number of carboxyl groups for the XAD-4 fractions may give them considerable geochemical significance for aspects of trace metal species, bioavailability of pollutants, mineral weathering and water acidification in marine environments.展开更多
Humic acid(HA)can adsorb onto mineral surfaces,modifying the physicochemical properties of the mineral.Therefore,understanding the sorption behavior of HA onto mineral surfaces is of particular interest,since the fate...Humic acid(HA)can adsorb onto mineral surfaces,modifying the physicochemical properties of the mineral.Therefore,understanding the sorption behavior of HA onto mineral surfaces is of particular interest,since the fate and transport of many organic and inorganic contaminants are highly correlated to HA adsorbed onto clay surfaces.Due to the extreme heterogeneity of HA,the extracted IHSS Leonardite humic acid(LHA)used in this work was fractionated using an ultrafiltration technique(UF)into different molecular size fractions(Fr1,>0.2μm;Fr2,0.2 pm-300,000 daltons;Fr3,300,000-50,000 daltons;Fr4,50,000-10,000 daltons;Fr5,10,000-1000 daltons).Equilibrium and the kinetics of LHA and fraction adsorption onto kaolinite and montmorillonite were investigated.The results demonstrated that the maximum adsorption capacity of LHA,Frl,Fr2,Fr3,Fr4,and Fr5 was 5.99,13.69,10.29,7.02,5.9&and 5.09 on kaolinite while it was 8.29,22.62,13.17,8.91,8.62,and 5.69 on montmorillonite,respectively.The adsorption equilibrium data showed that the adsorption behavior of LHA and its fractions could be described more practically by the Langmuir model than the Freundlich model.The rate of humic acid fraction adsorption onto clays increased with decreasing molecular size fraction and increasing carboxylic group content.Pseudo-first-and second-order models were used to assess the kinetic data and the rate constants.The results explained that LHA and its fractions adsorption on clay minerals conformed more to pseudosecondo rder.展开更多
Mangrove-derived dissolved organic matter(DOM) has an important effect on estuarine and coastal area on a large scale.In order to improve the understanding of origin,composition,and fate of DOM in mangrove-fringed est...Mangrove-derived dissolved organic matter(DOM) has an important effect on estuarine and coastal area on a large scale.In order to improve the understanding of origin,composition,and fate of DOM in mangrove-fringed estuarine and coastal areas,dissolved humic substances(DHS) were isolated from one mangrove pore-water sample and one near-shore seawater sample downstream the mangrove pore-water site in the eastern coast of Hainan Island,South China.Fulvic acids,humic acids and XAD-4 fractions were obtained from the two water samples by using a two-column array of XAD-8 and XAD-4 resins.Chemical and spectroscopic methods were used to analyze the features of these DHS.Compared to the mangrove pore-water DHS,the near-shore seawater DHS were found rich in 13 C with lower C/N ratios and more aliphatic compounds and carbohydrates,but less aromatic structures and carboxyl groups.As for the three fractions of the two DHS,XAD-4 fractions contain more aliphatics,carbohydrates,carboxyl groups,and enrich in 13 C with respect to both fulvic and humic acids.Photo-oxidation transformation and contribution from marine-derived DOM were considered as the main reasons resulted in the difference in compositional features for these DHS in this study.展开更多
以城市污水厂二级出水为研究对象,利用大孔吸附树脂将污水中溶解性有机物(Dissolved organic matter,DOM)分离成疏水酸性、中性、碱性物质和亲水性物质等4个组分,同时分析了各组分的有机物特性.结果表明,二级出水溶解性有机物中疏水酸...以城市污水厂二级出水为研究对象,利用大孔吸附树脂将污水中溶解性有机物(Dissolved organic matter,DOM)分离成疏水酸性、中性、碱性物质和亲水性物质等4个组分,同时分析了各组分的有机物特性.结果表明,二级出水溶解性有机物中疏水酸性物质是二级出水溶解性有机物的主要组成部分.4种组分中均含有腐殖质类物质,疏水酸性物质(Hydrophobic acids,HOA)和疏水中性物质(Hydrophobic neutrals,HON)中腐殖酸类峰的荧光强度较大,亲水性物质(Hydrophilic fraction,HI)中的蛋白峰荧光强度较大.腐殖质类物质分子量分布较为单一,主要分布在0.9 k Da左右,而疏水性组分蛋白类物质分子量分布较为广泛,在200 k Da左右及小于9 k Da时均有一定分布,亲水性组分蛋白类物质主要由分子量小于9 k Da的物质组成.X射线光电子能谱(X-ray photoelectron spectroscopy,XPS)分析结果表明,HOA、HON中含有较多的芳香族化合物,而疏水碱性物质(Hydrophobic bases,HOB)、HI中则含有较多的羰基和羧基类官能团.展开更多
基金Supported by the National Natural Science Foundation of China(No.41403108)the West Light Foundation of the Chinese Academy of Sciences(No.Y412011004)the Natural Science Foundation of Qinghai Province(No.2014-ZJ-937Q)
文摘Marine dissolved organic matter(DOM) is one of the largest dynamic pools of organic carbon in the global carbon cycle, yet DOM is still chemically poorly characterized. To better understand the origin, composition, and cycling of DOM in the China marginal sea, dissolved humic substances(DHS) were isolated from seawaters in two locations in the Southern Yellow Sea. The DHS were subdivided into fulvic acids(FAs), humic acids(HAs) and the XAD-4 fractions. Complementary analytical approaches were used to characterize the isolated DHS samples including stable carbon isotopic composition, Fourier transform infrared spectroscopy(FTIR), ^(13) C cross polarization magic angle spinning(CP/MAS) nuclear magnetic resonance(NMR), and pyrolysis gas chromatography-mass spectrometry(Py-GC/MS). The results demonstrated that both DHS samples encountered the influences from marine source, indicating that algal and microbial-derived materials are the predominant precursors for the studied samples. The three fractions of DHS showed diff erent properties. FAs presented more aromatic features, whereas HAs contained more aliphatic lipids and proteinaceous materials. The XAD-4 fractions were enriched in ^(13) C and contained more carbohydrates but less aromatic compounds. The lower molecular weight and higher heteroatom content and number of carboxyl groups for the XAD-4 fractions may give them considerable geochemical significance for aspects of trace metal species, bioavailability of pollutants, mineral weathering and water acidification in marine environments.
基金funded by a Fulbright Visiting Scholar fellowship to Mohamed El-sayed and performed at South Dakota State University
文摘Humic acid(HA)can adsorb onto mineral surfaces,modifying the physicochemical properties of the mineral.Therefore,understanding the sorption behavior of HA onto mineral surfaces is of particular interest,since the fate and transport of many organic and inorganic contaminants are highly correlated to HA adsorbed onto clay surfaces.Due to the extreme heterogeneity of HA,the extracted IHSS Leonardite humic acid(LHA)used in this work was fractionated using an ultrafiltration technique(UF)into different molecular size fractions(Fr1,>0.2μm;Fr2,0.2 pm-300,000 daltons;Fr3,300,000-50,000 daltons;Fr4,50,000-10,000 daltons;Fr5,10,000-1000 daltons).Equilibrium and the kinetics of LHA and fraction adsorption onto kaolinite and montmorillonite were investigated.The results demonstrated that the maximum adsorption capacity of LHA,Frl,Fr2,Fr3,Fr4,and Fr5 was 5.99,13.69,10.29,7.02,5.9&and 5.09 on kaolinite while it was 8.29,22.62,13.17,8.91,8.62,and 5.69 on montmorillonite,respectively.The adsorption equilibrium data showed that the adsorption behavior of LHA and its fractions could be described more practically by the Langmuir model than the Freundlich model.The rate of humic acid fraction adsorption onto clays increased with decreasing molecular size fraction and increasing carboxylic group content.Pseudo-first-and second-order models were used to assess the kinetic data and the rate constants.The results explained that LHA and its fractions adsorption on clay minerals conformed more to pseudosecondo rder.
基金Project(42030711)supported by the Key Project of National Natural Science Foundation of ChinaProject(42177391)supported by the National Natural Science Foundation of China。
基金Supported by the National Natural Science Foundation of China(Nos.40906041,41021064)the State Key Laboratory of Estuarine and Coastal Research (SKLEC) of East China Normal University(Nos.2012KYYW05,201202)
文摘Mangrove-derived dissolved organic matter(DOM) has an important effect on estuarine and coastal area on a large scale.In order to improve the understanding of origin,composition,and fate of DOM in mangrove-fringed estuarine and coastal areas,dissolved humic substances(DHS) were isolated from one mangrove pore-water sample and one near-shore seawater sample downstream the mangrove pore-water site in the eastern coast of Hainan Island,South China.Fulvic acids,humic acids and XAD-4 fractions were obtained from the two water samples by using a two-column array of XAD-8 and XAD-4 resins.Chemical and spectroscopic methods were used to analyze the features of these DHS.Compared to the mangrove pore-water DHS,the near-shore seawater DHS were found rich in 13 C with lower C/N ratios and more aliphatic compounds and carbohydrates,but less aromatic structures and carboxyl groups.As for the three fractions of the two DHS,XAD-4 fractions contain more aliphatics,carbohydrates,carboxyl groups,and enrich in 13 C with respect to both fulvic and humic acids.Photo-oxidation transformation and contribution from marine-derived DOM were considered as the main reasons resulted in the difference in compositional features for these DHS in this study.
文摘以城市污水厂二级出水为研究对象,利用大孔吸附树脂将污水中溶解性有机物(Dissolved organic matter,DOM)分离成疏水酸性、中性、碱性物质和亲水性物质等4个组分,同时分析了各组分的有机物特性.结果表明,二级出水溶解性有机物中疏水酸性物质是二级出水溶解性有机物的主要组成部分.4种组分中均含有腐殖质类物质,疏水酸性物质(Hydrophobic acids,HOA)和疏水中性物质(Hydrophobic neutrals,HON)中腐殖酸类峰的荧光强度较大,亲水性物质(Hydrophilic fraction,HI)中的蛋白峰荧光强度较大.腐殖质类物质分子量分布较为单一,主要分布在0.9 k Da左右,而疏水性组分蛋白类物质分子量分布较为广泛,在200 k Da左右及小于9 k Da时均有一定分布,亲水性组分蛋白类物质主要由分子量小于9 k Da的物质组成.X射线光电子能谱(X-ray photoelectron spectroscopy,XPS)分析结果表明,HOA、HON中含有较多的芳香族化合物,而疏水碱性物质(Hydrophobic bases,HOB)、HI中则含有较多的羰基和羧基类官能团.
