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1.
Immun Inflamm Dis ; 12(4): e1251, 2024 Apr.
Article in English | MEDLINE | ID: mdl-38607251

ABSTRACT

BACKGROUND: For a long time, the prevailing viewpoint suggests that shorter telomere contribute to chromosomal instability, which is a shared characteristic of both aging and cancer. The newest research presented that T cell immune deficiency rather than chromosome instability predisposes patients with short telomere syndromes to some cancers. However, the relationship between genetically determined telomere length (TL) and immune cells remains unclear. METHODS: The two-sample Mendelian randomization analysis was conducted to elucidate the potential causal relationship. The genetic data of TL and immune cells were obtained from the Genome-Wide Association Study. The inverse variance weighted (IVW) method was used to estimate the effects primarily and another four methods were as a supplement. Sensitivity analysis was used to test the results. RESULTS: The IVW method showed a significant correlation between TL and the percentage of T cells in lymphocytes (odds ratio [OR]: 1.222, 95% confidence interval [CI]: 1.014-1.472, p = .035), indicating that shorter TL significantly increases the risk of low T cell percentage. Further analysis of T cell subsets indicated that shorter TL may primarily lead to a lower percentage of Natural Killer T cells (OR: 1.574, 95% CI: 1.281-1.935, p < .001). Analysis of B cell subsets revealed that shorter TL may be associated with a higher percentage of Naive-mature B cells, and a lower percentage of Memory B cells. And the sensitivity analysis indicated the validity and robustness of our findings. CONCLUSION: In summary, our findings suggest that shorter TL may be associated with a decline in the percentage of T cell, as well as impediments in the differentiation of B cell, consequently leading to the onset of immunosenescence and immunodeficiency. The relevant mechanisms and potential therapeutic avenues still need further investigation.


Subject(s)
Genome-Wide Association Study , Growth Disorders , Hypercalcemia , Immunologic Deficiency Syndromes , Metabolic Diseases , Nephrocalcinosis , Thymus Gland/abnormalities , Humans , Mendelian Randomization Analysis , Lymphocytes
2.
Biochim Biophys Acta Mol Basis Dis ; 1870(5): 167140, 2024 Mar 26.
Article in English | MEDLINE | ID: mdl-38548092

ABSTRACT

Heart failure (HF) is one of the major causes of death among diabetic patients. Although studies have shown that curcumin analog C66 can remarkably relieve diabetes-associated cardiovascular and kidney complications, the role of SJ-12, SJ-12, a novel curcumin analog, in diabetic cardiomyopathy and its molecular targets are unknown. 7-week-old male C57BL/6 mice were intraperitoneally injected with single streptozotocin (STZ) (160 mg/kg) to develop diabetic cardiomyopathy (DCM). The diabetic mice were then treated with SJ-12 via gavage for two months. Body weight, fast blood glucose, cardiac utrasonography, myocardial injury markers, pathological morphology of the heart, hypertrophic and fibrotic markers were assessed. The potential target of SJ-12 was evaluated via RNA-sequencing analysis. The O-GlcNAcylation levels of SP1 were detected via immunoprecipitation. SJ-12 effectively suppressed myocardial hypertrophy and fibrosis, thereby preventing heart dysfunction in mice with STZ-induced heart failure. RNA-sequencing analysis revealed that SJ-12 exerted its therapeutic effects through the modulation of the calcium signaling pathway. Furthermore, SJ-12 reduced the O-GlcNAcylation levels of SP1 by inhibiting O-linked N-acetylglucosamine transferase (OGT). Also, SJ-12 stabilized Sarcoplasmic/Endoplasmic Reticulum Calcium ATPase 2a (SERCA2a), a crucial regulator of calcium homeostasis, thus reducing hypertrophy and fibrosis in mouse hearts and cultured cardiomyocytes. However, the anti-fibrotic effects of SJ-12 were not detected in SERCA2a or OGT-silenced cardiomyocytes, indicating that SJ-12 can prevent DCM by targeting OGT-dependent O-GlcNAcylation of SP1.These findings indicate that SJ-12 can exert cardioprotective effects in STZ-induced mice by reducing the O-GlcNAcylation levels of SP1, thus stabilizing SERCA2a and reducing myocardial fibrosis and hypertrophy. Therefore, SJ-12 can be used for the treatment of diabetic cardiomyopathy.

3.
Inflammopharmacology ; 32(1): 683-692, 2024 Feb.
Article in English | MEDLINE | ID: mdl-37855981

ABSTRACT

BACKGROUND: Previous observational studies have identified an association between rheumatoid arthritis (RA) and inflammatory bowel disease (IBD). However, the causal relationship between RA and IBD in the East Asian population remains uncertain. METHODS: The two-sample Mendelian randomization (MR) analysis was conducted to elucidate the potential causal relationship between RA and IBD. Summary-level data from genome-wide association studies (GWAS) in the East Asian population were utilized, including RA (n = 19,190) and IBD (n = 6543), including Crohn's disease (CD, n = 5409) and ulcerative colitis (UC, n = 4853). The inverse variance weighted (IVW) method was employed as the primary analysis, supplemented by weighted median, weighted mode, simple median, MR-Egger, and MR-PRESSO analyses. Sensitivity analyses were conducted to assess the robustness of the results. Genetic data for RA (n = 22,515) were utilized to validate the findings in the East Asian population. RESULTS: The IVW method showed no significant association between genetically predicted RA and overall IBD in the East Asian population (OR = 1.028; 95% CI: 0.935-1.129; P = 0.567). The subgroup analysis revealed a positive association between RA and CD (OR = 1.268; 95% CI: 1.108-1.451; P < 0.001), while a negative association was observed with UC (OR = 0.839; 95% CI: 0.710-0.993; P = 0.041). These findings were supported by another set of RA data. Additionally, an SNP rs2071475 was identified to play an important role in CD and UC. CONCLUSION: This study revealed a potential increased susceptibility to CD and a decreased susceptibility to UC in the East Asian population with RA. Furthermore, a key SNP rs2071475 was discovered along with its opposite effects in CD and UC. These findings provide new evidence for research on the corresponding molecular mechanisms and offer insights for clinical management of RA-associated IBD.


Subject(s)
Arthritis, Rheumatoid , Inflammatory Bowel Diseases , Humans , East Asian People , Genome-Wide Association Study , Mendelian Randomization Analysis , Inflammatory Bowel Diseases/genetics , Arthritis, Rheumatoid/genetics
4.
J Chromatogr A ; 1706: 464250, 2023 Sep 13.
Article in English | MEDLINE | ID: mdl-37541057

ABSTRACT

The stable isotopic composition of natural gas can be used to identify its origin and source. However, low concentrations of gaseous hydrocarbons in high-mature natural and shale gases hinder accurate determination of their compound- and position-specific isotopic compositions. In this study, an online C2+ hydrocarbon gas concentration system combined with gas chromatography-isotope ratio mass spectrometry (GC-IRMS) or gas chromatography-pyrolysis-gas chromatography-isotope ratio mass spectrometry (GC-Py-GC-IRMS) was developed to determine compound- and position-specific isotopic compositions of low-abundance gaseous hydrocarbons. The lower limit of the gas concentration required for isotope ratio determination using the online concentration system is 0.001% (0.003%) for compound-specific carbon (hydrogen) isotopes and 0.005% for position-specific carbon isotopes and is thus applicable to most natural gas samples. The online concentration technique does not cause significant isotopic fractionation effects, and the combination with GC-IRMS and GC-Py-GC-IRMS can accurately and precisely determine the compound-specific δ13C and δD values of low-content C2+ gaseous hydrocarbons and the position-specific δ13C values (δ13Ca, δ13Cb, and SP values) of propane in low-content propane samples, respectively. The application of our method to two natural gas samples from the Ordos and Sichuan basins further confirms that the online concentration method allows simple and rapid determination of the compound- and position-specific isotopic compositions of low-abundance gaseous hydrocarbons.


Subject(s)
Gases , Natural Gas , Gases/analysis , Natural Gas/analysis , Propane , Hydrocarbons , Carbon Isotopes/analysis
5.
J Biochem Mol Toxicol ; 37(3): e23274, 2023 Mar.
Article in English | MEDLINE | ID: mdl-36536496

ABSTRACT

BACKGROUND: Circular RNA (circRNA) has been confirmed to be a key regulator for pancreatic cancer (PC) progression, but the role of circ_0000284 in PC development remains unclear. METHODS: Quantitative real-time PCR was used to measure the expression of circ_0000284, microRNA (miR)-1179, and rhophilin 2 (RHPN2). PC cell proliferation, metastasis, angiogenesis, and apoptosis were assessed by EdU assay, transwell assay, tube formation assay, and flow cytometry. Relative protein expression was determined by western blot analysis. The interaction between miR-1179 and circ_0000284 or RHPN2 was confirmed by dual-luciferase reporter assay and RNA pull-down assay. RESULTS: Circ_0000284 was significantly upregulated in PC tissues and cells, and its knockdown inhibited PC cell proliferation, migration, invasion, and angiogenesis while promoting apoptosis. MiR-1179 was downregulated in PC tissues and cells, and it could be sponged by circ_0000284. Moreover, the miR-1179 inhibitor reversed the regulation of circ_0000284 knockdown on PC cell progression. The highly expressed RHPN2 was found in PC tissues and cells, and it could be targeted by miR-1179. Also, circ_0000284 sponged miR-1179 to regulate RHPN2 expression. Overexpressed RHPN2 could reverse the regulation of circ_0000284 knockdown on PC cell progression. In addition, interference of circ_0000284 was discovered to repress PC tumor growth by regulating miR-1179/RHPN2.RHPN2. CONCLUSION: To sum up, our data confirmed that circ_0000284 facilitated PC malignant progression depending on the regulation of miR-1179/RHPN2 axis, suggesting that circ_0000284 might be a potential target for PC treatment.


Subject(s)
MicroRNAs , Pancreatic Neoplasms , Humans , Pancreas , Cell Proliferation , Adaptor Proteins, Signal Transducing , Pancreatic Neoplasms
6.
ACS Omega ; 7(16): 14317-14331, 2022 Apr 26.
Article in English | MEDLINE | ID: mdl-35573216

ABSTRACT

The mechanical and creep properties of shale strongly influence artificial hydraulic fracturing, wellbore stability, and the evaluation of reservoir performance in shale gas exploration. This study characterized these mechanical and creep properties at the microscale through nanoindentation tests and evaluated their dependence on the indentation test parameters, specifically, the indentation load and the loading strain rate. The mechanical parameters (the Young's modulus and hardness) of shale were strongly influenced by the magnitude of an indentation load (2-400 mN). Both parameters decreased sharply as the load increased from 2 to 200 mN; they then remained relatively stable at loads of 200-400 mN, suggesting that large indentation loads (200-400 mN) can be used to detect the mechanical responses of bulk shale. In contrast, both parameters increased slightly as the loading strain rate increased from 0.005 to 0.1 s-1. The indentation creep (C IT), related to creep behavior, and the creep strain rate sensitivity (m), related to the creep mechanism of shale, both increased with increasing the indentation load, whereas they decreased with increasing the loading strain rate. This demonstrates that increasing the load or decreasing the loading strain rate can increase creep deformation in shale during nanoindentation creep testing. The values of m varied from 0.040 to 0.124 under different loading conditions, suggesting that dislocation power-law creep may be the main mechanism controlling creep in shale. This study standardizes the testing parameters for the characterization of the mechanical properties of shale by nanoindentation testing and also advances our understanding of the deformation mechanisms of shale at the microscale.

7.
J Colloid Interface Sci ; 621: 222-231, 2022 Sep.
Article in English | MEDLINE | ID: mdl-35461137

ABSTRACT

Liquid organic electrolytes commonly employed in commercial Li-ion batteries suffer from safety issues such as flammability and explosions. Replacing liquid electrolytes with nonflammable electrolytes has become increasingly attractive in the development of safe, high-energy Li-metal batteries (LMBs). In this work, nonflammable, robust, and flexible composite polymer-polymer electrolytes (PPEs) were successfully fabricated by flame-retardant solution casting with polyimide (PI) and polyvinylidene fluoride (PVDF). The optimized nonflammable PPEs (e.g., PPE-50) demonstrate not only good mechanical properties (i.e., a high tensile strength of 29.6 MPa with an elongation at break of 87.2%), but also high Li salts dissolubility, the former of which ensures the suppression of Li dendrites, while the latter further improves the ionic conductivity (∼1.86 × 10-4 S cm-1 at 30 °C). The resulting symmetric cells (Li|PPE-50|Li) offer excellent Li stripping and plating stability for 1000 h at 0.5 mA cm-2/0.25 mAh cm-2 and 600 h at 2.0 mA cm-2/1.0 mAh cm-2. In addition, the LiFePO4|PPE-50|Li half cells show high cycling performance (e.g., a reversible discharge capacity of 135.9 mAh g-1 after 300 cycles at 1C) and rate capability (e.g., 117.2 mAh g-1 at 4C). The PPE-50 is also compatible with a high-voltage cathode (e.g., LiNi0.5Mn0.3Co0.2O2), and the resulting batteries demonstrate long-term cycling stability with a high cut-off voltage of 4.5 V vs. Li/Li+. Because of the incorporation of a mechanically robust and thermally stable PI, a polar PVDF, and flame-retardant trimethyl phosphate (TMP) within PPEs, as well as the coordination between Li salts and TMP, and the interaction between Li salts and polymers (especially between Li bis(oxalato)borate) and PI, as well as the bis(oxalato)borate anion and PI), PPEs show great potential for practical and high-energy LMBs without safety concerns.

8.
J Chromatogr A ; 1666: 462878, 2022 Mar 15.
Article in English | MEDLINE | ID: mdl-35151052

ABSTRACT

Compound-specific isotope analysis of crocetane in sediments can be used to determine its origin. However, the co-elution of crocetane with phytane and complex substrates hinders the accurate determination of its isotopic composition. A heart-cutting two-dimensional gas chromatography-isotope ratio mass spectrometry (2D-GC-IRMS) method was developed to determine δ13C values of crocetane. Full chromatographic separation of crocetane was achieved with a 30 m CycloSil-B chiral capillary first column and a 60 m Chiraldex B-pH capillary second column (two series-connected 30 m Chiraldex B-pH capillary columns). Analyses of standard mixtures confirmed that the new method has satisfactory accuracy (deviations from the authentic values <0.5‰) and precision (RSDs <5%) for carbon isotope analyses of crocetane and phytane. The application of the method to two sediment samples indicates that baseline resolution is achieved (R >1.5) for crocetane and phytane, with 13C-depleted crocetane (δ13C values of -119.5‰ and -111.5‰ in the two natural samples, respectively) being an indicator of anaerobic oxidation of methane in cold seep areas. The new 2D-GC-IRMS method allows simple and efficient determination of the compound-specific carbon isotopic compositions of crocetane.


Subject(s)
Terpenes , Carbon Isotopes/analysis , Gas Chromatography-Mass Spectrometry/methods , Terpenes/analysis
9.
J Nanosci Nanotechnol ; 21(10): 5120-5130, 2021 10 01.
Article in English | MEDLINE | ID: mdl-33875097

ABSTRACT

Poly(cyclotriphosphazene-co-4,4'-diaminodiphenyl ether) (PPO) microspheres were prepared via a precipitation polymerization method, using hexachlorocyclotriphosphazene (HCCP) and 4,4'-diaminodiphenyl ether (ODA) as monomers. Silver-loaded PPO (PPOA) microspheres were generated by the in situ loading of silver nanoparticles onto the surface by Ag+ reduction. Our results showed that PPOA microspheres were successfully prepared with a relatively uniform distribution of silver nanoparticles on microsphere surfaces. PPOA microspheres had good thermal stability and excellent antibacterial activity towards Escherichia coli and Staphylococcus aureus. Furthermore, PPOA microspheres exhibited lower cytotoxicity when compared to citrate-modified silver nanoparticles (c-Ag), and good sustained release properties. Our data indicated that polyphosphazene-based PPOA microspheres are promising antibacterial agents in the biological materials field.


Subject(s)
Metal Nanoparticles , Silver , Anti-Bacterial Agents/pharmacology , Microbial Sensitivity Tests , Microspheres , Organophosphorus Compounds , Polymers , Silver/pharmacology
10.
J Nanosci Nanotechnol ; 21(1): 646-658, 2021 01 01.
Article in English | MEDLINE | ID: mdl-33213665

ABSTRACT

Shale gas has been playing an increasingly important role in meeting global energy demands. The heterogeneity of the pore structure in organic-rich shales greatly affects the adsorption, desorption, diffusion and flow of gas. The pore size distribution (PSD) is a key parameter of the heterogeneity of the shale pore structure. In this study, the Neimark-Kiselev (N-K) fractal approach was applied to investigate the heterogeneity in the PSD of the lower Silurian organic-rich shales in South China using low-pressure N2 adsorption, total organic carbon (TOC) content, maturity analysis, X-ray diffraction (XRD) and field emission scanning electron microscopy (FE-SEM) measurements. The results show that (1) the fractal dimension DN-K obtained by N-K theory better represents the heterogeneity of the PSD in shale at an approximately 1-100 nm scale. The DN-K values range from 2.3801 to 2.9915, with a mean of 2.753. The stronger the PSD heterogeneity is, the higher the DN-K value in shale is. (2) The clay-rich samples display multimodal patterns at pore sizes greater than 20 nm, which strongly effect the PSD heterogeneity. Quartz-rich samples display major peaks at less than or equal to a 10 nm pore size, with a smaller effect on the PSD heterogeneity in most cases. In other brittle mineral-rich samples, there are no obvious major peaks, and a weak heterogeneity of the PSDs is displayed. (3) A greater TOC content, maturity, clay content and pore size can cause stronger heterogeneity of the PSD and higher fractal dimensions in the shale samples. This study helps to understand and compare the PSD and fractal characteristics from different samples and provides important theoretical guidance and a scientific basis for the exploration and development of shale gas resources.

11.
Nanoscale ; 12(23): 12432-12443, 2020 Jun 21.
Article in English | MEDLINE | ID: mdl-32495797

ABSTRACT

At present, a technique potentially capable of measuring values of Young's modulus at the nanoscale is atomic force microscopy (AFM) working in the indentation mode. However, the question if AFM indentation data can be translated into absolute values of the modulus is not well-studied as yet, in particular, for the most interesting case of stiff nanocomposite materials. Here we investigate this question. A special sample of nanocomposite material, shale rock, was used, which is relatively homogeneous at the multi-micron scale. Two AFM modes, force-volume and PeakForce QNM were used in this study. The nanoindentation technique was used as a control benchmark for the measurement of effective Young's modulus of the shale sample. The indentation rate was carefully controlled. To ensure the self-consistency of the mechanical model used to analyze AFM data, the model was modified to take into account the presence of the surface roughness. We found excellent agreement between the average values of effective Young's modulus calculated within AFM and the nanoindenter benchmark method. At the same time, the softest and hardest areas of the sample were seen only with AFM.

12.
Environ Pollut ; 260: 114034, 2020 May.
Article in English | MEDLINE | ID: mdl-32014746

ABSTRACT

The demineralized fraction (DM), lipid-free fraction (LF), nonhydrolyzable organic carbon fraction (NHC), and black carbon (BC) were isolated from five marine surface sediments, and they were characterized by elemental analysis as well as CO2 and N2 adsorption techniques, respectively. The NHC fractions were characterized using advanced solid-state 13C nuclear magnetic resonance (NMR) and x-ray photoelectron spectroscopy (XPS). Then, the sorption isotherms of phenanthrene (Phen) and nonylphenol (NP) on all of the samples were investigated by a batch technique. The CO2 micropore volumes were corrected for the outer specific surface areas (SSAs) by using the N2-SSA. Significant correlations between the micropore-filling volumes of Phen and NP and the micropore volumes suggested that the micropore-filling mechanism dominated the Phen and NP sorption. Meanwhile, the (O + N)/C atomic ratios were negatively and significantly correlated with the sorption capacities of Phen and NP, indicating that the sedimentary organic matter (SOM) polarity also played a significant role in the sorption process. In addition, a strong linear correlation was demonstrated between the aromatic C and the sorption capacity of Phen for the NHC fractions. This study demonstrates the importance of the micropores, polarity, and aromaticity on the sorption processes of Phen and NP in the sediments.


Subject(s)
Phenanthrenes/chemistry , Phenols/chemistry , Adsorption , Geologic Sediments
13.
Environ Sci Technol ; 53(24): 14285-14295, 2019 12 17.
Article in English | MEDLINE | ID: mdl-31578063

ABSTRACT

Although spores/pollens are so abundant and ubiquitous in the environment, the role of these natural organic matter concerning fate and transport of organic pollutants in the environment is neglected. Lipid-free fractions and sporopollenins were isolated from seven spores/pollens collected from lower and higher biota species and were characterized by elemental analysis, CO2 adsorption techniques, and advanced solid-state 13C nuclear magnetic resonance spectroscopy. Then, the sorption isotherms of phenanthrene (Phen) on all the samples were investigated by a batch technique. The sporopollenins were a highly cross-linked polymer including alkyl carbon, poly(methylene) carbon, and aromatic carbon as well as oxygen functionalities; additionally, their sorption capacities (Koc) for Phen reached up to 1 170 000 mL/g, suggesting that some of the sporopollenins were good biopolymeric sorbents for the removal of hydrophobic organic contaminants in aquatic media. A highly significant and positive correlation between the sorption capacity of Phen and the aliphaticity of the sporopollenins suggested that their structure was critical to Phen sorption. Meanwhile, the (O + N)/C atomic ratios and polar groups were significantly and negatively correlated with the sorption capacity of Phen, indicating that accessibility also played a significant role in the sorption process. Moreover, variable correlations between the sorption capacities (Koc) and the micropore volumes of the spore/pollen fractions were observed. This study sheds light on the importance of the polarity, microporosity, and structure of sporopollenins in the sorption process of Phen.


Subject(s)
Phenanthrenes , Adsorption , Biopolymers , Biota , Carotenoids , Pollen , Spores
15.
Langmuir ; 35(13): 4481-4490, 2019 04 02.
Article in English | MEDLINE | ID: mdl-30836753

ABSTRACT

The applications of graphene-based adsorbents were limited because of their complicated manufacturing technology and hi cost, thus it is very important to prepare new inexpensive and easily manufactured graphene-based adsorbents. Herein, novel GCP hydrogels with different graphene oxide (GO), chitosan (CS), and poly(vinyl alcohol) (PVA) ratios were facilely prepared through a method of freeze-thaw physical cross-linking, which was green and low-cost, and the structural characterization and adsorptive property of the optimum GCP1:2:4 hydrogel toward Cd2+ and Ni2+ in wastewater was evaluated. It was found that the GCP1:2:4 hydrogel had good mechanical strength and a special 3D interconnection porous structure. The isotherms of adsorption used the Langmuir model, and the kinetics of adsorption following the pseudo-second-order model were confirmed. Moreover, the adsorption property with respect to Cd2+ and Ni2+ in wastewater has been largely effected by the pH and was less influenced by the ionic strength and humic acid, and the GCP1:2:4 hydrogel possessed excellent adsorptive and recyclable properties. These results demonstrated that the GCP1:2:4 hydrogel could serve as a desirable adsorbent to get rid of heavy metal ions in sewage.

16.
Sci Total Environ ; 642: 1050-1059, 2018 Nov 15.
Article in English | MEDLINE | ID: mdl-30045487

ABSTRACT

Black carbon was produced by slow pyrolysis under an oxygen-limited condition at 500 °C, and was modified by some chemical methods (oxidation, hydrolysis, activation, and surface recombination). The modified samples were characterized by using elemental analysis, Fourier transformed infrared spectroscopy (FTIR), X-ray photoelectron spectroscopy (XPS) surface analysis, Boehm titration, cation exchange capacity(CEC)analysis, CO2 adsorption analysis, and then used to investigate the sorption behavior of phenanthrene. The results showed that the activation of ZnCl2 gave a maximum nanopore volume of 96.5 µL/g and a specific surface area of 241 m2/g, while the oxidation of NaClO gave a minimum nanopore volume of 63.3 µL/g and a specific surface area of 158 m2/g. The FTIR, XPS, and Boehm titration analysis showed that the new oxygen-containing functional groups were introduced during the oxidation treatments of H2O2 and NaClO. The sorption of phenanthrene on all samples was typically nonlinear, and the nonlinear factor (n) was negatively correlated with Vo, especially with Vo at 0-1.1 nm. The sorption parameter (log KOC) was positively correlated with nanopore volume (Vo) and specific surface area (SSA). Moreover, the model analysis showed that the nanopore filling was the main sorption mechanism, and molecular sieve effect was observed in the sorption of phenanthrene.

17.
Environ Pollut ; 225: 628-636, 2017 Jun.
Article in English | MEDLINE | ID: mdl-28341327

ABSTRACT

The desorption kinetics and mechanism were investigated using a Tenax extraction technique on different sediments spiked with radiocarbon-labeled benzo[a]pyrene (BaP). Five sedimentary fractions were sequentially fractionated, and the only nonhydrolyzable organic carbon fractions (NHC) were characterized using advanced solid-state 13C nuclear magnetic resonance spectroscopy (NMR), improved six end-member model, and a CO2 gas adsorption technique. The sediments contained high percentages of algaenan and/or sporopollenin but low percentages of black carbon and lignin. A first-order, two-compartment kinetics model described the desorption process very well (R2 > 0.990). Although some of the organic carbon fractions were significantly related to the desorption kinetics parameters, the NHC fractions showed the highly significant correlation. Moreover, the nanoporosity or specific surface area (SSA) of the NHC fractions was highly related to their OC contents and aliphatic C (R2 = 0.960, p < 0.01). The multiple regression equations among the desorption kinetics parameters, structural parameters, and nanoporosity were well established (R2=>0.999). Nanoporosity and aromatic C were the dominant contributors. Furthermore, the enhanced percentages of desorbed BaP at elevated temperatures significantly showed a linear regression with the structure and nanoporosity. To our knowledge, the above evidence demonstrates for the first time that the transfer (or diffusion) of BaP in the nanopores of condensed aromatic components is the dominant mechanism of the desorption kinetics of BaP at organic matter particle scale.


Subject(s)
Benzo(a)pyrene/chemistry , Geologic Sediments/chemistry , Humic Substances/analysis , Models, Chemical , Adsorption , Benzo(a)pyrene/analysis , Kinetics , Soot
18.
Sci Total Environ ; 581-582: 874-884, 2017 Mar 01.
Article in English | MEDLINE | ID: mdl-28089533

ABSTRACT

The sources of sediment organic matter (SOM) could be explained by various indicators. To test their biases and associations, the present study determined multiple indicators for SOM source apportionment, including elemental analysis (carbon and nitrogen, and their stable isotope δ13C and δ15N), n-alkanes compositions as well as derivative indicators (e.g., terrigenous to aquatic ratio), and carbon isotopes of n-alkane in Lake Chaohu, a eutrophic lake. The spatial variation of anthropogenic effects could be revealed by SOM elemental variations. The n-alkanes of all samples had a bimodal distribution with the 1st peak at n-alkane with 17 carbons (C17) and the 2nd predominant peak at C29. The parity advantage index of n-alkanes indicated that the sediments had mixed characteristics of both endogenous and terrigenous sources. Some n-alkanes indicators also revealed eutrophication characteristics of dominant algae in Lake Chaohu. SOM received a mixed contribution of plankton (I), low-latitude terrestrial high-grade plants (II) and microbial material (III) as indicated by isotopic compositions of long-chain n-alkane. Multiport element model (MEM) showed the contribution of self-generated sources of organic matter in Lake Chaohu is >50%, indicating the historic serious eutrophication in Lake Chaohu. The main sources of SOM in the eastern part of the lake were algae and terrestrial input, with little input from microbes, and the contribution from algae decreased from west to east. The multiple indicators' judgment by MEM and principle component analysis (PCA) was of ecological significance and proposed because they offered scientific tools for disclosing the historic variations of SOM as well as their sources.

19.
Environ Pollut ; 219: 456-465, 2016 Dec.
Article in English | MEDLINE | ID: mdl-27238761

ABSTRACT

To better understand interaction mechanism of sediment organic matter with hydrophobic organic compounds, sorption of phenanthrene (Phen) and nonylphenol (NP) by bulk sediments and their fractions was investigated. Three surface sediments were selectively fractionated into different organic fractions, including the demineralized carbon (DM), lipid free carbon (LF), lipid (LP), and nonhydrolyzable carbon (NHC) fractions. The structure and microporosity of the isolated fractions were characterized by NMR and CO2 adsorption techniques, and used as sorbents for Phen and NP. The calculated micropore volumes (Vo) and specific surface area (SSA) values are positively related to the concentrations of aromatic C and char for the DM, LF and NHC fractions, suggesting that aromatic moieties and char component significantly contribute to the microporosity. The LF fractions exhibit greater sorption affinity than the DM fractions do, indicating that the presence of LP could block the accessibility of sorption sites for Phen and NP. Significant and positive correlations among log K'FOC values for Phen and NP and aromatic carbon and char contents, and Vo and SSA values suggest the aromatic moieties and microporosity dominate their sorption of HOCs by sediment organic matter (SOM). As the NHC fractions have much stronger sorption than other fractions do, they dominate the overall sorption by the bulk samples. This study indicated that the important roles of aromatic moieties, accessibility, and microporosity in the sorption of HOCs by SOM.


Subject(s)
Carbon/chemistry , Geologic Sediments/chemistry , Phenanthrenes/analysis , Phenols/analysis , Rivers/chemistry , Water Pollutants, Chemical/analysis , Adsorption , China , Environmental Restoration and Remediation , Hydrophobic and Hydrophilic Interactions , Magnetic Resonance Spectroscopy , Models, Theoretical , Phenanthrenes/chemistry , Phenols/chemistry , Porosity , Surface Properties , Water Pollutants, Chemical/chemistry
20.
Environ Sci Pollut Res Int ; 21(22): 13138-47, 2014 Nov.
Article in English | MEDLINE | ID: mdl-24996939

ABSTRACT

Lakes Dianchi (DC) and Bosten (BST) were determined to be at different stages of eutrophication, by use of total organic carbon content, bulk carbon isotopic composition, bulk nitrogen isotopic composition, and bound saturated fatty acid (BSFA) concentrations in sediment cores. A rapid increase in the supply of organic matter (OM) to DC began after the 1950s, while the environment and trophic status of BST remained constant as indicated by characteristics of OM input to sediments. The BSFA ratios of nC14 + nC16 + nC18/nC24 + nC26 + nC28 increase upward from 7 to 13 in the DC core, which are significantly greater than those from BST (2 to 3). This result is consistent with algae or bacteria being the dominant contribution of the OM increase induced by eutrophication in DC. The positive shift of nC16 compound-specific δ (13)C in the upper section might be an indicator of excess algal productivity, which was observed in the two lakes. The positive shifts of compound-specific δ (13)C of other BSFAs were also observed in the upper section of the core only from DC. The observed trends of compound-specific δ(13)C of BSFA originated from different sources became more consistent, which reflected the intensified eutrophication had profoundly affected production and preservation of OM in DC. The results observed for BST indicated that accumulation of algae did not affect the entire aquatic ecosystem until now.


Subject(s)
Fatty Acids/analysis , Geologic Sediments/analysis , Lakes/analysis , Water Pollutants, Chemical/analysis , Bacteria , Carbon Isotopes/analysis , China , Ecosystem , Eutrophication , Nitrogen Isotopes/analysis , Water Microbiology
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