A low-fouling electrochemical biosensor based on BSA hydrogel doped with carbon black for the detection of cortisol in human serum.

Electrochemical biosensors with high sensitivity can detect low concentrations of biomarkers, but their practical detection applications in complex biological environments such as human serum and sweat are severely limited by the biofouling. Herein, a conductive hydrogel based on bovine serum albumin (BSA) and conductive carbon black (CCB) was prepared for the construction of an antifouling biosensor. The BSA hydrogel (BSAG) was doped with CCB, and the prepared composite hydrogel exhibited good conductivity originated from the CCB and antifouling capability owing to the BSA hydrogel. An antifouling biosensor for the sensitive detection of cortisol was fabricated by drop-coating the conductive hydrogel onto a poly(3,4-ethylenedioxythiophene) (PEDOT) modified electrode and further immobilizing the cortisol aptamer. The constructed biosensor showed a linear range of 100 pg mL-1 - 10 µg mL-1 and a limit of detection of 26.0 pg mL-1 for the detection of cortisol, and it was capable of assaying cortisol accurately in complex human serum. This strategy of preparing antifouling and conductive hydrogels provides an effective way to develop robust electrochemical biosensors for biomarker detection in complex biological media.

Anisotropic Elastomer Ionomer Composite-Based Strain Sensors: Achieving High Sensitivity and Wide Detection for Human Motion Detection and Wireless Transmission.

Anisotropic strain sensors capable of multidirectional sensing are crucial for advanced sensor applications in human motion detection. However, current anisotropic sensors encounter challenges in achieving a balance among high sensitivity, substantial stretchability, and a wide linear detection range. To address these challenges, a facile freeze-casting strategy was employed to construct oriented filler networks composed of carbon nanotubes and conductive carbon black within a brominated butyl rubber ionomer (iBIIR) matrix. The resulting anisotropic sensor based on the iBIIR composites exhibited distinct gauge factors (GF) in the parallel and vertical directions (GF∥ = 4.91, while GF⊥ = 2.24) and a broad linear detection range over a strain range of 190%. This feature enables the sensor to detect various human activities, including uniaxial pulse, finder bending, elbow bending, and cervical spine movements. Moreover, the ion-cross-linking network within the iBIIR, coupled with strong π-cation interactions between the fillers and iBIIR macromolecules, imparted high strength (12.3 MPa, nearly twice that of pure iBIIR) and an ultrahigh elongation at break (>1800%) to the composites. Furthermore, the sensor exhibited exceptional antibacterial effectiveness, surpassing 99% against both Escherichia coli and Staphylococcus aureus. Notably, the sensor was capable of wireless sensing. It is anticipated that anisotropic sensors will have extensive application prospects in flexible wearable devices.

Molecular-weight dependent promotion and competition effects of natural organic matter on dissolved black carbon removal by coagulation.

Dissolved black carbon (DBC) is the ubiquitous component of dissolved organic matter pools with the high reactivity for disinfection byproducts formation. However, it is unknown that the influence of molecular weight (MW) of natural organic matter (NOM) on the DBC removal from potable water sources. Therefore, it was studied that the DBC removal by coagulation in the presence of the NOM with various molecular weights. The DBC removal was promoted due to the presence of NOM and the promotion degree decreased with decreasing MW of NOM. Furthermore, the removal ratio of humic-like component increased as the MW of NOM decreased, suggesting that the competition between DBC and NOM increased with decreasing MW. The functional groups after coagulation were the same with that before coagulation as the MW of NOM varied, suggesting that the molecular structure was not the key factor of influencing the DBC removal. This study will give the deep insight into the prediction of the DBC removal ratio by coagulation based on the MW of NOM in water sources.

Mechanism of soot and particulate matter formation during high temperature pyrolysis and gasification of waste derived from MSW.

This research investigates the formation mechanism of soot and particulate matter during the pyrolysis and gasification of waste derived from Municipal Solid Waste (MSW) in a laboratory scale drop tube furnace. Compared with CO2 gasification atmosphere, more ultrafine particles (PM0.2, aerodynamic diameter less than 0.2 µm) were generated in N2 atmosphere at 1200℃, which were mainly composed of polycyclic aromatic hydrocarbons (PAHs), graphitic carbonaceous soot and volatile alkali salts. High reaction temperatures promote the formation of hydrocarbon gaseous products and their conversion to PAHs, which ultimately leads to the formation of soot particles. The soot particles generated by waste derived from MSW pyrolysis and gasification both have high specific surface area and well-developed pore structure. Compared with pyrolysis, the soot generated by gasification of waste derived from MSW had smaller size and higher proportion of inorganic components. The higher pyrolysis temperature led to the collapse of the mesoporous structure of submicron particles, resulting in a decrease in total pore volume and an increase in specific surface area. Innovatively, this research provides an explanation for the effect of reaction temperature/ CO2 on the formation pathways and physicochemical properties of soot and fine particulate matter.

Highly Reactive Peroxide Species Promoted Soot Oxidation over an Ordered Macroporous Ce0.8Zr0.2O2 Integrated Catalyzed Diesel Particulate Filter.

Particulate matter, represented by soot particles, poses a significant global environmental threat, necessitating efficient control technology. Here, we innovatively designed and elaborately fabricated ordered hierarchical macroporous catalysts of Ce0.8Zr0.2O2 (OM CZO) integrated on a catalyzed diesel particulate filter (CDPF) using the self-assembly method. An oxygen-vacancy-enriched ordered macroporous Ce0.8Zr0.2O2 catalyst (VO-OM CZO) integrated CDPF was synthesized by subsequent NaBH4 reduction. The VO-OM CZO integrated CDPF exhibited a markedly enhanced soot oxidation activity compared to OM CZO and powder CZO coated CDPFs (T50: 430 vs 490 and 545 °C, respectively). The well-defined OM structure of the VO-OM CZO catalysts effectively improves the contact efficiency between soot and the catalysts. Meanwhile, oxygen vacancies trigger the formation of a large amount of highly reactive peroxide species (O22-) from molecular oxygen (O2) through electron abstraction from the three adjacent Ce3+ (3Ce3+ + Vö + O2 → 3Ce4+ + O22-), contributing to the efficient soot oxidation. This work demonstrates the fabrication of the ordered macroporous CZO integrated CDPF and reveals the importance of structure and surface engineering in soot oxidation, which sheds light on the design of highly efficient PM capture and removal devices.

Enhancing Extracellular Electron Transfer of a 3D-Printed Shewanella Bioanode with Riboflavin-Modified Carbon Black Bioink.

3D printing of a living bioanode holds the potential for the rapid and efficient production of bioelectrochemistry systems. However, the ink (such as sodium alginate, SA) that formed the matrix of the 3D-printed bioanode may hinder extracellular electron transfer (EET) between the microorganism and conductive materials. Here, we proposed a biomimetic design of a 3D-printed Shewanella bioanode, wherein riboflavin (RF) was modified on carbon black (CB) to serve as a redox substance for microbial EET. By introducing the medicated EET pathways, the 3D-printed bioanode obtained a maximum power density of 252 ± 12 mW/m2, which was 1.7 and 60.5 times higher than those of SA-CB (92 ± 10 mW/m2) and a bare carbon cloth anode (3.8 ± 0.4 mW/m2). Adding RF reduced the charge-transfer resistance of a 3D-printed bioanode by 75% (189.5 ± 18.7 vs 47.3 ± 7.8 Ω), indicating a significant acceleration in the EET efficiency within the bioanode. This work provided a fundamental and instrumental concept for constructing a 3D-printed bioanode.

The effect of the ageing process on the desorption of nonylphenol in black carbon-sediment systems: a kineto-mechanistic and modeling investigation.

Black carbon (BC) exhibits promising potential as a sediment amendment owing to its commendable adsorption capacity for hydrophobic organic contaminants (HOCs), thereby resulting in HOC-laden sediments. Desorption kinetic studies play a crucial role in comprehending the release potential of HOCs from BC-sediment systems. Although the adsorption capacity of BC for HOCs has been found to decrease with aging, there is limited research on its impact on HOC desorption kinetics. In this study, BCs derived from agricultural waste (rice straw carbon, RC) and industrial waste (fly ash carbon, FC), respectively, were used to investigate the desorption kinetics of nonylphenol (NP). Additionally, a predictive model was established using the fitting parameters obtained from the modified two-domain model. The results showed that desorption of NP was divided into three fractions: rapid fraction (Frap), slow fraction (Fslow) and resistant fraction (Fr). BCs significantly decreased, while ageing increased the desorption amount and rate of NP. The performance of RC in controlling NP release was superior to that of FC. The predicted values calculated by the established model exhibit significant positive correlations with the measured values (p < 0.01). Additionally, the correlation analysis between sorption sites and desorption fractions revealed that the concentration of NP in the desorbing fraction was nearly equivalent to that of NP in partition sites within aged sediment/FC-sediment systems. However, the aged RC-sediment systems do not conform well to this rule. In other words, the estimation of NP release risk from sediments with a strong adsorbent would be overestimated, if Frap + Fsolw is considered equivalent to the desorbing fraction.

Photo-Reactivity of dissolved black carbon unveiled by combination of optical spectroscopy and FT-ICR MS analysis: Effects of pyrolysis temperature.

Dissolved black carbon (DBC) has high photoactivity, which plays an important role in contaminants photodegradation. However, it is unclear how pyrolysis temperatures would affect the composition and photo-reactivity of DBC at the molecular level. Herein, we combined complementary techniques to study the characteristics of DBC pyrolyzed at 200 - 500 ℃, as well as the photoproduction of reactive species and the photodegradation of tetracycline (TC). Bulk composition characterization found that condensed aromatic carbonyl compounds (ConAC) with narrow molecular weights in DBC experienced an increase from 200 to 500 °C, which enhanced the photoproduction of 3DBC*,1O2, and ·OH. Molecular-level data suggested that 3DBC* and 1O2 were both related to the same DBC compounds. Comparatively, the patterns for ·OH were less pronounced, implying its precursor was not 3DBC* and had more complexity. Plentiful CHOx species of ConAC in DBC400 and DBC500 (DBCT, where T = pyrolysis temperature) accelerated the generation of 3DBC* and 1O2, enhancing the photodegradation of TC, and mainly triplet states of quinones reacted with TC. In contrast, DBC200 and DBC300 exhibited inhibition since massive CHOx species in lignin-like reduced 3TC* to TC. Our data revealed the diverse photochemical behavior mechanisms of DBC pyrolyzed at 200 - 500 ℃ at the molecular level and the implications for aquatic contaminants photochemistry.

Influence of Polycyclic Aromatic Compounds and Oxidation States of Soot Organics on the Metabolome of Human-Lung Cells (A549): Implications for Vehicle Fuel Selection.

Decades of research have established the toxicity of soot particles resulting from incomplete combustion. However, the unique chemical compounds responsible for adverse health effects have remained uncertain. This study utilized mass spectrometry to analyze the chemical composition of extracted soot organics at three oxidation states, aiming to establish quantitative relationships between potentially toxic chemicals and their impact on human alveolar basal epithelial cells (A549) through metabolomics-based evaluations. Targeted analysis using MS/MS indicated that particles with a medium oxidation state contained the highest total abundance of compounds, particularly oxygen-containing polycyclic aromatic hydrocarbons (OPAHs) composed of fused benzene rings and unsaturated carbonyls, which may cause oxidative stress, characterized by the upregulation of three specific metabolites. Further investigation focused on three specific OPAH standards: 1,4-naphthoquinone, 9-fluorenone, and anthranone. Pathway analysis indicated that exposure to these compounds affected transcriptional functions, the tricarboxylic acid cycle, cell proliferation, and the oxidative stress response. Biodiesel combustion emissions had higher concentrations of PAHs, OPAHs, and nitrogen-containing PAHs (NPAHs) compared with other fuels. Quinones and 9,10-anthraquinone were identified as the dominant compounds within the OPAH category. This knowledge enhances our understanding of the compounds contributing to adverse health effects observed in epidemiological studies and highlights the role of aerosol composition in toxicity.

Carbon black as a colorimetric label for an immunochromatographic test strip for severe fever with thrombocytopenia syndrome virus detection.

To combat the ongoing threat posed by severe fever with thrombocytopenia syndrome virus (SFTSV), especially in underserved areas, there is an urgent need for an affordable and reliable point-of-care diagnostic tool. This study presents a carbon black-based immunochromatographic test strip (CB-ICTS) for the detection of SFTSV, which is both quick and easy to operate. The study optimized the specific steps for carbon black-labeled antibodies, as well as the amount of carbon black and anti-SFTSV antibody used. Under optimal experimental conditions, the linear range and limit of detection of the CB-ICTS were evaluated using different concentrations of SFTSV standard samples. The detection range of the CB-ICTS for SFTSV was found to be 0.1-1000 ng mL-1, with a limit of detection of 100 pg mL-1. The precision and accuracy of the CB-ICTS were assessed by examining spiked healthy human serum samples, which displayed recoveries ranging from 91.58 to 105.4% with a coefficient of variation of less than 11%. This work evaluated the specificity of the CB-ICTS using various biomarkers (CA125, AFP, CA199, CEA, and HCG) and demonstrated that the CB-ICTS is highly specific for detecting SFTSV, suggesting its potential for the early diagnosis of SFTSV. In addition, the study evaluated the CB-ICTS in serum samples from patients with SFTSV, and the results were highly consistent with those detected by the polymerase chain reaction (PCR) method. Overall, this study demonstrates the feasibility and effectiveness of using the CB-ICTS as a reliable point-of-care diagnostic tool for the early detection of SFTSV.

Evolution hydrothermal aging mechanism for Ag/CeO2 catalysts in regeneration of catalytic diesel particulate filter with DFT calculation.

In order to avoid the high cost of existing precious metal catalyst like Pt, Ag/CeO2 was the most promising catalysts for mobile source soot emission control technologies, but there was a clear trade-off between hydrothermal aging resistance and catalytic oxidation performance hindered the application of this catalyst. In order to reveal the hydrothermal aging mechanism of Ag/CeO2 catalysts, the TGA (thermogravimetric analysis) experiments were investigated to reveal the mechanism of Ag modification on catalytic activity of CeO2 catalyst between fresh and hydrothermal aging and were also characterized with the related characterization experiments to in-depth research the lattice morphology and valence changes. The degradation mechanism of Ag/CeO2 catalysts in vapor with high-temperature was also explained and demonstrated based on density functional and molecular thermodynamics theories. The experimental and simulation data showed that the catalytic activity of soot combustion within Ag/CeO2 decreased more significantly after hydrothermal aging than CeO2 due to the less agglomerated, which caused by the decreased in OII/OI and Ce3+/Ce4+ compared with CeO2. As shown in density function theory (DFT) calculation, the decreased surface energy and the increased oxygen vacancy formation energy of the low Mille index surface after Ag modification led to the instability structure and the high catalytic activity. Ag modification also increased the adsorption energy and Gibbs free energy of H2O on the low Miller index surface compared to CeO2, indicating that the desorption temperature of H2O molecules in (1 1 0) and (1 0 0) was higher than (1 1 1) in CeO2 and Ag/CeO2, which led to the migration of (1 1 1) crystal surfaces to (1 1 0) and (1 0 0) in the vapor environment. These conclusions can provide a valuable addition to the regenerative application of Ce-based catalysts in diesel exhaust aftertreatment system the aerial pollution.

Electrospun Ce-Mn oxide as an efficient catalyst for soot combustion: Ce-Mn synergy, soot-catalyst contact, and catalytic oxidation mechanism.

Increasing the contact efficiency and improving the intrinsic activity are two effective strategies to obtain efficient catalysts for soot combustion. Herein, the electrospinning method is used to synthesize fiber-like Ce-Mn oxide with a strong synergistic effect. The slow combustion of PVP in precursors and highly soluble manganese acetate in spinning solution facilitates the formation of fibrous Ce-Mn oxides. The fluid simulation clearly indicates that the slender and uniform fibers provide more interwoven macropores to capture soot particles than the cubes and spheres do. Accordingly, electrospun Ce-Mn oxide exhibits better catalytic activity than reference catalysts, including Ce-Mn oxides by co-precipitation and sol-gel methods. The characterizations suggest that Mn3+ substitution into fluorite-type CeO2 enhances the reducibility through the acceleration of Mn-Ce electron transfer, improves the lattice oxygen mobility by weakening the Ce-O bonds, and induces oxygen vacancies for the activation of O2. The theoretical calculation reveals that the release of lattice oxygen becomes easy because of a low formation energy of oxygen vacancy, while the high reduction potential is beneficial for the activation of O2 on Ce3+-Ov (oxygen vacancies). Due to above Ce-Mn synergy, the CeMnOx-ES shows more active oxygen species and higher oxygen storage capacity than CeO2-ES and MnOx-ES. The theoretical calculation and experimental results suggest that the adsorbed O2 is more active than lattice oxygen and the catalytic oxidation mainly follows the Langmuir-Hinshelwood mechanism. This study indicates that electrospinning is a novel method to obtain efficient Ce-Mn oxide.

Insight into the effect of catalytic reactions on correlations of soot oxidation activity and microspatial structures.

A catalyst is usually coated on Diesel particulate filter (DPF) for assisted regeneration. In this paper, the oxidation activity and pore structure evolutions of soot under the effect of CeO2 are explored. CeO2 effectively increases the oxidation activity of soot and reduces the initial activation energy; in the meantime, the addition of CeO2 changes the soot oxidation mode. Pure soot particles tend to produce the porous structure in the oxidation process. Mesopores promote the diffusion of oxygen, and macropores contribute to reduce the agglomeration of soot particles. Additionally, CeO2 provides the active oxygen for soot oxidation and promotes the multi-point oxidation at the beginning of soot oxidation. With the oxidation proceeding, catalysis causes the collapsion of soot microspatial structures, in the meantime, the macropores caused by the catalytic oxidation are filled by CeO2. It results in the tight contact between soot and catalyst, further promoting the formation of the available active oxygen for soot oxidation. This paper is meaningful to analyze the oxidation mechanism of soot under catalysis, which lays a foundation for improving the regeneration efficiency of DPF and reducing the particle emission.

Photochemical Aging Induces Changes in the Effective Densities, Morphologies, and Optical Properties of Combustion Aerosol Particles.

Effective density (ρeff) is an important property describing particle transportation in the atmosphere and in the human respiratory tract. In this study, the particle size dependency of ρeff was determined for fresh and photochemically aged particles from residential combustion of wood logs and brown coal, as well as from an aerosol standard (CAST) burner. ρeff increased considerably due to photochemical aging, especially for soot agglomerates larger than 100 nm in mobility diameter. The increase depends on the presence of condensable vapors and agglomerate size and can be explained by collapsing of chain-like agglomerates and filling of their voids and formation of secondary coating. The measured and modeled particle optical properties suggest that while light absorption, scattering, and the single-scattering albedo of soot particle increase during photochemical processing, their radiative forcing remains positive until the amount of nonabsorbing coating exceeds approximately 90% of the particle mass.

Surface adsorbed and lattice oxygen activated by the CeO2/Co3O4 interface for enhancive catalytic soot combustion: Experimental and theoretical investigations.

Metal oxide-oxide interface on supported catalyst has been rarely studied due to the complex interfacial structure and synthetic challenge. Herein, different Ag-supported CeO2/Co3O4 samples with various covered-state of CeO2 were prepared for catalytic soot oxidation. In comparison, catalytic activity was significantly improved by grafting CeO2 on Co3O4, in which the best performing Ag/CoCe-2 exhibited remarkable catalytic performance towards soot oxidation with a T50 of 290.5 â„ƒ under 10 % O2/N2. Catalyst characterization investigated by Scanning Electron Microscope (SEM), quasi in-situ X-ray Photoelectron Spectroscopy (XPS), in-situ Raman, etc. revealed that this outstanding promotion in catalytic activity can be principally ascribed to the formation of the CeO2/Co3O4 interface. An appropriate CeO2 dosage maximized the contact and interaction between Co3O4 and CeO2, resulting in the largest CeO2/Co3O4 interface featured with abundant generated superoxide species and activated surface lattice oxygen. Density functional theory (DFT) calculations were also carried out for the oxygen vacancy formation energy, Gibbs free energy, etc. In presence of the CeO2/Co3O4 interface, a charge density redistribution around the adsorbed reactants at oxygen vacancies could be formed, owing to the efficient charge transfer enhanced by the electron-appealing effect. The change in electronic structure favored reducing the oxygen vacancy formation energy and boosting the lattice oxygen activation induced by the hybridized Co-O-Ce bonds, finally lowering the adsorption and activation barriers for reactive species and accelerating the reaction kinetics.

Carbon Black Integrated Polylactic Acid Electrodes Obtained by Fused Deposition Modeling: A Powerful Tool for Sensing of Sulfanilamide Residues in Honey Samples.

Sulfanilamide (SFL) is used to prevent infections in honeybees. However, many regulatory agencies prohibit or establish maximum levels of SFL residues in honey samples. Hence, we developed a low-cost and portable electrochemical method for SFL detection using a disposable device produced through 3D printing technology. In the proposed approach, the working electrode was printed using a conductive filament based on carbon black and polylactic acid and it was associated with square wave voltammetry (SWV). Under optimized SWV parameters, linear concentration ranges (1-10 µmol L-1 and 12.5-35.0 µmol L-1), a detection limit of 0.26 µmol L-1 (0.05 mg L-1), and suitable RSD values (2.4% for inter-electrode; n = 3) were achieved. The developed method was selective in relation to other antibiotics applied in honey samples, requiring only dilution in the electrolyte. The recovery values (85-120%) obtained by SWV were statistically similar (95% confidence level) to those obtained by HPLC, attesting to the accuracy of the analysis and the absence of matrix interference.

Understanding the reaction kinetics of diesel exhaust soot during oxidation process.

The purpose of the present study is to better understand the reaction kinetics of diesel exhaust soot during oxidation process. A thermogravimetric analyzer was used to oxidize real diesel exhaust soot generated from a Euro VI diesel engine under non-isothermal conditions. The Friedman-Reich-Levi method and the Sestak-Berggren model were used to determine the oxidation kinetics. Raman spectroscopy and high-resolution transmission electron microscopy were employed to follow the changes of the soot structure during oxidation. The activation energy gradually increased with increasing conversion level during soot oxidation. The oxidation process of diesel exhaust soot could be described as three-step kinetics, and the calculated conversions fitted the experimental results very well. The kinetic predictions of diesel soot oxidation that were obtained using the proposed kinetic models were more accurate and precise than those with the common first-order model. The structural order increased as oxidation progressed, which was responsible for the increased activation energy. The structural ordering was principally caused by the preferential oxidation of the disordered fraction in the diesel soot, especially for the amorphous carbon, which was oxidized in the initial stage of the oxidation reaction.

Importance of surface charge of soot nanoparticles in determining inhalation toxicity in mice.

Physicochemical properties of nanoparticles are important in regulating nanoparticle toxicity; however, the contribution of nanoparticle charge remains unclear. The objective of this study was to investigate the pulmonary effects of inhalation of charged soot nanoparticles. We established a stably charged nanoparticle generation system for whole-body exposure in BALB/c mice, which produced positively charged, negatively charged, and neutral soot nanoparticles in a wide range of concentrations. After a 7-day exposure, pulmonary toxicity was assessed, together with proteomics analysis. The charged soot nanoparticles on average carried 1.17-1.35 electric charges, and the sizes for nanoparticles under different charging conditions were all fixed at 69 ~ 72 nm. We observed that charged soot nanoparticles induced cytotoxic LDH and increased lung permeability, with the release of 8-isoprostane and caspase-3 and systemic IL-6 in mice, especially for positively charged soot nanoparticles. Next, we observed that positive-charged soot nanoparticles upregulated Eif2, Eif4, sirtuin, mammalian target of rapamycin (mTOR), peroxisome proliferator-activated receptors (PPAR), and HIPPO-related signaling pathways in the lungs compared with negatively charged soot nanoparticles. HIF1α, sirt1, E-cadherin, and Yap were increased in mice's lungs by positively charged soot nanoparticle exposure. In conclusion, carbonaceous nanoparticles carrying electric ions, especially positive-charged, are particularly toxic when inhaled and should be of concern in terms of pulmonary health protection.

Novel insights into the temporal molecular fractionation of dissolved black carbon at the iron oxyhydroxide - water interface.

As the most reactive and mobile fraction of black carbon, dissolved black carbon (DBC) inexorably interacts with minerals in the biosphere. Nevertheless, the research on the mechanisms and compositions of DBC assembly at the mineral-water interface remains limited. In this study, we revealed the "kinetic architecture" of DBC on iron oxyhydroxide at novel insights based on quantitative and qualitative approaches. The results indicated that high molecular weight, highly unsaturated, oxygen-rich (such as carboxyl-rich fraction, phenolics), aliphatics, and long C chains compounds were preferentially adsorbed on the iron oxyhydroxide. 2D-COS analyses directly disclosed the sequential fractionation: aromatic and phenolic groups > aliphatic groups, and few aromatics were continuously adsorbed after the rapid adsorption. Quantitative determinations identified that aromatic and phenolic components were adsorbed rapidly over the first 60 min, while aromatics achieved the dynamic equilibrium until ∼300 min, which was consistent with the 2D-COS observations. Our findings supported the hypothesis that "mineral-OM" and "OM-OM" interactions worked simultaneously, and the adsorption might be co-driven by ligand exchange, hydrophobic interactions, and other mechanisms. This work provided the theoretical basis for organic carbon storage and turnover, and it was valuable for predicting the behaviors and fates of contaminants at the soil-water interface and surface water.

Variations in surface functional groups, carbon chemical state and graphitization degree during thermal deactivation of diesel soot particles.

The thermal deactivation of diesel soot particles exerts a significant influence on the control strategy for the regeneration of diesel particulate filters (DPFs). This work focused on the changes in the surface functional groups, carbon chemical state, and graphitization degree during thermal treatment in an inert gas environment at intermediate temperatures of 600°C, 800°C, and 1000°C and explore the chemical species that were desorbed from the diesel soot surface during thermal treatment using a thermogravimetric analyser coupled with a gas-chromatograph mass spectrometer (TGA-GC/MS). The surface functional groups and carbon chemical state were characterized using Fourier transform infrared spectroscopy (FT-IR) and X-ray photoelectron spectroscopy (XPS). The graphitization degree was evaluated by means of Raman spectroscopy (RS). The concentrations of aliphatic C-H, C-OH, C=O, and O-C=O groups are reduced for diesel soot and carbon black when increasing the thermal treatment temperature, while the sp2/sp3 hybridized ratio and graphitization degree enhance. These results provide comprehensive evidence of the decreased reactivity of soot samples. Among oxygenated functional groups, the percentage reduction during thermal treatment is the largest for the O-C=O groups owing to its worst thermodynamic stability. TGA-GC/MS results show that the aliphatic and aromatic chains and oxygenated species would be desorbed from the soot surface during 1000°C thermal treatment of diesel soot.