Petroporphyrins were enriched and purified from atmospheric residues of two typical heavy oils, Canadian oil sand bitumen (OSAR, Ni: 80 ppm, V: 190 ppm, S: 3.97 wt%) and Chinese Liaohe heavy oil (LHAR, Ni: 68.7 ppm, V: 1.81 ppm, S: 0.36 wt%) by silica gel chromatography. The separation and purification were confirmed by atomic absorption spectroscopy (AAS) combined with UV-vis spectroscopy, and the petroporphyrins were characterized by positive-ion electrospray ionization (ESI) Fourier transform-ion cyclotron resonance mass spectrometry (FT-ICR MS). Vanadyl and nickel porphyrins in OSAR are simultaneously identified by mass measurement and isotopic fine structure. Vanadyl porphyrins with structures of N 4 VO, N 4 VO 2 and N 4 VOS are all detected as protonated analyte ([M+H] + ). Both molecular ion (M +• ) and analyte ([M+H] + ) as well as their corresponding isotopes are observed for N 4 Ni porphyrins in OSAR and LHAR with an average mass resolving power of over 400 000 (m/∆m 50% ). This is rarely detected by FT-ICR MS using ESI technique previously. Formation of molecular ion can be attributed to the low oxidation potential of nickel porphyrins, effect of oil matrix on the solution conductivity and the relatively low flow rate of solution into the capillary. Three more highly unsaturated types of N 4 VO porphyrins were identified in addition to the six well-documented structures. Compared to N 4 VO porphyrins, N 4 VOS porphyrins present higher DBE ranging from 21 to 27 while N 4 VO 2 porphyrins show lower DBE ranging from 18 to 20 and narrower carbon number distribution, suggesting possible different origins of sulfur (pyrolysis of kerogen) and oxygen (diagenesis of chlorophyills). Ni/V and ratio of relative abundance of ETIO porphyrins to DPEP porphyrins (∑ETIO/∑DPEP) for nickel porphyrins indicate that Liaohe oil and Canadian oil sand bitumen are continental and marine sediment, respectively, and Liaohe oil has a higher maturity.Enrichment by the simple chromatographic method facilitates the mass spectral identification of nickel porphyrins even for heavy residue with low content of nickel and high content of sulfur.
This review highlights the currently exploited working concepts of lab-on-a-molecule probes, with a particular focus on what is required for multianalyte detection and quantification in competitive assays. Both, chemosensor and chemodosimeter approaches are considered. The multifaceted design strategies and the orthogonal protocols are evaluated in order to identify and categorise the successful conceptions and to single out unknown territory and challenges for future work.
Hospital-acquired
infections are a serious threat to the recovery
of patients. To prevent such infections, an antibacterial coating
is an effective method to eliminate bacterial colonization on healthcare-related
surfaces. Herein, we report an antibacterial hydrogel composed of
silver-containing polyoxometalate (AgP5W30 POM)
and carboxymethyl chitosan (CMC). The silver ion is encapsulated inside
the POM cage and demonstrates long-lasting bacteriostasis after repeated
exposure to both Gram-positive and Gram-negative bacteria. The chemical
structure of chitosan derivatives, as well as the concentration and
pH, is studied to tune the mechanical properties of the hydrogel.
The hydrogel undergoes a gel–sol transition above the critical
temperature and possesses self-healing ability. This hydrogel can
be readily coated on the surface of versatile bulk materials, which
is especially convenient for porous objects and resists the growth
of Staphylococcus aureus, Escherichia coli, and methicillin-resistant S. aureus (MRSA). In summary, we envision that the
AgP5W30-CMC hydrogel has great potential to
serve as an antibacterial coating to decrease the prevalence of hospital-acquired
infections.
Direct three-colour fluorescence cross-correlation spectroscopy can reveal interactions between three fluorescently labelled biomolecules, giving insight toward the complex events that constitute signal transduction pathways. Here we provide the optical and theoretical basis for this technology and demonstrate its ability to detect specific biological associations between nanoparticle-labelled DNA molecules.
An immunoassay based on surface enhanced Raman scattering (SERS) spectroscopy was developed to detect muramidase released protein (MRP) antibody against Streptococcus suis II (SS2) utilizing thorny gold nanoparticles (tAuNPs) as SERS substrates. Initially, tAuNPs with multi-branches were prepared by the seed-mediated growth method in the absence of templates and surfactants, facilitating p-mercaptobenzoic acid (pMBA) conjugation covalently onto the tAuNPs through S-Au bonds. The obtained immuno-SERS tag affording strong Raman signals made it possible to establish an application of indirect detection of the MRP antibody against SS2 with a sandwich assay at a highly sensitive level. The Raman intensity at 1588 cm(-1) was proportional to the logarithm of the concentration of MRP antibody in the range of 10 pg mL(-1) to 0.1 μg mL(-1). The detection sensitivity was significantly improved to 0.1 pg mL(-1) by using the immuno-SERS tags. Furthermore, the proposed SERS approach was applied to detect MRP antibody in pig serum samples, and the results agreed well with those of ELISA, indicating great potential for clinical application in diagnostic immunoassays.
The characterization and antioxidant activity on Maillard reaction products (MRPs) derived from xylose and bovine casein hydrolysate (BCH) was investigated at 100 °C and initial pH 8.0 as a function of reaction time. The pH values and free amino groups contents of xylose–BCH MRPs remarkably decreased with the reaction time up to 8 h, whereas their browning intensities significantly increased (p < 0.05). After 4 h of heat treatment, the fluorescence properties of xylose–BCH MRPs reached the maximum. There was a production of higher and smaller molecular substances in xylose–BCH MRPs with an increased reaction time, as analyzed by size exclusion chromatography. The 2,2-diphenyl-1-picryl-hydrazyl (DPPH) free radical scavenging capacity and ferrous reducing activity of xylose-BCH MRPs gradually increased with the reaction time extended from 0 to 8 h.
With access to the solution structures of nanocomposites of coordination nanocages (CNCs) via scattering and chromatography techniques, their mysterious solution dynamics have been, for the first time, resolved, and interestingly, the surface macromolecules can be substituted by extra free macromolecules in solutions. Obvious exchange of macromolecules can be observed in the solution mixtures of CNC nanocomposites at high temperatures, revising the understanding of the dynamics of CNC nanocomposites. Being distinct from nanocomposites of a simple coordination complex, the quantified solution dynamics of CNC nanocomposites indicates a typical logarithmic time dependence with the dissociation of surface macromolecules as the thermodynamically limiting step, suggesting strongly coupled and hierarchically constrained dynamics among the surface macromolecules. Their dynamics can be activated only upon application of high temperature or selected solvents, and therefore, the rational design of polymer assemblies, for example, hybrid-arm star polymers with precisely controlled compositions and reprocessable, robust CNC-cross-linked supramolecular polymer networks, is facilitated.
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