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1.
J Am Chem Soc ; 142(6): 3060-3068, 2020 Feb 12.
Article in English | MEDLINE | ID: mdl-31965789

ABSTRACT

Charge carrier recombination plays a vital role in the CH3NH3PbI3 perovskite solar cell. By investigating a possible synergy between ion migration and charge carrier recombination, we demonstrate that the nonradiative recombination accelerates by an order of magnitude during iodide migration. The migration induces lattice distortion that brings electrons and holes close to each other and increases their electrostatic interactions. The wave function localization in the same spatial region, and the enhanced lattice and iodide movements increase the nonadiabatic coupling. At the same time, quantum coherence lasts longer, because electron and hole energy levels become correlated. All these factors greatly increase the recombination rate. Moreover, the energy level of the iodide vacancy created during the migration moves from inside the conduction band in the equilibrated structure into the band gap, acting as a typical efficient nonradiative charge recombination center. Our work shows that the different dynamic processes are strongly correlated in halide perovskites and demonstrates that defects, considered to be benign, can become very detrimental under non-equilibrium conditions. The reported results strongly suggest that ion migration should be avoided in halide perovskites, both for its own reasons, such as the large current-voltage hysteresis, and because it greatly accelerates charge carrier losses.

2.
Nano Lett ; 19(9): 6078-6086, 2019 Sep 11.
Article in English | MEDLINE | ID: mdl-31434484

ABSTRACT

Two-dimensional transition metal dichalcogenides (TMDs) draw strong interest in materials science, with applications in optoelectronics and many other fields. Good performance requires high carrier concentrations and long lifetimes. However, high concentrations accelerate energy exchange between charged particles by Auger-type processes, especially in TMDs where many-body interactions are strong, thus facilitating carrier trapping. We report time-resolved optical pump-THz probe measurements of carrier lifetimes as a function of carrier density. Surprisingly, the lifetime reduction with increased density is very weak. It decreases only by 20% when we increase the pump fluence 100 times. This unexpected feature of the Auger process is rationalized by our time-domain ab initio simulations. The simulations show that phonon-driven trapping competes successfully with the Auger process. On the one hand, trap states are relatively close to band edges, and phonons accommodate efficiently the electronic energy during the trapping. On the other hand, trap states localize around defects, and the overlap of trapped and free carriers is small, decreasing carrier-carrier interactions. At low carrier densities, phonons provide the main charge trapping mechanism, decreasing carrier lifetimes compared to defect-free samples. At high carrier densities, phonons suppress Auger processes and lower the dependence of the trapping rate on carrier density. Our results provide theoretical insights into the diverse roles played by phonons and Auger processes in TMDs and generate guidelines for defect engineering to improve device performance at high carrier densities.

3.
Wei Sheng Yan Jiu ; 49(6): 1002-1007, 2020 Nov.
Article in Zh | MEDLINE | ID: mdl-33413763

ABSTRACT

OBJECTIVE: To evaluate the present situation of sodium and iodine content and the correlation in pre-packaged foods in the market. METHODS: After collecting samples from physical and online supermarkets, the contents of sodium and iodine of samples were detected by inductively coupled plasma mass spectrometry, SPSS 26. 0 was applied to analyze the correlation between sodium and iodine and the utilization rate of iodized salt was calculated in pre-packaged foods. RESULTS: Among various types of pre-packaged foods, fish, poultry, meat and egg products sodium(M=884 mg/100 g), iodine(M=40. 5 µg/100 g), preserved foods sodium(M=940 mg/100 g), iodine(M=40. 5 µg/100 g), animal foods sodium(M=786 mg/100 g), iodine(M=34. 9 µg/100 g) were all high in sodium and iodine content. The correlation coefficient of sodium and iodine content in staple and instant foods of animal foods was 0. 730(P<0. 01) and vegetable foods was 0. 777(P<0. 01), the preserved foods of animal foods was 0. 518(P<0. 01) and vegetable foods was 0. 973(P<0. 01). The utilization rate of iodized salt in pre-packaged foods was 88. 46% after removing those samples that could cause the iodine loss, such as baked foods. CONCLUSION: The sodium and iodine content in pre-packaged foods vary with different categories.


Subject(s)
Iodine , Sodium, Dietary , Food Labeling , Food, Preserved , Sodium/analysis , Sodium Chloride, Dietary
4.
Nano Lett ; 18(6): 4008-4014, 2018 06 13.
Article in English | MEDLINE | ID: mdl-29772904

ABSTRACT

Two-dimensional transition metal dichalcogenides (TMDs) have drawn strong attention due to their unique properties and diverse applications. However, TMD performance depends strongly on material quality and defect morphology. Experiments show that samples grown by chemical vapor deposition (CVD) outperform those obtained by physical vapor deposition (PVD). Experiments also show that CVD samples exhibit vacancy defects, while antisite defects are frequently observed in PVD samples. Our time-domain ab initio study demonstrates that both antisites and vacancies accelerate trapping and nonradiative recombination of charge carriers, but antisites are much more detrimental than vacancies. Antisites create deep traps for both electrons and holes, reducing energy gaps for recombination, while vacancies trap primarily holes. Antisites also perturb band-edge states, creating significant overlap with the trap states. In comparison, vacancy defects overlap much less with the band-edge states. Finally, antisites can create pairs of electron and hole traps close to the Fermi energy, allowing trapping by thermal activation from the ground state and strongly contributing to charge scattering. As a result, antisites accelerate charge recombination by more than a factor of 8, while vacancies enhance the recombination by less than a factor of 2. Our simulations demonstrate a general principle that missing atoms are significantly more benign than misplaced atoms, such as antisites and adatoms. The study rationalizes the existing experimental data, provides theoretical insights into the diverse behavior of different classes of defects, and generates guidelines for defect engineering to achieve high-performance electronic, optoelectronic, and solar-cell devices.

5.
J Am Chem Soc ; 140(46): 15753-15763, 2018 Nov 21.
Article in English | MEDLINE | ID: mdl-30362747

ABSTRACT

Advances in perovskite solar cells require development of means to control and eliminate the nonradiative charge recombination pathway. Using ab initio nonadiabatic molecular dynamics, we demonstrate that charge recombination in perovskites is extremely sensitive to the charge state of the halogen vacancy. A missing iodine anion in MAPbI3 has almost no effect on charge losses. However, when the vacancy is reduced, the recombination is accelerated by up to 2 orders of magnitude. The acceleration occurs due to formation of a deep hole trap in the singly reduced vacancy, and both deep and shallow hole traps for the doubly reduced vacancy. The shallow hole involves a significant rearrangement of the Pb-I lattice, leading to a new chemical species: a Pb-Pb dimer bound by the vacancy charge, and under-coordinated iodine bonds. Hole trapping by the singly reduced iodide vacancy operates parallel to recombination of free electron and hole, accelerating charge losses by a factor of 5. The doubly reduced vacancy acts by a sequential mechanism-free hole, to shallow trap, to deep trap, to free electron, and accelerates the recombination by a factor of 50. The study demonstrates that iodine anion vacancy can be beneficial to the performance, because it causes minor changes to the charge carrier lifetime, while increasing charge carrier concentration. However, the neutral iodine and iodine cation vacancies should be strongly avoided. The detailed insights into the charge carrier trapping and relaxation mechanisms provided by the simulation are essential for development of efficient photocatalytic, photovoltaic, optoelectronic and related devices.

6.
Nano Lett ; 17(12): 7962-7967, 2017 12 13.
Article in English | MEDLINE | ID: mdl-29172545

ABSTRACT

Two-dimensional transition metal dichalcogenides (TMDs) have appeared on the horizon of materials science and solid-state physics due to their unique properties and diverse applications. TMD performance depends strongly on material quality and defect morphology. Calculations predict that sulfur adatom and vacancy are among the most energetically favorable defects in MoS2 with vacancies frequently observed during chemical vapor deposition. By performing ab initio quantum dynamics calculations we demonstrate that both adatom and vacancy accelerate nonradiative charge carrier recombination but this happens through different mechanisms. Surprisingly, holes never significantly populate the shallow trap state created by the sulfur adatom because the trap is strongly localized and decoupled from free charges. Charge recombination bypasses the hole trap. Instead, it occurs directly between free electron and hole. The recombination is faster than in pristine MoS2 because the adatom strongly perturbs the MoS2 layer, breaks its symmetry, and allows more phonon modes to couple to the electronic subsystem. In contrast, the sulfur vacancy accelerates charge recombination by the traditional mechanism involving charge trapping, followed by recombination. This is because the hole and electron traps created by the vacancy are much less localized than the hole trap created by the adatom. Because the sulfur adatom accelerates charge recombination by a factor of 7.9, compared to 1.7 due to vacancy, sulfur adatoms should be strongly avoided. The generated insights highlight the diverse behavior of different types of defects, reveal unexpected features, and provide the mechanistic understanding of charge dynamics needed for tailoring TMD properties and building high-performance devices.

7.
Nano Lett ; 17(7): 4038-4046, 2017 07 12.
Article in English | MEDLINE | ID: mdl-28586230

ABSTRACT

To realize the full potential of transition metal dichalcogenides interfaced with bulk semiconductors for solar energy applications, fast photoinduced charge separation, and slow electron-hole recombination are needed. Using a combination of time-domain density functional theory with nonadiabatic molecular dynamics, we demonstrate that the key features of the electron transfer (ET), energy relaxation and electron-hole recombination in a MoS2-TiO2 system are governed by the weak van der Waals interfacial interaction and interface polarization. Electric fields formed at the interface allow charge separation to happen already during the photoexcitation process. Those electrons that still reside inside MoS2, transfer into TiO2 slowly and by the nonadiabatic mechanism, due to weak donor-acceptor coupling. The ET time depends on excitation energy, because the TiO2 state density grows with energy, increasing the nonadiabatic transfer rate, and because MoS2 sulfur atoms start to contribute to the photoexcited state at higher energies, increasing the coupling. The ET is slower than electron-phonon energy relaxation because the donor-acceptor coupling is weak, rationalizing the experimentally observed injection of primarily hot electrons. The weak van der Waals MoS2-TiO2 interaction ensures a long-lived charge separated state and a short electron-hole coherence time. The injection is promoted primarily by phonons within the 200-800 cm-1 range. Higher frequency modes are particularly important for the electron-hole recombinations, because they are able to accept large amounts of electronic energy. The predicted time scales for the forward and backward ET, and energy relaxation can be measured by time-resolved spectroscopies. The reported simulations generate a detailed time-domain atomistic description of the complex interplay of the charge and energy transfer processes at the MoS2/TiO2 interface that are of fundamental importance to photovoltaic and photocatalytic applications. The results suggest that even though the photogenerated charge-separated state is long-lived, the slower charge separation, compared to the electron-phonon energy relaxation, can present problems in practical applications.

8.
Int J Mol Sci ; 19(6)2018 Jun 05.
Article in English | MEDLINE | ID: mdl-29874795

ABSTRACT

Cervical cancer is a common gynecological malignancy with high incidence and mortality. Drugs commonly used in chemotherapy are often accompanied by strong side-effects. To find an anti-cervical cancer drug with high effects and low toxicity, luteoloside was used to treat the cervical cancer cell line Hela to investigate its effects on cell morphology, proliferation, apoptosis, and related proteins. The study demonstrated that luteoloside could inhibit proliferation remarkably; promote apoptosis and cytochrome C release; decrease the mitochondrial membrane potential and reactive oxygen species level; upregulate the expression of Fas, Bax, p53, phospho-p38, phospho-JNK, and cleaved PARP; downregulate the expression of Bcl-2 and phospho-mTOR; activate caspase-3 and caspase-8; change the nuclear morphology, and fragmentate DNA in Hela cells. These results strongly suggest that luteoloside can significantly inhibit the proliferation and trigger apoptosis in Hela cells. In contrast, luteoloside had less proliferation inhibiting effects on the normal cell lines HUVEC12 and LO2, and minor apoptosis promoting effects on HUVEC12 cells. Furthermore, the luteoloside-induced apoptosis in Hela cells is mediated by both intrinsic and extrinsic pathways and the effects of luteoloside may be regulated by the mitogen-activated protein kinases and mTOR signaling pathways via p53.


Subject(s)
Apoptosis/drug effects , Cell Proliferation/drug effects , Glucosides/administration & dosage , Luteolin/administration & dosage , Uterine Cervical Neoplasms/drug therapy , Female , HeLa Cells , Human Umbilical Vein Endothelial Cells , Humans , MAP Kinase Kinase 1/genetics , Membrane Potential, Mitochondrial/drug effects , Reactive Oxygen Species/metabolism , Signal Transduction/drug effects , TOR Serine-Threonine Kinases/genetics , Tumor Suppressor Protein p53/genetics , Uterine Cervical Neoplasms/genetics , Uterine Cervical Neoplasms/pathology
9.
J Am Chem Soc ; 139(19): 6707-6717, 2017 05 17.
Article in English | MEDLINE | ID: mdl-28445637

ABSTRACT

Ultrafast charge recombination in hematite (α-Fe2O3) severely limits its applications in solar energy conversion and utilization, for instance, in photoelectrochemical water splitting. We report the first time-domain ab initio study of charge relaxation dynamics in α-Fe2O3 with and without the oxygen vacancy (Ov) defect, using non-adiabatic molecular dynamics implemented within time-dependent density functional theory. The simulations show that the hole trapping is the rate-limiting step in the electron-hole recombination process for both neutral and ionized Ov systems. The electron trapping is fast, and the trapped electron are relatively long-lived. A similar asymmetry is found for the relaxation of free charge carriers: relaxation of photoholes in the valence band is slower than relaxation of photoelectrons in the conduction band. The slower dynamics of holes offers an advantage to water oxidation at α-Fe2O3 photoanodes. Notably, the neutral Ov defect accelerates significantly the charge recombination rate, by about a factor of 30 compared to the ideal lattice, due to the stronger electron-vibrational coupling at the defect. However, the recombination rate in the ionized Ov defect is decreased by a factor of 10 with respect to the neutral defect, likely due to expansion of the local iron shell around the Ov site. The Ov defect ionization in α-Fe2O3 photoanodes is important for increasing both electrical conductivity and charge carrier lifetimes. The simulations reproduce well the time scales for the hot carrier cooling, trapping and recombination available from transient spectroscopy experiments, and suggest two alternative mechanisms for the Ov-assisted electron-hole recombination. The study provides a detailed atomistic understanding of carrier dynamics in hematite, and rationalizes the experimentally reported activation of α-Fe2O3 photoanodes by incorporation of Ov defects.

10.
Electrophoresis ; 36(9-10): 1186-95, 2015 May.
Article in English | MEDLINE | ID: mdl-25781419

ABSTRACT

Matrix effect (ME) is commonly seen in electrophoretic separation, but this phenomenon lacks any systematic study. Our work aimed to find out the relationship between separation efficiency and current, and then figure out an effective, simple, and economic solution to overcome the negative impact of ME. This present study showed that small amount of NaCl (≤0.005 mg/mL) in the sample had no impact on the separation but enhanced the sensitivity. However, when concentration of NaCl increased above 0.005 mg/mL, it alleviated the separation efficiency, sensitivity, and migration time. Besides, increasing NaCl concentration resulted in increasing turning point. The study of relationship of current and NaCl concentration indicated that when the TP of a sample is higher than 62.36 µA, desalination is necessary. Since the reported desalination methods are either expensive or complicated, we developed a simple and economic method by simply adding 12 times (volume) of chloroform/methanol (2:1, v/v) into the sample. When applied this method to turtle jelly, the number of theoretical plate (N) of 20 amino acids got up to threefold enhancement.


Subject(s)
Amino Acids/analysis , Chromatography, Micellar Electrokinetic Capillary/methods , Meat Products/analysis , Turtles , Animal Shells/chemistry , Animals , Reproducibility of Results , Sensitivity and Specificity
11.
J Agric Food Chem ; 71(28): 10830-10840, 2023 Jul 19.
Article in English | MEDLINE | ID: mdl-37401810

ABSTRACT

Bigeye tuna (BET, Thunnus obesus) is one of the most nutritious and luxurious cosmopolitan fish. The cooked BET products are capturing the interests of consumers by enhancing flavor and ensuring microbiological safety; however, the lipidomic fingerprints during daily cooking processes have not been investigated. In this work, lipid phenotypic data variation in BET during air-frying, roasting, and boiling was studied comprehensively using iKnife rapid evaporative ionization mass spectrometry (REIMS). The outstanding lipid ions mainly including fatty acids (FAs) and phospholipids (PLs) were identified structurally. It was demonstrated that the rates of heat transfer and lipid oxidation in air-fried BET were slower than those in roasted and boiled BET by elucidating the lipid oxidation and PL hydrolysis mechanism. Furthermore, multivariate REIMS data analysis (e.g., discriminant analysis, support vector machine, neutral network, and machine learning models) was used to characterize the lipid profile change in different cooked BET samples, among which FAC22:6, PL18:3/22:6, PL18:1/22:6, and others were the salient contributing features for determining the cooked BET samples. These results may provide a potential strategy for a healthy diet by controlling and improving functional food quality in daily cooking.


Subject(s)
Phospholipids , Tuna , Animals , Mass Spectrometry , Fishes , Cooking
12.
Luminescence ; 26(6): 592-7, 2011.
Article in English | MEDLINE | ID: mdl-21374792

ABSTRACT

A novel method was developed using capillary electrophoresis (CE) coupled with tris(2,2'-bipyridyl)ruthenium(II) electrogenerated chemiluminescence (ECL) for highly sensitive detection of metformin hydrochloride (MH) derivatizatized with acetaldehyde. The precolumn derivatization of MH with acetaldehyde was performed in phosphate buffer solution (0.3 mol/L, pH 7.5) at room temperature for 120 min. The effects of acetaldehyde concentration, buffer pH, electrokinetic voltage and injection time were investigated. Under optimized detection conditions, the MH ECL detection sensitivity was more than 120 times that without derivatization. The linear concentration range for MH was 0.001-15.00 µg/mL (with a correlation coefficient of 0.9992). The detection limit was 0.31 ng/mL with a signal:noise ratio of 3. The recoveries of MH in human urine were in the range 98.50-99.72%. Copyright © 2011 John Wiley & Sons, Ltd.


Subject(s)
Acetaldehyde/chemistry , Electrophoresis, Capillary/methods , Hypoglycemic Agents/analysis , Metformin/analysis , Humans , Hydrogen-Ion Concentration , Limit of Detection , Luminescence , Male , Middle Aged , Reproducibility of Results
13.
Food Chem ; 354: 129565, 2021 Aug 30.
Article in English | MEDLINE | ID: mdl-33756323

ABSTRACT

Polyunsaturated phospholipids are abundant in clam (Corbicula fluminea) but difficult to be fully extracted. Herein, graphene/fibrous silica (G/KCC-1) nanohybrids were synthesized, characterized, and applied for solid-phase extraction (SPE) of phospholipids in clam. The effectiveness of G/KCC-1 SPE was verified by hydrophilic interaction chromatography mass spectrometry (HILIC-MS) based lipidomics and statistical analysis. The ions of PE 16:0/18:1 (m/z 716.4), PC 16:0/20:5 (m/z 824.6) and etc. were regarded as the main difference among the crude lipids, acetone washed extract, and eluate of G/KCC-1 SPE. Finally, this method was validated in terms of linearity (R2 0.9965 to 0.9981), sensitivity (LOD 0.19-0.51 µg·mL-1 and LOQ 0.48 - 1.47 µg·mL-1), and precision (RSDintra-day ≤ 7.16% and RSDinter-day ≤ 7.30%). In conclusion, the G/KCC-1 SPE and HILIC-MS method was shown to be accurate and efficient in selective extracting and phenotyping phospholipids in C. fluminea.


Subject(s)
Chromatography, Liquid , Corbicula/metabolism , Graphite/chemistry , Lipidomics/methods , Mass Spectrometry , Silicon Dioxide/chemistry , Solid Phase Extraction , Animals , Hydrophobic and Hydrophilic Interactions , Phenotype , Seafood/analysis
14.
Food Chem ; 334: 127558, 2021 Jan 01.
Article in English | MEDLINE | ID: mdl-32711269

ABSTRACT

Shellfishes contain plasmalogens correlating to the functions of brain, heart, etc. Herein, a mild acid hydrolysis and hydrophilic interaction chromatography (HILIC) tandem mass spectrometry method was developed for analyzing plasmalogens in six shellfish species. A total of 19 plasmalogen molecular species were successfully identified, including nine phosphatidylcholine plasmalogen (plasPC), seven phosphatidylethanolamine plasmalogen (plasPE), and three phosphatidylserine plasmalogen (plasPS). The quantitative results indicated that mussel (32 µg·mg-1) possessed the highest content of plasmalogens, followed by oyster (21 µg·mg-1) and razor clam (15 µg·mg-1). The statistic models showed that the plasPE P-18:0/20:5 (m/z 748), plasPE P-16:0/22:2 & P-18:0/20:2 (m/z 754) and plasPS were the most contributing difference between shellfishes. The results indicated that this method was sensitive and precise to determine plasmalogens in shellfish, and mussel was demonstrated to be a good choice for the large-scale preparation of plasmalogens.


Subject(s)
Bivalvia/chemistry , Chromatography/methods , Plasmalogens/analysis , Shellfish/analysis , Tandem Mass Spectrometry/methods , Animals , Food Analysis/methods , Hydrophobic and Hydrophilic Interactions , Lipidomics/methods , Ostrea/chemistry , Phosphatidylcholines/analysis , Phosphatidylserines/analysis , Plasmalogens/chemistry
15.
J Sep Sci ; 33(15): 2356-60, 2010 Aug.
Article in English | MEDLINE | ID: mdl-20680932

ABSTRACT

A novel method for the determination of galanthamine (GAL) in Bulbus Lycoridis Radiatae has been developed based on coupling CE with an end-column tris(2,2'-bipyridyl)ruthenium(II) electrochemiluminescence (ECL). Parameters affecting CE separation and ECL detection were investigated and optimized. Baseline separation of GAL from other components in the Bulbus Lycoridis Radiatae sample was achieved with an 18 mmol/L phosphate running buffer at pH 9.0. Under the optimized conditions: 12 kV CE-separation voltage, ECL detection potential at 1.25 V with 5 mmol/L Ru(bpy)(3)(2+) and 50 mmol/L phosphate buffer at pH 7.5 in the detection reservoir, the linear range of GAL concentration was from 0.8 ng/mL to 2 microg/mL, whereas the detection limit was 0.25 ng/mL (S/N=3). The proposed method was successfully demonstrated for the determination of GAL in Bulbus Lycoridis Radiatae.


Subject(s)
Drugs, Chinese Herbal/chemistry , Electrophoresis, Capillary , Galantamine/analysis , Luminescent Measurements/methods , Plant Roots/chemistry , Medicine, Chinese Traditional
16.
J Chem Theory Comput ; 16(4): 2053-2064, 2020 Apr 14.
Article in English | MEDLINE | ID: mdl-32119549

ABSTRACT

Nonadiabatic Molecular Dynamics (NAMD) of excited states has been widely used in the simulation of photoinduced phenomena. However, the inability to treat bond breaking and forming processes with single-reference electronic structure methods limits their application in photochemistry for extended molecular systems. In this work, the extension of excited-state NAMD for open-shell systems is developed and implemented in the NEXMD software. We present the spin-unrestricted CIS and TD-SCF formalism for the ground and excited states, analytical derivatives, and nonadiabatic derivative couplings for the respective potential energy surfaces. This methodology is employed to study the photochemical reaction of three model molecules. The results demonstrate the advantage of the open-shell approach in modeling photochemical reactions, especially involving bond breaking processes. We find that the open-shell method lowers the reaction barrier at the bond-breaking limits resulting in larger calculated photochemical quantum yields compared to the respective closed-shell results. We also address problems related to spin contamination in the open-shell method, especially when molecular geometries are far from equilibrium.

17.
J Agric Food Chem ; 68(7): 2240-2248, 2020 Feb 19.
Article in English | MEDLINE | ID: mdl-31975589

ABSTRACT

An electric soldering iron ion source (ESII) coupling with rapid evaporative ionization mass spectrometry (REIMS) was developed and used for in situ monitoring the dynamic variation trend in oxidation characteristics of fish oil during storage. The lipidomics profiles of fish oil stored at various days were acquired by ESII-REIMS. The fatty acid and triacylglycerol species were structurally identified, and their abundances were analyzed according to multivariate statistical models mainly including principle component analysis as well as orthogonal partial least-squares analysis. On the shared and unique structure plot, the ions of m/z 255.23, 281.24, 877.72, and 901.72 displayed the most significant variation among the oxidized fish oil samples. Based on receiver operating characteristic curve analysis with an optimal Youden index of 0.91, these markers were further verified. The variation of viscosity and volatiles were also evaluated to further verify the oxidation characteristics of fish oil. The study demonstrated that ESII-REIMS technology used as an advanced detection method could ensure fish oil quality during storage.


Subject(s)
Fish Oils/chemistry , Lipidomics/methods , Mass Spectrometry/methods , Fatty Acids/chemistry , Food Storage , Mass Spectrometry/instrumentation , Oxidation-Reduction , Triglycerides/chemistry , Viscosity
18.
J Phys Chem Lett ; 10(11): 2676-2683, 2019 Jun 06.
Article in English | MEDLINE | ID: mdl-31066278

ABSTRACT

Oxygen vacancies in TiO2 nanoparticles are important for charge carrier dynamics, with recent studies reporting contradictory results on TiO2 nanoparticle photocatalytic activity. We demonstrate that ground state multiplicity, defect levels, and formation energies depend strongly on vacancy location. Quantum dynamics simulations show that charges are trapped within several picoseconds and recombine over a broad range of time scales from tens of picoseconds to nanoseconds. Specifically, nanoparticles with missing partially coordinated surface oxygens showed fast recombination, while nanoparticles with missing highly coordinated subsurface oxygens or singly coordinated oxygens at tips showed slow recombination, even slower than in the pristine system. The results are rationalized by energy gaps and electron-hole localization, the latter determining nonadiabatic coupling and quantum coherence time. The diverse charge recombination scenarios revealed by the nonadiabatic dynamics simulations rationalize the contradictory experimental results for photocatalytic activity and provide guidelines for rational design of nanoscale metal oxides for solar energy harvesting and utilization.

19.
J Pharm Biomed Anal ; 48(4): 1249-53, 2008 Dec 01.
Article in English | MEDLINE | ID: mdl-18976877

ABSTRACT

A novel and sensitive method for the determination of amoxicillin (AM) in human urine has been established using capillary electrophoresis (CE) coupled with electrochemiluminescence (ECL) detection, based on the ECL enhancement of Tris(2,2'-bipyridyl) ruthenium(II) with AM. The effects of several factors such as the detection potential, the concentration and the pH of phosphate buffer, the electrokinetic voltage and the injection time were investigated. Under the optimal conditions, the linear concentration of AM ranged from 1.0 ng/ml to 8.0 microg/ml (with a correlation coefficient of 0.9999). The limit of detection was 0.31 ng/ml. The mean recovery was 95.77% with relative standard deviations of no larger than 2.2%. This method is quick (the total run time within 6 min). This method has been successfully applied to a pharmacokinetic study in human urine after oral administration of AM.


Subject(s)
Amoxicillin/pharmacokinetics , Amoxicillin/urine , Anti-Bacterial Agents/pharmacokinetics , Anti-Bacterial Agents/urine , Electrophoresis, Capillary/methods , Luminescent Measurements/methods , Online Systems , 2,2'-Dipyridyl/chemistry , Buffers , Calibration , Electrochemistry , Humans , Hydrogen-Ion Concentration , Indicators and Reagents/chemistry , Phosphates/chemistry , Reproducibility of Results , Ruthenium/chemistry
20.
Article in English | MEDLINE | ID: mdl-29107730

ABSTRACT

Plastron is a nutritive and superior functional food. Due to its limited supply yet enormous demands, some functional foods supposed to contain plastron may be forged with other substitutes. This paper reports a novel and simple method for determination of the authenticity of plastron-derived functional foods based on comparison of the amino acid (AA) profiles of plastron and its possible substitutes. By applying micellar electrokinetic chromatography (MEKC), 18 common AAs along with another 2 special AAs - hydroxyproline (Hyp) and hydroxylysine (Hyl) were detected in all plastron samples. Since chicken, egg, fish, milk, pork, nail and hair lacked of Hyp and Hyl, plastron could be easily distinguished. For those containing collagen, a statistical analysis technique - principal component analysis (PCA) was adopted and plastron was successfully distinguished. When applied the proposed method to authenticate turtle shell glue in the market, fake products were commonly found.


Subject(s)
Amino Acids/analysis , Chromatography, Micellar Electrokinetic Capillary/methods , Functional Food/analysis , Tissue Extracts/analysis , Tissue Extracts/chemistry , Animals , Chickens , Functional Food/classification , Hair/chemistry , Humans , Limit of Detection , Linear Models , Meat/analysis , Milk/chemistry , Nails/chemistry , Ovum/chemistry , Reproducibility of Results , Swine
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