The chemical activation of various precursors is effective for creating additional closed pores in hard carbons for sodium storage.However,the formation mechanism of closed pores under the influence of pore-forming ag...The chemical activation of various precursors is effective for creating additional closed pores in hard carbons for sodium storage.However,the formation mechanism of closed pores under the influence of pore-forming agents is not well understood.Herein,an effective chemical activation followed by a high-temperature self-healing strategy is employed to generate interconnected closed pores in lignin-derived hard carbon(HCs).By systematic experimental design combined with electron paramagnetic res-onance spectroscopy,it can be found that the content of free radicals in the carbon matrix influences the closure of open pores at high temperatures.Excessively high activation temperature(>700 C)leads to a low free radical concentration,making it difficult to achieve self-healing of open pores at high tempera-tures.By activation at 700°C,a balance between pore making and self-healing is achieved in the final hard carbon.A large number of free radicals triggers rapid growth and aggregation of carbon microcrys-tals,blocking pre-formed open micropores and creating additional interconnected closed pores in as-obtained hard carbons.As a result,the optimized carbon anode(LK-700-1300)delivers a high reversible capacity of 330.8 mA h g^(-1) at 0.03 A g^(-1),which is an increase of 86 mA h g^(-1) compared to the pristine lignin-derived carbon anode(L-700-1300),and exhibits a good rate performance(202.1 mA h g^(-1) at 1 A g^(-1)).This work provides a universal and effective guidance for tuning closed pores of hard carbons from otherprecursors.展开更多
The aim of this work is to detect electrogenerated hydroxyl radicals and chlorine by simple and less expensive methods. Preparative electrolyses of perchloric acid (HClO4) and sodium chloride (NaCl) were performed on ...The aim of this work is to detect electrogenerated hydroxyl radicals and chlorine by simple and less expensive methods. Preparative electrolyses of perchloric acid (HClO4) and sodium chloride (NaCl) were performed on a boron-doped diamond (BDD) electrode. The hydroxyl radicals were quantified indirectly by assaying the samples from the HClO4 (0.1 M) electrolysis with a 10−4 M potassium permanganate solution. The investigations showed that the amount of hydroxyl radicals depends on the concentration of HClO4 and the current density. As for chlorine, a qualitative determination was carried out. A mixture of the electrolyte solution of HClO4 (0.1 M) + NaI (0.2 M) + 2 mL of hexane, taken in this order, leads to a purplish-pink coloration attesting to the presence of Cl2. The same test was carried out with NaBr and NaI giving pale and very pale pink colourations, respectively, showing that the intensity of the colouration depends on the strength of the oxidant present. In addition, oxidants were detected during the electrooxidation of metronidazole (MNZ). The results showed the participation of electrogenerated hydroxyl radicals. The generation of chlorine has also been proven. Furthermore, the degradation leads to a chemical oxygen demand (COD) removal rate of 83.48% and the process is diffusion-controlled.展开更多
Background,aim,and scope Environmentally persistent free radicals(EPFRs)have received significant attention due to their longer lifetime and stable existence in various environments.The strong environmental migration ...Background,aim,and scope Environmentally persistent free radicals(EPFRs)have received significant attention due to their longer lifetime and stable existence in various environments.The strong environmental migration ability of particulate matter allows EPFRs to migrate over long-distance transport,thereby impacting the quality of the local atmospheric environment.Additionally,EPFRs can also adhere to atmospheric particles and interact with typical gaseous pollutants to affect atmospheric chemical reactions.EPFRs can produce some reactive organic species,promoting oxidative stress in the human body,damaging biological macromolecules and ultimately affecting the organism health.EPFRs are considered as a novel type of pollutant that affects human health.Despite their significance,there are few literatures available on the characteristics and fate behaviors of EPFRs up to date.Therefore,supplemental reviews are crucial for providing comprehensive understanding of EPFRs.Materials and methods This review summarizes the characteristics of EPFRs in particulate matter,outlines the generation mechanism and influencing factors of EPFRs,and the impacts of EPFRs on environmental quality and organism health.Results The content of EPFRs in particulate matter ranges from 1017 to 1020 spins∙g−1.Due to the strong mobility of atmospheric particulate matter,the long-term exposure to high levels of EPFRs may aggravate the impact of particulate matter on human health.The interaction between EPFRs and typical gaseous pollutants can alter their fate and influence atmospheric chemical reactions.EPFRs are mainly produced by transition metal elements and substituted aromatic hydrocarbons through electron transfer.Additionally,the chemical bond rupture of organic substances through heat treatment or ultraviolet radiation can also produce EPFRs,and heterogeneous reactions are capable producing them as well.The production of EPFRs is not only influenced by transition metal elements and precursors,but also by various environmental factors such as oxygen,temperature,light radiation,and relative humidity.Discussion EPFRs in atmospheric particulates matters are usually rich in fine particulates with obvious seasonal and regional variations.They can easily enter the human respiratory tract and lungs with inhalable particulates,thereby increasing the risk of exposure.Additionally,EPFRs in atmospheric particulates can interact with some typical gaseous pollutants,impacting the life and fate of EPFRs in the atmosphere,and alter atmospheric chemical reactions.Traditionally,EPFRs are generated by transition metal elements and substituted aromatic hydrocarbons undergoing electron transfer in the post-flame and cool-zone regions of combustion systems and other thermal processes to remove HCl,H2O or CO groups,ultimately produce semiquinones,phenoxyls,and cyclopentadienyls.Recent studies have indicated that EPFRs can also be generated under the conditions of without transition metal elemental.Organics can also produce EPFRs through chemical bond rupture during heat treatment or light radiation conditions,as well as through some heterogeneous reactions and photochemical secondary generation of EPFRs.The presence or absence of oxygen has different effects on the type and yield of EPFRs.The concentration,type,and crystal type of transition metal elements will affect the type,content,and atmospheric lifetime of EPFRs.It is generally believed that the impact of transition metal element types on EPFRs is related to the oxidation-reduction potential.The combustion temperature or heat treatment process significantly affects the type and amount of EPFRs.Factors such as precursor loading content,pH conditions,light radiation and relative humidity also influence the generation of EPFRs.EPFRs can interact with pollutants in the environment during their migration and transformation process in environmental medium.This process accelerates the degradation of pollutants and plays a crucial role in the migration and transformation of organic pollutants in environmental media.The reaction process of EPFRs may lead to the production of reactive oxygen species(ROS)such as∙OH,which can induce oxidative stress,inflammation and immune response to biological lung cells and tissues,leading to chronic respiratory and cardiopulmonary dysfunction,cardiovascular damage and neurotoxic effects,ultimately impacting the health of organisms.Conclusions The interaction mechanism between EPFRs in particulate matter and gaseous pollutants remains unclear.Furthermore,research on the generation mechanism of EPFRs without the participation of transition metals is not comprehensive,and the detection of EPFRs is limited to simple qualitative categories and lack accurate qualitative analysis.Recommendations and perspectives Further research should be conducted on the generation mechanism,measurement techniques,migration pathways,and transformation process of EPFRs.It is also important to explore the interaction between EPFRs in atmospheric particulate matter and typical gaseous pollutants.展开更多
Biochar is a well-known material for pollutant removal owing to its low cost and rich surface functionality. A kind of highly active substance, called environmentally persistent free radicals(EPFRs), can be produced i...Biochar is a well-known material for pollutant removal owing to its low cost and rich surface functionality. A kind of highly active substance, called environmentally persistent free radicals(EPFRs), can be produced in the preparation process of biochar, playing an important role in the removal of pollutants.In this study, sludge-derived biochars(SBC_(120) and SBC_(270)) were prepared by the hydrothermal carbonization under two temperatures(120℃ and 270℃) to investigate their removal abilities of Cr(Ⅵ). The maximum removal amounts of Cr(Ⅵ) by SBC_(120) and SBC_(270) were 16.58 and 22.93 mg·g^(-1), respectively. It was further revealed that the appearance of Cr(Ⅲ), as a result of EPFRs on sludge-derived biochar(SBC) transferred electrons to Cr(Ⅵ) in neutral solutions. That is to say, oxygen-centered(O-centered) EPFRs on SBC_(120) and carbon-centered(C-centered) EPFRs on SBC_(270) all could be used as electron donors to Cr(Ⅵ) to make it become Cr(Ⅲ). This study not only provides a theoretical basis for the mechanism of pollutants removal by sludge-derived biochar but also offers a new perspective on the direct effect of EPFRs on pollutants.展开更多
[ Objective ] The research aimed to provide reference for the application of extracts from sweet potato leaves in anti-aging cosmetics. [ Method ] The extraction and storage conditions for free radicals scavenging sub...[ Objective ] The research aimed to provide reference for the application of extracts from sweet potato leaves in anti-aging cosmetics. [ Method ] The extraction and storage conditions for free radicals scavenging substances from sweet potato leaves were optimized by orthogonal test and the bioactive components in extracts were investigated by correlation analysis. [ Result] Sweet potato leaves contain the bioactive substances scavenging DPPH free radical and hydroxyl free radical. Extracting solvent species is the most important factor that influencing extraction yield. The optimal extraction and storage conditions are as following: water as solvent, pH 8.0 of extracting liquid, storage at 25 ℃. There is a good positive linear relationship between the content of total phenols in sweet potato leaves and corresponding scavenging rates against both the DPPH free radical and hydroxyl free radical. For the content of total flavones in sweet potato leaves, just a correlation with scavenging rate against hydroxyl free radical shown in test. [ Conclusion] The phenols in ex- tracts could effectively scavenge both the DPPH free radical and hydroxyl free radical, whereas the flavones in extracts can only function on the hydroxyl free radical.展开更多
Objective To study the abnormal reactions of a series of free radicals and the oxidative damages induced by free radical abnormal reactions in the bodies of patients with chronic glomerulonephritis. Methods Eighty ...Objective To study the abnormal reactions of a series of free radicals and the oxidative damages induced by free radical abnormal reactions in the bodies of patients with chronic glomerulonephritis. Methods Eighty chronic glomerulonephritis patients (CGNP) and eighty healthy adult volunteers (HAV) were enrolled in a random control study, in which concentrations of nitric oxide (NO) in plasma, lipoperoxides (LPO) in plasma and in erythrocytes, and vitamin C (VC), vitamin E (VE) and beta-carotene (?CAR) in plasma as well as activities of superoxide dismutase (SOD), catalase (CAT) and glutathione peroxidase (GPX) in erythrocytes were determined with spectrophotometric assays. Results Compared with the average values of the above biochemical parameters in the HAV group, the average values of NO in plasma, and LPO in plasma and erythrocytes in the CGNP group were significantly increased (P = 0.0001), while those of VC, VE and -CAR in plasma as well as those of SOD, CAT and GPX in erythrocytes in the CGNP group were significantly decreased (P = 0.0001). Pearson product-moment correlation analysis showed that with increase of the concentration of blood creatinine as well as prolongation of the course of disease in the CGNP, the concentrations of NO in plasma, and LPO in plasma and erythrocytes in the CGNP increased gradually, while the concentrations of VC, VE and ?CAR in plasma as well as the activities of SOD, CAT and GPX in erythrocytes in the CGNP decreased gradually (P = 0.002454 0.000001). The relative risk ratio (RR) of the above biochemical parameters reflecting oxidative damages in the bodies of CGNP ranged from 6.061 to 72.429. The reliability coefficient (alpha) that the above biochemical parameters were used to reflect the oxidative damages of the CGNP was 0.8137, standardized item alpha = 0.9728, Hotelling抯 T-Squared = 1135680.191, F = 53274.6478, P = 0.000001. Conclusions The findings in this study show that in the bodies of CGNP a series of free radical chain reactions result in severe pathological aggravation and induce oxidative damages in their bodies. Therefore, suitable dose of antioxidants should be supplemented to them so as to alleviate oxidative damages in their bodies.展开更多
A crude polysaccharide was extracted from Physalis alkekengi L. fruit. HPLC was used for the component analysis of the polysaccharide. The results indicate that Physalis alkekengi L. polysaccharide(PAP) was composed...A crude polysaccharide was extracted from Physalis alkekengi L. fruit. HPLC was used for the component analysis of the polysaccharide. The results indicate that Physalis alkekengi L. polysaccharide(PAP) was composed of rhamnose, xylose, arabinose, galactose, and glucose. Free radicals scavenging activity of PAP was studied through 3 free radicals scavenging tests. PAP exhibited high scavenging effects on OH and DPPH radicals, and both the scavenging rates were about 80%. The scavenging rate of O2^- radical was about 22%.展开更多
Enhancing the chemical reaction processes by means of the energy released in the collapse of micro bubbles or cavities in the cavitation flow is a new research area. In the previous work, a new approach of measuring c...Enhancing the chemical reaction processes by means of the energy released in the collapse of micro bubbles or cavities in the cavitation flow is a new research area. In the previous work, a new approach of measuring concentration of free hydroxyl radicals induced in cavitation flow by using methylene blue as the indicator was developed and used to study concentration of free radical induced in Venturi cavitation flow under various experimental conditions. In the present research, the radial evolution of a cavity bubble and the corresponding collapse pressure in sonic cavitation field are obtained by solving three different bubble dynamics equations: Rayleigh equation, Rayleigh-Plesset equation and Gilmore equation. By comparing with the experimental data on the radial evolution of a cavity bubble in the literature, it is found that the predicted results by the Gilmore equation, which takes account of the compressibility of fluid in addition to the viscosity and interfacial tension, agree with the experimental ones better than those by other two equations. Moreover, the theoretically predicted collapse pressures are consistent with the concentration of the free hydroxyl radical induced in the experimental venture. Thus, the concentration of the liberated free hydroxyl radical not only influences the reaction rate but also is used as an available parameter for measuring collapse intensity of cavities.展开更多
Objective:To explore the nature of deficiency in spleen-yin syndrome,which could provide scientific theoretical support and practical guidance for clinical Traditional Chinese Medicine(TCM)syndrome differentiation ...Objective:To explore the nature of deficiency in spleen-yin syndrome,which could provide scientific theoretical support and practical guidance for clinical Traditional Chinese Medicine(TCM)syndrome differentiation based on biology,and had a strong clinical significance.Methods:Serum Cu and Zn were detected by atomic absorption spectrophotometer,serum vitamin E by high performance liquid chromatography,serum vitamin C by 2,4-Dinitrophenylhydrazine Colorimetry,total superoxide dismutase(SOD)and Cu and Zn- SOD by the xanthine oxidase method,and malondialdehyde(MDA)by the 2-thiobarbituric acid method(TBA).Total antioxidant capacity was detected by a colorimetry kit.Amylase Activity was detected by an automatic biochemical analyzer.Lysozyme was detected by lysozyme detection plate,the diameter of bacteriolysis circle was measured and the corresponding content of lysozyme was obtained from a table of standard curve values.Results: No significant difference in total SOD and Cu,Zn-SOD was found between deficiency in spleen-yin group and normal group.However,such factors in deficiency in kidney-yin group were significantly lower than the other groups(P〈0.05).The MDA content in both deficiency in spleen-yin group and deficiency in kidney-yin group were significantly higher than that of normal group(P〈0.05),while the total antioxidant capacity was significantly lower than normal group(P〈0.05).The vitamin E content in deficiency in kidney-yin group was significantly lower than that in the other two groups(P〈0.05).No significant difference in the contents of vitamin C,Cu and Zn were observed in these groups.The Zn/Cu level in deficiency in kidney-yin group and the vitamin E level in deficiency in spleen-yin group decreased,but with no significant difference.Amylase activity in unit time in cases with deficiency in spleen-yin was lower than and had significant differences with that in normal cases,and higher than that in cases with deficiency in kidney-yin.The sectional velocity of saliva and the ratio of lysozyme in normal case group were significantly higher than other two groups,while deficiency in the spleen-yin group was significantly higher than the deficiency in kidney-yin group.Conclusion:All the results indicated that the objective pathological mechanism between the deficiency in spleen-yin and deficiency in kidney-yin was different.展开更多
A light purple organic active substance capable of scavenging hydroxyl radical(OH) with a high efficiency was extracted from Oyster shell at an extraction rate of 2.49%. It was found for the first time that this act...A light purple organic active substance capable of scavenging hydroxyl radical(OH) with a high efficiency was extracted from Oyster shell at an extraction rate of 2.49%. It was found for the first time that this active substance may scavenge OH with the efficiency far higher than that of vitamin C. This active substance may scavenge also superoxide radical(O2) although the scavenging efficiency is far lower than that of vitamin C. Infrared spectrometry and routine chemical analysis primarily reveal that this active substance belongs to glycoprotein.展开更多
AIM: To investigate the therapeutic effects of resveratrol (RESV) as a free radical scavenger on experimental severe acute pancreatitis (SAP). METHODS: Seventy-two male Sprague-Dawley rats were divided randomly ...AIM: To investigate the therapeutic effects of resveratrol (RESV) as a free radical scavenger on experimental severe acute pancreatitis (SAP). METHODS: Seventy-two male Sprague-Dawley rats were divided randomly into sham operation group, SAP group, and resveratrol-treated group. Pancreatitis was induced by intraductal administration of 0.1 mL/kg 4% sodium taurocholate. RESV was given intravenously at a dose of 20 mg/kg body weight. All animals were killed at 3, 6, 12 h after induction of the model. Serum amylase, pancreatic superoxide dismutase (SOD), malondialdehyde (MDA), and myeloperoxidase (MPO) were determined. Pathologic changes of the pancreas were observed under optical microscope. RESULTS: The serum amylase, pancreatic MPO and the score of pathologic damage increased after the induction of pancreatitis, early (3, 6 h) SAP samples were characterized by decreased pancreatic SOD and increased pancreatic MDA. Resveratrol exhibited a protective effect against lipid peroxidation in cell membrane caused by oxygen free radicals in the early stage of SAP. This attenuation of the redox state impairment reduced cellular oxidative damage, as reflected by lower serum amylase, less severe pancreatic lesions, normal pancreatic MDA levels, as well as diminished neutrophil infiltration in pancreas. CONCLUSION: RESV may exert its therapeutic effect on SAP by lowering pancreatic oxidative free radicals and reducing pancreatic tissue infiltration of neutrophils.展开更多
In recent years,there have been numerous studies on Fenton or Fenton-like reactions mediated by nonfree radicals such as singlet oxygen(1O_(2));however,there are few studies on the synergistic effect of 1O_(2) and fre...In recent years,there have been numerous studies on Fenton or Fenton-like reactions mediated by nonfree radicals such as singlet oxygen(1O_(2));however,there are few studies on the synergistic effect of 1O_(2) and free radicals on the degradation of organic molecules,such as phenol in Fenton reaction.In this study,a cocatalyst,CoP,commonly used in photocatalysis was synthesized using a simple two-step method,and a CoP/Fe^(2+)/AM1.5 system was constructed by introducing Fe^(2+)and simulated sunlight(AM1.5)irradiation.The newly constructed CoP/Fe^(2+)/AM1.5 system could effectively degrade various organic pollutants,including dyes,phenols,and antibiotics.Radical quenching experiments and electron paramagnetic resonance detection confirmed that there were three reactive oxygen species(ROS)in the CoP/Fe^(2+)/AM1.5 system,including·OH_(ads),·O_(2)^(-),and 1O_(2).Further,combined with the liquid chromatogram of phenol,its intermediate products,and the fluorescence diagram of o-hydroxybenzoic acid,it can be concluded that a synergistic effect exists between 1O_(2) and the surface-adsorbed·OH_(ads) in the CoP/Fe^(2+)/AM1.5 system.The controllable formation of surface 1O_(2) and·OH_(ads) was achieved through the oxidation(Co^(3+))and reduction(Pδ−)centers exposed on the CoP surface,and the synergistic effect between them results in phenol’s hydroxylation,ring-opening,and degradation.The study of this new mechanism provides a new perspective for revealing the surface interface reaction between ROS and organic pollutants.展开更多
Purpose:The aim of this study was to investigate the impact of total soy saponins(TS) on the free radical metabolism from the quadriceps femoris muscle,serum testosterone,lactate dehydrogenase(LDH),and blood urea nitr...Purpose:The aim of this study was to investigate the impact of total soy saponins(TS) on the free radical metabolism from the quadriceps femoris muscle,serum testosterone,lactate dehydrogenase(LDH),and blood urea nitrogen(BUN) in rats exercised to exhaustion.Methods:A one-time exhausted treadmill exercise session was used.Sprague-Dawley rats were divided into 4 groups:a control group—animals receiving no TS and no exercise(NTSNE),animals receiving TS but no exercise group(TSNE),animals receiving no TS but exercised to exhaustion group(NTSE),and animals receiving TS and exercised to exhaustion group(TSE).The TSNE and TSE groups were fed TS at a dosage of 20 mg/kg body weight once per day for 2 weeks.The NTSE group was given a placebo,and the NTSNE group was not given any treatment.The NTSE and TSE groups were exercised at speed of 30 m/min on treadmill until exhausted.The exercise time and exercise distance were recorded when the rats became exhausted and the rats were then decapitated and anatomized immediately.A 10% homogenate of the quadriceps femoris tissue was prepared.The levels of superoxide dismutase(SOD),catalase(CAT),malondialdehyde(MDA),glutathione peroxidase(GSH-Px),glutathione reductase(GR),reduced glutathione(GSH),total antioxidant capacity(T-AOC),LDH,BUN,and serum testosterone were tested.Results:TS significantly increased the exercise time to exhaustion by 20.62%(p < 0.05).The MDA levels were decreased significantly in the TSNE group than in NTSNE group(p < 0.05);the T-AOC levels increased significantly in the TSNE group than in the other 3 groups(p < 0.01,p < 0.05,p < 0.05).The LDH activity significantly increased in the NTSE group than in TSNE group(p < 0.05).The BUN levels significantly increased in the NTSE group than in the other 3 groups(p < 0.01,p < 0.01,p < 0.05),and significantly increased in the TSE group than in NTSNE and TSNE groups(both p < 0.01).The serum testosterone levels increased significantly in the TSNE group than in the other 3 groups(all p < 0.01).SOD,CAT,GSH-Px,GR,and GSH were not statistically different among the groups.Conclusion:TS can significantly improve the exercised rats' serum testosterone level and antioxidant activity in their quadriceps femoris to varying degrees,decrease MDA and serum LDH and BUN levels,increase the exercise time,and delay the occurrence of the fatigue.展开更多
As the most abundant source of biomass in nature for sustainable production of fuels and chemicals,efficient depolymerization of cellulose under mild conditions,due to the difficulty in selective cleavage of itsβ-1,4...As the most abundant source of biomass in nature for sustainable production of fuels and chemicals,efficient depolymerization of cellulose under mild conditions,due to the difficulty in selective cleavage of itsβ-1,4-glycosidic bonds,still remains challenging.Here,we report a novel method for oxidative cleavage of the glycosidic bonds by free radicals.Probed by the cellobiose reaction,it was found that·OH radicals,generated from the decomposition of H2O2 catalyzed by CuSO4 or CuO/SiO2,were efficient for selective conversion of cellobiose to glucose and gluconic acid at a low temperature of 333 K,and their selectivities reached 30.0%and 34.6%,respectively,at 23.4%cellobiose conversion.Other radicals,such as·SO4?,also exhibited high efficacy in the cellobiose reaction.Mechanistic studies suggest that the oxidative cleavage of theβ-1,4-glycosidic bond by the free radicals involve formation of the carbon radical intermediate via abstraction of the H atom dominantly at the C1 position.Following this oxidative mechanism,treatment of microcrystalline cellulose with·OH by impregnation with H2O2 and CuSO4 catalyst at 343 K led to significant enhancement in its hydrolysis efficiency.These results demonstrate the effectiveness of this new method in the oxidative cleavage of glycosidic bonds,and its viability for the efficient depolymerization of cellulose at low temperatures,which can be further improved,for example,by exploring new free radicals and optimizing their reactivity and selectivity.展开更多
Lead dioxide electrodes on Ti substrates were prepared by thermal-deposition or electro-deposition. The amount of hydroxyl radicals generated at the electrodes prepared by the above-mentioned two methods was compared ...Lead dioxide electrodes on Ti substrates were prepared by thermal-deposition or electro-deposition. The amount of hydroxyl radicals generated at the electrodes prepared by the above-mentioned two methods was compared with that at the electrodes mingled with Bi or La prepared by electro-deposition. The experimental results indicate that the highest concentration of hydroxyl radicals generated by thermal-deposition, electro-deposition mingled with nothing, electro-deposition mingled with Bi or La was 0.781, 1.048, 1.838 or 2.044 μmol/L, respectively. When phenol was electrolyzed on the four electrodes at a current density of 30 mA/cm2, the removal efficiency of phenol after electrolysis for 1.5 h was 87.30%, 93.55%, 97.95% or 98.70%, TOC removal efficiency after electrolysis for 5 h was 86.76%, 94.26%, 98.53% or 99.60%, respectively. Through the degradation experiments of phenol, the amount of hydroxyl radicals was responsible for the removal efficiency of phenol. The electro-catalytic characteristics were investigated by SEM, the generation amount of hydroxyl radicals, the degradation degree of phenol and the stability and conductivity of the electrodes were also investigated. The experimental results indicate that the four electrodes all show good electro-catalytic characteristics; the electro-catalytic characteristics of the electrode mingled with La were superior to those of the other three ones, and the electrochemical degradation of phenol followed one-step reaction dynamics.展开更多
With the physical method of micro-gap gas discharge, OH. radicals were produced by the ionization of O2 in air and H2O in the gaseous state, in order to explore more effective method totreat the ship's ballast water....With the physical method of micro-gap gas discharge, OH. radicals were produced by the ionization of O2 in air and H2O in the gaseous state, in order to explore more effective method totreat the ship's ballast water. The surface morphology of Al2O3 dielectric layer was analysed using Atomic Force Microscopy (AFM), where the size of Al2O3 particles was in the range of 2 μm to 5 μm. At the same time, the biochemical effect of hydroxyl radicals on the introduced organisms and the quality of ship's ballast water were studied. The results indicate that the main reasons of cell death are lipid peroxide and damage of the antioxidant enzyme system in Catalase (CAT), Peroxidase (POD) and Superoxide dismutase (SOD). In addition, the quality of the ballast water was greatly improved.展开更多
Geothermometer is one of the most useful methods to reconstruct the thermal history of sedimentary basins. This paper introduces the application of free radicals concentration of organic matter as a thermal indicator ...Geothermometer is one of the most useful methods to reconstruct the thermal history of sedimentary basins. This paper introduces the application of free radicals concentration of organic matter as a thermal indicator in the thermal history reconstruction of carbonate succession, based on anhydrous thermal simulation results of type I and H1 kerogen. A series of free radicals data are obtained under thermal simulation of different heating temperatures and times, and quantitative modds between free radical concentration (Ng) of organic matter and time-temperature index (TTI) for types I and type H1 kerogen are also obtained. This Ng.TTI relation was used to model the Ordovician thermal gradients of Well TZ12 in the Tarim Basin. The modeling result is corresponding to the results obtained by apatite fission track data and published data. This new method of thermal history reconstruction will be benefit to the hydrocarbon generation and accumulation study and resource assessment of carbonate succession.展开更多
Materials with function of producing negative ions effection,containing valency-variable rare earth elements and semiconductor oxide,were fabricated.Free radicals produced by the materials were tested.The result shows...Materials with function of producing negative ions effection,containing valency-variable rare earth elements and semiconductor oxide,were fabricated.Free radicals produced by the materials were tested.The result shows that the materials can produce quite a few free radicals as·O^-_2 no matter whether they are under illumination of ultraviolet radiation or under visible light radiation,or under no light radiation, demonstrating semiconductor oxide can be catalysed under the visible light radiation.At the same time the result shows there is direct relation between the number of free radicals and of the negative ion produced by the materials,which meant that during photo-catalyzed and redox process of valency-variable rare earth elements free radicals translate into negative ions. A circular model is presented involving circulating change of valency-variable rare earth elements and water and oxygen absorbed on the surface of materials under the condition of photocatalysis.展开更多
The qualitative and quantitative analyses of reactive oxygen species are essential to determine their steady-state concentration and related reaction mechanisms in environmental aquatic systems. In this study, salicyl...The qualitative and quantitative analyses of reactive oxygen species are essential to determine their steady-state concentration and related reaction mechanisms in environmental aquatic systems. In this study, salicylic acid was employed as an innovative molecular probe of hydroxyl radical(OH) generated in aqueous nitrate and nitrite solutions through photochemical reactions. Kinetic studies showed that the steady-state concentrations of OH in aqueous NO- 3(10 mmol/L, pH=5) and NO- 2(10 mmol/L, pH=5) solutions under ultraviolet irradiation were at a same magnitude, 10 -15 mol/L. Apparent quantum yields of OH at 313 nm were measured as 0.011 and 0.07 for NO- 3 and NO- 2 respectively, all comparable to the results of previous studies.展开更多
基金supported by the National Natural Science Foundation of China (22379157,22179139)the Key Research and Development (R&D) Projects of Shanxi Province(202102040201003)+1 种基金the Research Program of Shanxi Province(202203021211203)the ICC CAS (SCJC-XCL-2023-10 and SCJC-XCL-2023-13)
文摘The chemical activation of various precursors is effective for creating additional closed pores in hard carbons for sodium storage.However,the formation mechanism of closed pores under the influence of pore-forming agents is not well understood.Herein,an effective chemical activation followed by a high-temperature self-healing strategy is employed to generate interconnected closed pores in lignin-derived hard carbon(HCs).By systematic experimental design combined with electron paramagnetic res-onance spectroscopy,it can be found that the content of free radicals in the carbon matrix influences the closure of open pores at high temperatures.Excessively high activation temperature(>700 C)leads to a low free radical concentration,making it difficult to achieve self-healing of open pores at high tempera-tures.By activation at 700°C,a balance between pore making and self-healing is achieved in the final hard carbon.A large number of free radicals triggers rapid growth and aggregation of carbon microcrys-tals,blocking pre-formed open micropores and creating additional interconnected closed pores in as-obtained hard carbons.As a result,the optimized carbon anode(LK-700-1300)delivers a high reversible capacity of 330.8 mA h g^(-1) at 0.03 A g^(-1),which is an increase of 86 mA h g^(-1) compared to the pristine lignin-derived carbon anode(L-700-1300),and exhibits a good rate performance(202.1 mA h g^(-1) at 1 A g^(-1)).This work provides a universal and effective guidance for tuning closed pores of hard carbons from otherprecursors.
文摘The aim of this work is to detect electrogenerated hydroxyl radicals and chlorine by simple and less expensive methods. Preparative electrolyses of perchloric acid (HClO4) and sodium chloride (NaCl) were performed on a boron-doped diamond (BDD) electrode. The hydroxyl radicals were quantified indirectly by assaying the samples from the HClO4 (0.1 M) electrolysis with a 10−4 M potassium permanganate solution. The investigations showed that the amount of hydroxyl radicals depends on the concentration of HClO4 and the current density. As for chlorine, a qualitative determination was carried out. A mixture of the electrolyte solution of HClO4 (0.1 M) + NaI (0.2 M) + 2 mL of hexane, taken in this order, leads to a purplish-pink coloration attesting to the presence of Cl2. The same test was carried out with NaBr and NaI giving pale and very pale pink colourations, respectively, showing that the intensity of the colouration depends on the strength of the oxidant present. In addition, oxidants were detected during the electrooxidation of metronidazole (MNZ). The results showed the participation of electrogenerated hydroxyl radicals. The generation of chlorine has also been proven. Furthermore, the degradation leads to a chemical oxygen demand (COD) removal rate of 83.48% and the process is diffusion-controlled.
文摘Background,aim,and scope Environmentally persistent free radicals(EPFRs)have received significant attention due to their longer lifetime and stable existence in various environments.The strong environmental migration ability of particulate matter allows EPFRs to migrate over long-distance transport,thereby impacting the quality of the local atmospheric environment.Additionally,EPFRs can also adhere to atmospheric particles and interact with typical gaseous pollutants to affect atmospheric chemical reactions.EPFRs can produce some reactive organic species,promoting oxidative stress in the human body,damaging biological macromolecules and ultimately affecting the organism health.EPFRs are considered as a novel type of pollutant that affects human health.Despite their significance,there are few literatures available on the characteristics and fate behaviors of EPFRs up to date.Therefore,supplemental reviews are crucial for providing comprehensive understanding of EPFRs.Materials and methods This review summarizes the characteristics of EPFRs in particulate matter,outlines the generation mechanism and influencing factors of EPFRs,and the impacts of EPFRs on environmental quality and organism health.Results The content of EPFRs in particulate matter ranges from 1017 to 1020 spins∙g−1.Due to the strong mobility of atmospheric particulate matter,the long-term exposure to high levels of EPFRs may aggravate the impact of particulate matter on human health.The interaction between EPFRs and typical gaseous pollutants can alter their fate and influence atmospheric chemical reactions.EPFRs are mainly produced by transition metal elements and substituted aromatic hydrocarbons through electron transfer.Additionally,the chemical bond rupture of organic substances through heat treatment or ultraviolet radiation can also produce EPFRs,and heterogeneous reactions are capable producing them as well.The production of EPFRs is not only influenced by transition metal elements and precursors,but also by various environmental factors such as oxygen,temperature,light radiation,and relative humidity.Discussion EPFRs in atmospheric particulates matters are usually rich in fine particulates with obvious seasonal and regional variations.They can easily enter the human respiratory tract and lungs with inhalable particulates,thereby increasing the risk of exposure.Additionally,EPFRs in atmospheric particulates can interact with some typical gaseous pollutants,impacting the life and fate of EPFRs in the atmosphere,and alter atmospheric chemical reactions.Traditionally,EPFRs are generated by transition metal elements and substituted aromatic hydrocarbons undergoing electron transfer in the post-flame and cool-zone regions of combustion systems and other thermal processes to remove HCl,H2O or CO groups,ultimately produce semiquinones,phenoxyls,and cyclopentadienyls.Recent studies have indicated that EPFRs can also be generated under the conditions of without transition metal elemental.Organics can also produce EPFRs through chemical bond rupture during heat treatment or light radiation conditions,as well as through some heterogeneous reactions and photochemical secondary generation of EPFRs.The presence or absence of oxygen has different effects on the type and yield of EPFRs.The concentration,type,and crystal type of transition metal elements will affect the type,content,and atmospheric lifetime of EPFRs.It is generally believed that the impact of transition metal element types on EPFRs is related to the oxidation-reduction potential.The combustion temperature or heat treatment process significantly affects the type and amount of EPFRs.Factors such as precursor loading content,pH conditions,light radiation and relative humidity also influence the generation of EPFRs.EPFRs can interact with pollutants in the environment during their migration and transformation process in environmental medium.This process accelerates the degradation of pollutants and plays a crucial role in the migration and transformation of organic pollutants in environmental media.The reaction process of EPFRs may lead to the production of reactive oxygen species(ROS)such as∙OH,which can induce oxidative stress,inflammation and immune response to biological lung cells and tissues,leading to chronic respiratory and cardiopulmonary dysfunction,cardiovascular damage and neurotoxic effects,ultimately impacting the health of organisms.Conclusions The interaction mechanism between EPFRs in particulate matter and gaseous pollutants remains unclear.Furthermore,research on the generation mechanism of EPFRs without the participation of transition metals is not comprehensive,and the detection of EPFRs is limited to simple qualitative categories and lack accurate qualitative analysis.Recommendations and perspectives Further research should be conducted on the generation mechanism,measurement techniques,migration pathways,and transformation process of EPFRs.It is also important to explore the interaction between EPFRs in atmospheric particulate matter and typical gaseous pollutants.
基金supported by the Beijing Municipal Natural Science Foundation (8202007)the National Natural Science Foundation of China (52170148)。
文摘Biochar is a well-known material for pollutant removal owing to its low cost and rich surface functionality. A kind of highly active substance, called environmentally persistent free radicals(EPFRs), can be produced in the preparation process of biochar, playing an important role in the removal of pollutants.In this study, sludge-derived biochars(SBC_(120) and SBC_(270)) were prepared by the hydrothermal carbonization under two temperatures(120℃ and 270℃) to investigate their removal abilities of Cr(Ⅵ). The maximum removal amounts of Cr(Ⅵ) by SBC_(120) and SBC_(270) were 16.58 and 22.93 mg·g^(-1), respectively. It was further revealed that the appearance of Cr(Ⅲ), as a result of EPFRs on sludge-derived biochar(SBC) transferred electrons to Cr(Ⅵ) in neutral solutions. That is to say, oxygen-centered(O-centered) EPFRs on SBC_(120) and carbon-centered(C-centered) EPFRs on SBC_(270) all could be used as electron donors to Cr(Ⅵ) to make it become Cr(Ⅲ). This study not only provides a theoretical basis for the mechanism of pollutants removal by sludge-derived biochar but also offers a new perspective on the direct effect of EPFRs on pollutants.
基金Scientific Research Program of Beijing Municipal Commission of Education (KM200710011007)~~
文摘[ Objective ] The research aimed to provide reference for the application of extracts from sweet potato leaves in anti-aging cosmetics. [ Method ] The extraction and storage conditions for free radicals scavenging substances from sweet potato leaves were optimized by orthogonal test and the bioactive components in extracts were investigated by correlation analysis. [ Result] Sweet potato leaves contain the bioactive substances scavenging DPPH free radical and hydroxyl free radical. Extracting solvent species is the most important factor that influencing extraction yield. The optimal extraction and storage conditions are as following: water as solvent, pH 8.0 of extracting liquid, storage at 25 ℃. There is a good positive linear relationship between the content of total phenols in sweet potato leaves and corresponding scavenging rates against both the DPPH free radical and hydroxyl free radical. For the content of total flavones in sweet potato leaves, just a correlation with scavenging rate against hydroxyl free radical shown in test. [ Conclusion] The phenols in ex- tracts could effectively scavenge both the DPPH free radical and hydroxyl free radical, whereas the flavones in extracts can only function on the hydroxyl free radical.
文摘Objective To study the abnormal reactions of a series of free radicals and the oxidative damages induced by free radical abnormal reactions in the bodies of patients with chronic glomerulonephritis. Methods Eighty chronic glomerulonephritis patients (CGNP) and eighty healthy adult volunteers (HAV) were enrolled in a random control study, in which concentrations of nitric oxide (NO) in plasma, lipoperoxides (LPO) in plasma and in erythrocytes, and vitamin C (VC), vitamin E (VE) and beta-carotene (?CAR) in plasma as well as activities of superoxide dismutase (SOD), catalase (CAT) and glutathione peroxidase (GPX) in erythrocytes were determined with spectrophotometric assays. Results Compared with the average values of the above biochemical parameters in the HAV group, the average values of NO in plasma, and LPO in plasma and erythrocytes in the CGNP group were significantly increased (P = 0.0001), while those of VC, VE and -CAR in plasma as well as those of SOD, CAT and GPX in erythrocytes in the CGNP group were significantly decreased (P = 0.0001). Pearson product-moment correlation analysis showed that with increase of the concentration of blood creatinine as well as prolongation of the course of disease in the CGNP, the concentrations of NO in plasma, and LPO in plasma and erythrocytes in the CGNP increased gradually, while the concentrations of VC, VE and ?CAR in plasma as well as the activities of SOD, CAT and GPX in erythrocytes in the CGNP decreased gradually (P = 0.002454 0.000001). The relative risk ratio (RR) of the above biochemical parameters reflecting oxidative damages in the bodies of CGNP ranged from 6.061 to 72.429. The reliability coefficient (alpha) that the above biochemical parameters were used to reflect the oxidative damages of the CGNP was 0.8137, standardized item alpha = 0.9728, Hotelling抯 T-Squared = 1135680.191, F = 53274.6478, P = 0.000001. Conclusions The findings in this study show that in the bodies of CGNP a series of free radical chain reactions result in severe pathological aggravation and induce oxidative damages in their bodies. Therefore, suitable dose of antioxidants should be supplemented to them so as to alleviate oxidative damages in their bodies.
基金Supported by the Science and Technique Foundation of Jilin Province, China(No20020503-2)
文摘A crude polysaccharide was extracted from Physalis alkekengi L. fruit. HPLC was used for the component analysis of the polysaccharide. The results indicate that Physalis alkekengi L. polysaccharide(PAP) was composed of rhamnose, xylose, arabinose, galactose, and glucose. Free radicals scavenging activity of PAP was studied through 3 free radicals scavenging tests. PAP exhibited high scavenging effects on OH and DPPH radicals, and both the scavenging rates were about 80%. The scavenging rate of O2^- radical was about 22%.
基金Supported by the National Natural Science Foundation of China (10472024).
文摘Enhancing the chemical reaction processes by means of the energy released in the collapse of micro bubbles or cavities in the cavitation flow is a new research area. In the previous work, a new approach of measuring concentration of free hydroxyl radicals induced in cavitation flow by using methylene blue as the indicator was developed and used to study concentration of free radical induced in Venturi cavitation flow under various experimental conditions. In the present research, the radial evolution of a cavity bubble and the corresponding collapse pressure in sonic cavitation field are obtained by solving three different bubble dynamics equations: Rayleigh equation, Rayleigh-Plesset equation and Gilmore equation. By comparing with the experimental data on the radial evolution of a cavity bubble in the literature, it is found that the predicted results by the Gilmore equation, which takes account of the compressibility of fluid in addition to the viscosity and interfacial tension, agree with the experimental ones better than those by other two equations. Moreover, the theoretically predicted collapse pressures are consistent with the concentration of the free hydroxyl radical induced in the experimental venture. Thus, the concentration of the liberated free hydroxyl radical not only influences the reaction rate but also is used as an available parameter for measuring collapse intensity of cavities.
文摘Objective:To explore the nature of deficiency in spleen-yin syndrome,which could provide scientific theoretical support and practical guidance for clinical Traditional Chinese Medicine(TCM)syndrome differentiation based on biology,and had a strong clinical significance.Methods:Serum Cu and Zn were detected by atomic absorption spectrophotometer,serum vitamin E by high performance liquid chromatography,serum vitamin C by 2,4-Dinitrophenylhydrazine Colorimetry,total superoxide dismutase(SOD)and Cu and Zn- SOD by the xanthine oxidase method,and malondialdehyde(MDA)by the 2-thiobarbituric acid method(TBA).Total antioxidant capacity was detected by a colorimetry kit.Amylase Activity was detected by an automatic biochemical analyzer.Lysozyme was detected by lysozyme detection plate,the diameter of bacteriolysis circle was measured and the corresponding content of lysozyme was obtained from a table of standard curve values.Results: No significant difference in total SOD and Cu,Zn-SOD was found between deficiency in spleen-yin group and normal group.However,such factors in deficiency in kidney-yin group were significantly lower than the other groups(P〈0.05).The MDA content in both deficiency in spleen-yin group and deficiency in kidney-yin group were significantly higher than that of normal group(P〈0.05),while the total antioxidant capacity was significantly lower than normal group(P〈0.05).The vitamin E content in deficiency in kidney-yin group was significantly lower than that in the other two groups(P〈0.05).No significant difference in the contents of vitamin C,Cu and Zn were observed in these groups.The Zn/Cu level in deficiency in kidney-yin group and the vitamin E level in deficiency in spleen-yin group decreased,but with no significant difference.Amylase activity in unit time in cases with deficiency in spleen-yin was lower than and had significant differences with that in normal cases,and higher than that in cases with deficiency in kidney-yin.The sectional velocity of saliva and the ratio of lysozyme in normal case group were significantly higher than other two groups,while deficiency in the spleen-yin group was significantly higher than the deficiency in kidney-yin group.Conclusion:All the results indicated that the objective pathological mechanism between the deficiency in spleen-yin and deficiency in kidney-yin was different.
基金Supported by the Natural Science Foundation of Fujian Province, China(NoC0510029)the Specialized Foundation for Creative Team of Young and Middle-aged Teachers of Jimei University, China(No2006A003)
文摘A light purple organic active substance capable of scavenging hydroxyl radical(OH) with a high efficiency was extracted from Oyster shell at an extraction rate of 2.49%. It was found for the first time that this active substance may scavenge OH with the efficiency far higher than that of vitamin C. This active substance may scavenge also superoxide radical(O2) although the scavenging efficiency is far lower than that of vitamin C. Infrared spectrometry and routine chemical analysis primarily reveal that this active substance belongs to glycoprotein.
文摘AIM: To investigate the therapeutic effects of resveratrol (RESV) as a free radical scavenger on experimental severe acute pancreatitis (SAP). METHODS: Seventy-two male Sprague-Dawley rats were divided randomly into sham operation group, SAP group, and resveratrol-treated group. Pancreatitis was induced by intraductal administration of 0.1 mL/kg 4% sodium taurocholate. RESV was given intravenously at a dose of 20 mg/kg body weight. All animals were killed at 3, 6, 12 h after induction of the model. Serum amylase, pancreatic superoxide dismutase (SOD), malondialdehyde (MDA), and myeloperoxidase (MPO) were determined. Pathologic changes of the pancreas were observed under optical microscope. RESULTS: The serum amylase, pancreatic MPO and the score of pathologic damage increased after the induction of pancreatitis, early (3, 6 h) SAP samples were characterized by decreased pancreatic SOD and increased pancreatic MDA. Resveratrol exhibited a protective effect against lipid peroxidation in cell membrane caused by oxygen free radicals in the early stage of SAP. This attenuation of the redox state impairment reduced cellular oxidative damage, as reflected by lower serum amylase, less severe pancreatic lesions, normal pancreatic MDA levels, as well as diminished neutrophil infiltration in pancreas. CONCLUSION: RESV may exert its therapeutic effect on SAP by lowering pancreatic oxidative free radicals and reducing pancreatic tissue infiltration of neutrophils.
文摘In recent years,there have been numerous studies on Fenton or Fenton-like reactions mediated by nonfree radicals such as singlet oxygen(1O_(2));however,there are few studies on the synergistic effect of 1O_(2) and free radicals on the degradation of organic molecules,such as phenol in Fenton reaction.In this study,a cocatalyst,CoP,commonly used in photocatalysis was synthesized using a simple two-step method,and a CoP/Fe^(2+)/AM1.5 system was constructed by introducing Fe^(2+)and simulated sunlight(AM1.5)irradiation.The newly constructed CoP/Fe^(2+)/AM1.5 system could effectively degrade various organic pollutants,including dyes,phenols,and antibiotics.Radical quenching experiments and electron paramagnetic resonance detection confirmed that there were three reactive oxygen species(ROS)in the CoP/Fe^(2+)/AM1.5 system,including·OH_(ads),·O_(2)^(-),and 1O_(2).Further,combined with the liquid chromatogram of phenol,its intermediate products,and the fluorescence diagram of o-hydroxybenzoic acid,it can be concluded that a synergistic effect exists between 1O_(2) and the surface-adsorbed·OH_(ads) in the CoP/Fe^(2+)/AM1.5 system.The controllable formation of surface 1O_(2) and·OH_(ads) was achieved through the oxidation(Co^(3+))and reduction(Pδ−)centers exposed on the CoP surface,and the synergistic effect between them results in phenol’s hydroxylation,ring-opening,and degradation.The study of this new mechanism provides a new perspective for revealing the surface interface reaction between ROS and organic pollutants.
基金supported by the National Natural Science Foundation of China(No.11101354)
文摘Purpose:The aim of this study was to investigate the impact of total soy saponins(TS) on the free radical metabolism from the quadriceps femoris muscle,serum testosterone,lactate dehydrogenase(LDH),and blood urea nitrogen(BUN) in rats exercised to exhaustion.Methods:A one-time exhausted treadmill exercise session was used.Sprague-Dawley rats were divided into 4 groups:a control group—animals receiving no TS and no exercise(NTSNE),animals receiving TS but no exercise group(TSNE),animals receiving no TS but exercised to exhaustion group(NTSE),and animals receiving TS and exercised to exhaustion group(TSE).The TSNE and TSE groups were fed TS at a dosage of 20 mg/kg body weight once per day for 2 weeks.The NTSE group was given a placebo,and the NTSNE group was not given any treatment.The NTSE and TSE groups were exercised at speed of 30 m/min on treadmill until exhausted.The exercise time and exercise distance were recorded when the rats became exhausted and the rats were then decapitated and anatomized immediately.A 10% homogenate of the quadriceps femoris tissue was prepared.The levels of superoxide dismutase(SOD),catalase(CAT),malondialdehyde(MDA),glutathione peroxidase(GSH-Px),glutathione reductase(GR),reduced glutathione(GSH),total antioxidant capacity(T-AOC),LDH,BUN,and serum testosterone were tested.Results:TS significantly increased the exercise time to exhaustion by 20.62%(p < 0.05).The MDA levels were decreased significantly in the TSNE group than in NTSNE group(p < 0.05);the T-AOC levels increased significantly in the TSNE group than in the other 3 groups(p < 0.01,p < 0.05,p < 0.05).The LDH activity significantly increased in the NTSE group than in TSNE group(p < 0.05).The BUN levels significantly increased in the NTSE group than in the other 3 groups(p < 0.01,p < 0.01,p < 0.05),and significantly increased in the TSE group than in NTSNE and TSNE groups(both p < 0.01).The serum testosterone levels increased significantly in the TSNE group than in the other 3 groups(all p < 0.01).SOD,CAT,GSH-Px,GR,and GSH were not statistically different among the groups.Conclusion:TS can significantly improve the exercised rats' serum testosterone level and antioxidant activity in their quadriceps femoris to varying degrees,decrease MDA and serum LDH and BUN levels,increase the exercise time,and delay the occurrence of the fatigue.
文摘As the most abundant source of biomass in nature for sustainable production of fuels and chemicals,efficient depolymerization of cellulose under mild conditions,due to the difficulty in selective cleavage of itsβ-1,4-glycosidic bonds,still remains challenging.Here,we report a novel method for oxidative cleavage of the glycosidic bonds by free radicals.Probed by the cellobiose reaction,it was found that·OH radicals,generated from the decomposition of H2O2 catalyzed by CuSO4 or CuO/SiO2,were efficient for selective conversion of cellobiose to glucose and gluconic acid at a low temperature of 333 K,and their selectivities reached 30.0%and 34.6%,respectively,at 23.4%cellobiose conversion.Other radicals,such as·SO4?,also exhibited high efficacy in the cellobiose reaction.Mechanistic studies suggest that the oxidative cleavage of theβ-1,4-glycosidic bond by the free radicals involve formation of the carbon radical intermediate via abstraction of the H atom dominantly at the C1 position.Following this oxidative mechanism,treatment of microcrystalline cellulose with·OH by impregnation with H2O2 and CuSO4 catalyst at 343 K led to significant enhancement in its hydrolysis efficiency.These results demonstrate the effectiveness of this new method in the oxidative cleavage of glycosidic bonds,and its viability for the efficient depolymerization of cellulose at low temperatures,which can be further improved,for example,by exploring new free radicals and optimizing their reactivity and selectivity.
基金the Environment Bureau of Jilin Province, China(No.2006-11)Scientific Institute of Changchun City(No. 2007KZ15)985 Project of Jilin University
文摘Lead dioxide electrodes on Ti substrates were prepared by thermal-deposition or electro-deposition. The amount of hydroxyl radicals generated at the electrodes prepared by the above-mentioned two methods was compared with that at the electrodes mingled with Bi or La prepared by electro-deposition. The experimental results indicate that the highest concentration of hydroxyl radicals generated by thermal-deposition, electro-deposition mingled with nothing, electro-deposition mingled with Bi or La was 0.781, 1.048, 1.838 or 2.044 μmol/L, respectively. When phenol was electrolyzed on the four electrodes at a current density of 30 mA/cm2, the removal efficiency of phenol after electrolysis for 1.5 h was 87.30%, 93.55%, 97.95% or 98.70%, TOC removal efficiency after electrolysis for 5 h was 86.76%, 94.26%, 98.53% or 99.60%, respectively. Through the degradation experiments of phenol, the amount of hydroxyl radicals was responsible for the removal efficiency of phenol. The electro-catalytic characteristics were investigated by SEM, the generation amount of hydroxyl radicals, the degradation degree of phenol and the stability and conductivity of the electrodes were also investigated. The experimental results indicate that the four electrodes all show good electro-catalytic characteristics; the electro-catalytic characteristics of the electrode mingled with La were superior to those of the other three ones, and the electrochemical degradation of phenol followed one-step reaction dynamics.
基金supported by the Key Project of National Support Plan from Science and Technology Ministry of China (2006BAC11B06) the Key Project of International Cooperation from the Ministry of Science and Technology of China (2005DFA20800)+1 种基金the Support Plan of National New Century Excellent Youth of China (NCET-04-0286, -05-0398) the Project of National Natural Science Foundation of China (No. 60371035)
文摘With the physical method of micro-gap gas discharge, OH. radicals were produced by the ionization of O2 in air and H2O in the gaseous state, in order to explore more effective method totreat the ship's ballast water. The surface morphology of Al2O3 dielectric layer was analysed using Atomic Force Microscopy (AFM), where the size of Al2O3 particles was in the range of 2 μm to 5 μm. At the same time, the biochemical effect of hydroxyl radicals on the introduced organisms and the quality of ship's ballast water were studied. The results indicate that the main reasons of cell death are lipid peroxide and damage of the antioxidant enzyme system in Catalase (CAT), Peroxidase (POD) and Superoxide dismutase (SOD). In addition, the quality of the ballast water was greatly improved.
基金This work is funded by the National Natural Science Foundation of China (Grant 40472066)the National Major Fundamental Research and Development Project (Nos. 2005CB422102 and 1999043302).
文摘Geothermometer is one of the most useful methods to reconstruct the thermal history of sedimentary basins. This paper introduces the application of free radicals concentration of organic matter as a thermal indicator in the thermal history reconstruction of carbonate succession, based on anhydrous thermal simulation results of type I and H1 kerogen. A series of free radicals data are obtained under thermal simulation of different heating temperatures and times, and quantitative modds between free radical concentration (Ng) of organic matter and time-temperature index (TTI) for types I and type H1 kerogen are also obtained. This Ng.TTI relation was used to model the Ordovician thermal gradients of Well TZ12 in the Tarim Basin. The modeling result is corresponding to the results obtained by apatite fission track data and published data. This new method of thermal history reconstruction will be benefit to the hydrocarbon generation and accumulation study and resource assessment of carbonate succession.
文摘Materials with function of producing negative ions effection,containing valency-variable rare earth elements and semiconductor oxide,were fabricated.Free radicals produced by the materials were tested.The result shows that the materials can produce quite a few free radicals as·O^-_2 no matter whether they are under illumination of ultraviolet radiation or under visible light radiation,or under no light radiation, demonstrating semiconductor oxide can be catalysed under the visible light radiation.At the same time the result shows there is direct relation between the number of free radicals and of the negative ion produced by the materials,which meant that during photo-catalyzed and redox process of valency-variable rare earth elements free radicals translate into negative ions. A circular model is presented involving circulating change of valency-variable rare earth elements and water and oxygen absorbed on the surface of materials under the condition of photocatalysis.
文摘The qualitative and quantitative analyses of reactive oxygen species are essential to determine their steady-state concentration and related reaction mechanisms in environmental aquatic systems. In this study, salicylic acid was employed as an innovative molecular probe of hydroxyl radical(OH) generated in aqueous nitrate and nitrite solutions through photochemical reactions. Kinetic studies showed that the steady-state concentrations of OH in aqueous NO- 3(10 mmol/L, pH=5) and NO- 2(10 mmol/L, pH=5) solutions under ultraviolet irradiation were at a same magnitude, 10 -15 mol/L. Apparent quantum yields of OH at 313 nm were measured as 0.011 and 0.07 for NO- 3 and NO- 2 respectively, all comparable to the results of previous studies.