The application of a mixture of bentazone(3-isopropyl-1H-2,1,3-benzothiadiazin-4(3H)-one-2,2-dioxide)and atrazine (6-chloro-N2-ethyl-N4-isopropyl-1,3,5-triazine-2,4-diamine)is a practical approach to enhance the herbi...The application of a mixture of bentazone(3-isopropyl-1H-2,1,3-benzothiadiazin-4(3H)-one-2,2-dioxide)and atrazine (6-chloro-N2-ethyl-N4-isopropyl-1,3,5-triazine-2,4-diamine)is a practical approach to enhance the herbicidal effect.Labo- ratory incubation experiments were performed to study the degradation of bentazone and atrazine applied in combination and individually in maize rhizosphere and non-rhizosphere soils.After a lag phase,the degradation of each individual herbicide in the non-autoclaved soil could be adequately described using a first-order kinetic equation.During a 30-d in- cubation,in the autoclaved rhizosphere soil,bentazone and atrazine did not noticeably degrade,but in the non-autoclaved soil,they rapidly degraded in both non-rhizosphere and rhizosphere soils with half-lives of 19.9 and 20.2 d for bentazone and 29.1 and 25.7 d for atrazine,respectively.The rhizosphere effect significantly enhanced the degradation of atrazine, but had no significant effect on bentazone.These results indicated that biological degradation accounted for the degrada- tion of both herbicides in the soil.When compared with the degradation of the herbicide applied alone,the degradation rates of the herbicides applied in combination in the soils were lower and the lag phase increased.With the addition of a surfactant,Tween-20,a reduced lag phase of degradation was observed for both herbicides applied in combination. The degradation rate of bentazone accelerated,whereas that of atrazine remained nearly unchanged.Thus,when these two herbicides were used simultaneously,their persistence in the soil was generally prolonged,and the environmental contamination potential increased.展开更多
The utilization of chelation reaction between metals and tannins is a common tanning method in leather chemistry.Herein,a novel combination tanning mechanism inspired environmentally benign catalyst(CMBT-Fe^(0))was sy...The utilization of chelation reaction between metals and tannins is a common tanning method in leather chemistry.Herein,a novel combination tanning mechanism inspired environmentally benign catalyst(CMBT-Fe^(0))was synthesized by immobilizing Fe nanoparticles onto bayberry tannin(BT)grafted chitosan microfibers(CM).The obtained catalyst featured a well-defined microfibrous structure,on which Fe^(0)nanoparticles were highly dispersed to exhibit exceptional catalytic activity for the degradation of tetracycline(TC).The catalytic activity of CMBT-Fe^(0)was 1.72 times higher than that of the commercial Fe^(0)nanoparticles without immobilization,with 95.03%of TC degraded within 90.0 min.The CMBT-Fe^(0)catalysts were recycled 6 times,with the removal rate of TC maintained at 82.56%.Furthermore,a possible mechanism responsible for the catalytic removal of TC was provided by analyzing the catalytic degradation products via liquid chromatography-mass spectrometry.Therefore,our investigation successfully developed efficient catalysts to address the concerned environmental issue of antibiotic pollution.展开更多
Short-chain chlorinated paraffins（SCCPs） are still controversial candidates for inclusion in the Stockholm Convention.The inherent mixture nature of SCCPs makes it rather difficult to explore their environmental beh...Short-chain chlorinated paraffins（SCCPs） are still controversial candidates for inclusion in the Stockholm Convention.The inherent mixture nature of SCCPs makes it rather difficult to explore their environmental behaviors.A virtual molecule library of 42,720 C10-SCCP congeners covering the full structure spectrum was constructed.We explored the structural effects on the thermodynamic parameters and environmental degradability of C10-SCCPs through semi-empirical quantum chemical calculations.The thermodynamic properties were acquired using the AM1 method,and frontier molecular orbital analysis was carried out to obtain the EHOMO,ELUMO and ELUMO-EHOMO for degradability exploration at the same level.The influence of the chlorination degree（NCl on the relative stability and environmental degradation was elucidated.A novel structural descriptor,μ,was proposed to measure the dispersion of the chlorine atoms within a molecule.There were significant correlations between thermodynamic values and NCl,while the reported NCl-dependent pollution profile of C10-SCCPs in environmental samples was basically consistent with the predicted order of formation stability of C10-SCCP congeners.In addition,isomers with largeμ showed higher relative stability than those with small μ.This could be further verified by the relationship between μ and the reactivity of nucleophilic substitution and · OH attack respectively.The C10-SCCP congeners with less Cl substitution and lower dispersion degree are susceptible to environmental degradation via nucleophilic substitution and hydroxyl radical attack,while direct photolysis of C10-SCCP congeners cannot readily occur due to the large ELUMO-EHOMO values.The chlorination effect and the conclusions were further checked with appropriate density functional theory（DFT） calculations.展开更多
基金the Natural Science Basic Research Plan in Shaanxi Province of China(No.2004K03-G3)the Scientific Research Fund of the Department of Education of Shaanxi ProvinceChina(No.04JK234)
文摘The application of a mixture of bentazone(3-isopropyl-1H-2,1,3-benzothiadiazin-4(3H)-one-2,2-dioxide)and atrazine (6-chloro-N2-ethyl-N4-isopropyl-1,3,5-triazine-2,4-diamine)is a practical approach to enhance the herbicidal effect.Labo- ratory incubation experiments were performed to study the degradation of bentazone and atrazine applied in combination and individually in maize rhizosphere and non-rhizosphere soils.After a lag phase,the degradation of each individual herbicide in the non-autoclaved soil could be adequately described using a first-order kinetic equation.During a 30-d in- cubation,in the autoclaved rhizosphere soil,bentazone and atrazine did not noticeably degrade,but in the non-autoclaved soil,they rapidly degraded in both non-rhizosphere and rhizosphere soils with half-lives of 19.9 and 20.2 d for bentazone and 29.1 and 25.7 d for atrazine,respectively.The rhizosphere effect significantly enhanced the degradation of atrazine, but had no significant effect on bentazone.These results indicated that biological degradation accounted for the degrada- tion of both herbicides in the soil.When compared with the degradation of the herbicide applied alone,the degradation rates of the herbicides applied in combination in the soils were lower and the lag phase increased.With the addition of a surfactant,Tween-20,a reduced lag phase of degradation was observed for both herbicides applied in combination. The degradation rate of bentazone accelerated,whereas that of atrazine remained nearly unchanged.Thus,when these two herbicides were used simultaneously,their persistence in the soil was generally prolonged,and the environmental contamination potential increased.
基金supported by National Key R&D Program of China(2021YFC2103800)the Technical Development Project of Sichuan University(No.22H0798)Fundamental Research Funds for the Central Universities.
文摘The utilization of chelation reaction between metals and tannins is a common tanning method in leather chemistry.Herein,a novel combination tanning mechanism inspired environmentally benign catalyst(CMBT-Fe^(0))was synthesized by immobilizing Fe nanoparticles onto bayberry tannin(BT)grafted chitosan microfibers(CM).The obtained catalyst featured a well-defined microfibrous structure,on which Fe^(0)nanoparticles were highly dispersed to exhibit exceptional catalytic activity for the degradation of tetracycline(TC).The catalytic activity of CMBT-Fe^(0)was 1.72 times higher than that of the commercial Fe^(0)nanoparticles without immobilization,with 95.03%of TC degraded within 90.0 min.The CMBT-Fe^(0)catalysts were recycled 6 times,with the removal rate of TC maintained at 82.56%.Furthermore,a possible mechanism responsible for the catalytic removal of TC was provided by analyzing the catalytic degradation products via liquid chromatography-mass spectrometry.Therefore,our investigation successfully developed efficient catalysts to address the concerned environmental issue of antibiotic pollution.
基金jointly supported by the Chinese Academy of Sciences (Nos. KZCX2-YW-BR-25, XDB14030500 and YSW2013B01)the National High Technology Research and Development Program (863) of China (No. 2013AA065201)
文摘Short-chain chlorinated paraffins（SCCPs） are still controversial candidates for inclusion in the Stockholm Convention.The inherent mixture nature of SCCPs makes it rather difficult to explore their environmental behaviors.A virtual molecule library of 42,720 C10-SCCP congeners covering the full structure spectrum was constructed.We explored the structural effects on the thermodynamic parameters and environmental degradability of C10-SCCPs through semi-empirical quantum chemical calculations.The thermodynamic properties were acquired using the AM1 method,and frontier molecular orbital analysis was carried out to obtain the EHOMO,ELUMO and ELUMO-EHOMO for degradability exploration at the same level.The influence of the chlorination degree（NCl on the relative stability and environmental degradation was elucidated.A novel structural descriptor,μ,was proposed to measure the dispersion of the chlorine atoms within a molecule.There were significant correlations between thermodynamic values and NCl,while the reported NCl-dependent pollution profile of C10-SCCPs in environmental samples was basically consistent with the predicted order of formation stability of C10-SCCP congeners.In addition,isomers with largeμ showed higher relative stability than those with small μ.This could be further verified by the relationship between μ and the reactivity of nucleophilic substitution and · OH attack respectively.The C10-SCCP congeners with less Cl substitution and lower dispersion degree are susceptible to environmental degradation via nucleophilic substitution and hydroxyl radical attack,while direct photolysis of C10-SCCP congeners cannot readily occur due to the large ELUMO-EHOMO values.The chlorination effect and the conclusions were further checked with appropriate density functional theory（DFT） calculations.
