Tetracyclines constitute one of the most important antibiotic families and represent a classic example of phototoxicity. The photoproducts of tetracyclines and their parent compounds have potentially adverse effects o...Tetracyclines constitute one of the most important antibiotic families and represent a classic example of phototoxicity. The photoproducts of tetracyclines and their parent compounds have potentially adverse effects on natural ecosystem. In this study, the self-sensitized oxidation products of tetracycline (TC) and oxytetracycline (OTC) were determined and the effects of Ca2+ and Mg2+on self-sensitized degradation were investigated. The Ca2+ and Mg2+ in the natural water sample accounted for enhancement (pH 7.3) and inhibition (pH 9.0) of photodegradation of TC and OTC due to the formation of metal-ions complexes. The formation of Mg2+ complexes was unfavorable for the photodegradation of the tetracyclines at both pH values. In contrast, the Ca2+ complexes facilitated the attack of singlet oxygen (102) arising from self-sensitization at pH 7.3 and enhanced TC photodegradation. For the first time, self- sensitized oxidation products of TC and OTC were verified by quenching experiments and detected by LC/ESI-DAD-MS. The products had a nominal mass 14 Da higher than the parent drugs (designated M+ 14), which resulted from the 102 attack of the dimethylamino group on the C-4 atom of the tetracyclines. The presence of Ca2+ and Mg2+ also affected the generation of M+ 14 due to the formation of metal-ions complexes with TC and OTC. The findings suggest that the metal-ion complexation has significant impact on the self- sensitized oxidation processes and the photoproducts of tetracyclines.展开更多
The aqueous photodegradation of the widely used antibiotic chlortetracycline(CTC) was investigated under simulated sunlight.The quantum yield of photodegradation increased from 3.3 × 10-4 to 8.5 × 10-3 wit...The aqueous photodegradation of the widely used antibiotic chlortetracycline(CTC) was investigated under simulated sunlight.The quantum yield of photodegradation increased from 3.3 × 10-4 to 8.5 × 10-3 within the pH range of 6.0 to 9.0.The presence of Ca2+,Fe3+,and NO3-enhanced the photodegradation of CTC,whereas Mg2+,Mn2+,and Zn2+ inhibited the degradation with the order Mn2+ Zn2+ Mg2+ at pH 7.3.The monovalent cations(Na+ and K+) had negligible effect on the photolysis of CTC.Fulvic acid(FA) decreased the photodegradation of CTC due to light screening effect.Hydrogen peroxide(H2O2) was formed concurrently with direct photodegradation of CTC.The generation rate of H2O2 increased from 0.027 to 0.086 μmol/(L.min) when the pH ranged from 6.0 to 9.0.The CTC solution was about three-fold more toxic to the Photobacterium phosphoreum bacteria after irradiation,suggesting that the photoproducts and H2O2 formed in the CTC solution exhibited high risk on the bacteria.By LC-ESI(+)-MS,the photoproducts of CTC were identified.The direct photodegradation of CTC was involved in hydroxylation and N-demethyl/dedismethyl processes.The main photoproducts included the iso-CTC analog containing hydroxyl groups(m/z 511.4 and 495.4),and the N-demethyl/dedismethyl products of the photoproduct m/z 495.4(m/z 481.3 and 467.4).In addition,the photochemical dechlorination of CTC led to tetracycline(m/z 445.5).展开更多
The sunlight photodegradation half-lives of 20 mg/L acetochlor were 151, 154 and 169 days in de-ionized water, river water and paddy water, respectively. When exposed to ultraviolet (UV) light, acetochlor in aqueous s...The sunlight photodegradation half-lives of 20 mg/L acetochlor were 151, 154 and 169 days in de-ionized water, river water and paddy water, respectively. When exposed to ultraviolet (UV) light, acetochlor in aqueous solution was rapidly degraded. The half-lives were 7.1, 10.1, and 11.5 min in de-ionized water, river water and paddy water, respectively. Photoproducts of acetochlor were identified by gas chromatography/mass spectrometry(GC/MS) and found at least twelve photoproducts resulted from dechlorination with subsequent hydroxylation and cyclization processes. The chemical structures of ten photoproducts were presumed on the basis of mass spectrum interpretation and literature data. Photoproducts are identified as 2-ethyl-6-methylaniline; N,N-diethylaniline; 4,8-dimethyl-2-oxo-1,2,3,4- tetrahydroquino-line; 2-oxo-N-(2-ethyl-6-methylphenyl)-N-(ethoxymethyl)acetamide; N-(ethoxymethyl)-2′-ethyl-6′-methylformanilide;1-hydroxyacetyl-2-ethoxyl-7-ethylind ole; 8-ethyl-1-ethoxymethyl-2-oxo-1,2,3,4-tetrahydroquinoline; 4,8-dimethyl-1-ethoxymethyl-2-oxo-1,2,3,4-tetrahydroquinoline; 2-hydroxy-2′-ethyl-6′-methyl-N-(ethoxymethyl)acetanilide and a compound related to acetochlor. The other two photoproducts were detected by GC/MS although their chemical structure was unknown.展开更多
The hydrolysis and photolysis of clomazone in aqueous solutions and natural water were assessed under natural and controlled conditions. Kinetics of hydrolysis and photolysis of clomazone were determined by HPLC-DAD. ...The hydrolysis and photolysis of clomazone in aqueous solutions and natural water were assessed under natural and controlled conditions. Kinetics of hydrolysis and photolysis of clomazone were determined by HPLC-DAD. Photoproducts were identiifed by HPLC-MS. No noticeable hydrolysis occurred in aqueous buffer solutions ((25±2)°C, pH (4.5±0.1), pH (7.4±0.1), pH (9.0±0.1);(50±2)°C, pH (4.5±0.1), pH (7.4±0.1)) or in natural water up to 90 d. At pH (9.0±0.1) and (50±2)°C the half-life of clomazone was 50.2 d. Clomazone photodecomposition rate in aqueous solutions under UV radiation and natural sunlight followed ifrst-order kinetics. Degradation rates were faster under UV light (half-life of 51-59 min) compared to sunlight (half-life of 87-136 d). Under UV light, four major photoproducts were detected and tentatively identiifed according to HPLC-MS spectral information such as 2-chlorobenzamide, N-hydroxy-(2-benzyl)-2-methylpropan-amide, 2-[2-phenol]-4,4-dimethyl-3-isoxazolidinone and 2-[(4,6-dihydroxyl-2-chlorine phenol)]-4,4-dimethyl-3-isoxazolidinone. These results suggested that clomazone photodegradation proceeds via several reaction pathways:1) dehalogenation;2) substitution of chlorine group by hydroxyl;3) cleavage of the side chain. Photosensitizers, such as H2O2 and ribolfavin, could enhance photolysis of clomazone in natural sunlight. In summary, we found that photoreaction is an important dissipation pathway of clomazone in natural water systems.展开更多
Direct photochemical degradations of progesterone (PR) and testosterone (TR), two naturally produced hormones, have been conducted in non-buffered aqueous solution (pH ranging between 5.5 and 6.0). The irradiation exp...Direct photochemical degradations of progesterone (PR) and testosterone (TR), two naturally produced hormones, have been conducted in non-buffered aqueous solution (pH ranging between 5.5 and 6.0). The irradiation experiments were carried out in a batch reactor upon monochromatic (254 nm) and polychromatic (λ > 290 nm) at 25°C. GLC/MS and LC/UV-DAD/MS analyses were performed to investigate phototransformation products after a solid phase extraction (SPE) step for analytes concentration. For each compound several by-products have been identified and are the same ones under both irradiation conditions. Because of the presence of the same chromophore (α, β-unsaturated group) absorbing UV radiations in both hormones, the majority of chromatographic peaks correspond to by-products formed according to identical mechanisms involving isomerization, enolization, oxidation and hydration to lead to the generation of lumiketone, cyclopentenone, spiro-hydration, oxidation and hydroxylation photoproducts.展开更多
Atorvastatin, widely prescribed hypolipidemic drug, undergoes rapid, probably self-sensitised, degradation (less than 20% left after 25-minute irradiation) if irradiated by wavelengths 300 - 350 nm in aqueous solution...Atorvastatin, widely prescribed hypolipidemic drug, undergoes rapid, probably self-sensitised, degradation (less than 20% left after 25-minute irradiation) if irradiated by wavelengths 300 - 350 nm in aqueous solution. When ferric ions are added to the reaction mixture, the degradation follows first order kinetics with a rate constant of 0.130 min<sup><span style="white-space:nowrap;"><span style="white-space:nowrap;">−</span></span>1</sup>. Photochemical degradation may thus represent a significant way of environmental transformation of this pharmaceutical. Toxicity testing of atorvastatin and atorvastatin photoproducts performed on the water plant <em>Lemna minor</em> revealed that atorvastatin itself exhibited no observable toxic effect measured as leaf area growth inhibition, while the photoproducts showed a significant toxicity to the plant, which shows the extreme importance of investigating not only toxicity of drugs themselves on aquatic organisms but also effects of their transformation products.展开更多
The photochemical degradation of triadimefon in seawater was investigated under different reaction conditions in this study. The results showed that triadimefon could be effectively degraded by the irradiation of a hi...The photochemical degradation of triadimefon in seawater was investigated under different reaction conditions in this study. The results showed that triadimefon could be effectively degraded by the irradiation of a high-pressure mercury lamp and the photodegradation rates were influenced by aquatic media, heavy metal ions and photosensitizers. The photochemical degradation of triadimefon followed the first-order reaction kinetic behavior, with the rate constants ranging from 0.0027 to 0.0128 min-1 under the studied conditions. The photolysis of triadimefon was slower in natural seawater than in distilled water or synthetic seawater. All the heavy metal ions studied in this paper had inhibition effects on the photolysis of triadimefon. Acetone, as a common photosensitizer, could accelerate the photolysis of triadimefon. Three photoproducts were identified by GC-MS analysis. Our study confirmed that photochemical degradation is an effective pathway to remove triadimefon in seawater.展开更多
DNA damage in the form of cyclobutane pyrimidine dimers(CPDs) and (6-4) photoproducts(6-4PPs) induced by UV-B radiation in Arabidopsis thaliana at different temperatures was investigated using ELISA with specific mono...DNA damage in the form of cyclobutane pyrimidine dimers(CPDs) and (6-4) photoproducts(6-4PPs) induced by UV-B radiation in Arabidopsis thaliana at different temperatures was investigated using ELISA with specific monoclonal antibodies. CPDs and 6-4PPs increased during 3 h UV-B exposure, but further exposure led to decreases. Contrary to the commonly accepted view that DNA damage induced by UV-B radiation is temperature-independent because of its photochemical nature, we found UV-B-induction of CPDs and 6-4PPs in Arabidopsis to be slower at a low than at a high temperature. Photorepair of CPDs at 24℃ was much faster than that at 0℃ and 12℃, with 50% CPDs removal during 1 h exposure to white light. Photorepair of 6-4PPs at 12℃ was very slow as compared with that at 24℃, and almost no removal of 6-4PPs was detected after 4 h exposure to white light at 0℃. There was evidence to suggest that temperature-dependent DNA damage and photorepair could have important ecological implications.展开更多
Carbon monoxide(CO) plays a significant role in global warming and atmospheric chemistry. Global oceans are net natural sources of atmospheric CO. CO at surface ocean is primarily produced from the photochemical degra...Carbon monoxide(CO) plays a significant role in global warming and atmospheric chemistry. Global oceans are net natural sources of atmospheric CO. CO at surface ocean is primarily produced from the photochemical degradation of chromophoric dissolved organic matter(CDOM). In this study, the effects of photobleaching, temperature and the origin(terrestrial or marine) of CDOM on the apparent quantum yields(AQY) of CO were studied for seawater samples collected from Jiaozhou Bay. Our results demonstrat that photobleaching, temperature and the origin of CDOM strongly affected the efficiency of CO photoproduction. The concentration, absorbance and fluorescence of CDOM exponentially decreased with increasing light dose. Terrestrial riverine organic matter could be more prone to photodegradation than the marine algae-derived one. The relationships between CO AQY and the dissolved organic carbon-specific absorption coefficient at 254 nm for the photobleaching study were nonlinear, whereas those of the original samples were strongly linear. This suggests that: 1) terrestrial riverine CDOM was more efficient than marine algae-derived CDOM for CO photoproduction; 2) aromatic and olefinic moieties of the CDOM pool were affected more strongly by degradation processes than by aliphatic ones. Water temperature and the origin of CDOM strongly affected the efficiency of CO photoproduction. The photoproduction rate of CO in autumn was estimated to be 31.98 μmol m-2 d-1 and the total DOC photomineralization was equivalent to 3.25%- 6.35% of primary production in Jiaozhou Bay. Our results indicate that CO photochemistry in coastal areas is important for oceanic carbon cycle.展开更多
The photoproduction of the f1(1285)meson off the proton target is investigated within an effective Lagrangian approach.The t-channelρ-andω-exchange diagrams,u-channel nucleon-exchange diagram,generalized contact ter...The photoproduction of the f1(1285)meson off the proton target is investigated within an effective Lagrangian approach.The t-channelρ-andω-exchange diagrams,u-channel nucleon-exchange diagram,generalized contact term,and s-channel pole diagrams of the nucleon and a minimal number of nucleon resonances are taken into account in constructing the reaction amplitudes to describe the experimental data.Three different models,that is,the Feynman,Regge,and interpolated Regge models,are employed,where the t-channel reaction amplitudes are constructed in Feynman,Regge,and interpolated Regge types,respectively.The results show that neither the Feynman model with two nucleon resonances nor the interpolated Regge model with one nucleon resonance can satisfactorily reproduce the available data forγp→f1(1285)p.Nevertheless,in the Regge model,when any one of the N(1990)7/2^(+),N(2000)5/2^(+),N(2040)3/2^(+),N(2060)5/2^(-),N(2100)1/2^(+),N(2120)3/2^(-),N(2190)7/2^(-),N(2300)1/2^(+),and N(2570)5/2^(-)resonances is considered,the data can be well described.The resulting resonance parameters are consistent with those advocated in the Particle Data Group(PDG)review.Further analysis shows that,in the high-energy region,the peaks of γp→f1(1285)p differential cross sections at forward angles are dominated by the contributions from t-channelρ-andω-exchange diagrams,while in low-energy region,the s-channel pole diagrams of resonances also provide significant contributions to theγp→f1(1285)p cross sections.展开更多
基金supported by the National Natural Science Foundation of China (No. 21007018,51078161)the Natural Science Foundation of Hubei Province (No. 2010CDB01104)+1 种基金the Research Fund for the Doctoral Program of Higher Education of China (No. 20100142120004)the 11th Five-year Plan of National Water Environmental Special Program of China (No. 2008ZX07211-10-02)
文摘Tetracyclines constitute one of the most important antibiotic families and represent a classic example of phototoxicity. The photoproducts of tetracyclines and their parent compounds have potentially adverse effects on natural ecosystem. In this study, the self-sensitized oxidation products of tetracycline (TC) and oxytetracycline (OTC) were determined and the effects of Ca2+ and Mg2+on self-sensitized degradation were investigated. The Ca2+ and Mg2+ in the natural water sample accounted for enhancement (pH 7.3) and inhibition (pH 9.0) of photodegradation of TC and OTC due to the formation of metal-ions complexes. The formation of Mg2+ complexes was unfavorable for the photodegradation of the tetracyclines at both pH values. In contrast, the Ca2+ complexes facilitated the attack of singlet oxygen (102) arising from self-sensitization at pH 7.3 and enhanced TC photodegradation. For the first time, self- sensitized oxidation products of TC and OTC were verified by quenching experiments and detected by LC/ESI-DAD-MS. The products had a nominal mass 14 Da higher than the parent drugs (designated M+ 14), which resulted from the 102 attack of the dimethylamino group on the C-4 atom of the tetracyclines. The presence of Ca2+ and Mg2+ also affected the generation of M+ 14 due to the formation of metal-ions complexes with TC and OTC. The findings suggest that the metal-ion complexation has significant impact on the self- sensitized oxidation processes and the photoproducts of tetracyclines.
基金supported by the National Natural Science Foundation of China(No.21007018,51078161)the Natural Science Foundation of Hubei Province (No.2010CDB01104)+1 种基金the Research Fund for the Doctoral Program of Higher Education of China(No. 20100142120004)the 11th Five-year Plan of National Water Environmental Special Program of China(No.2008ZX07211-10-02)
文摘The aqueous photodegradation of the widely used antibiotic chlortetracycline(CTC) was investigated under simulated sunlight.The quantum yield of photodegradation increased from 3.3 × 10-4 to 8.5 × 10-3 within the pH range of 6.0 to 9.0.The presence of Ca2+,Fe3+,and NO3-enhanced the photodegradation of CTC,whereas Mg2+,Mn2+,and Zn2+ inhibited the degradation with the order Mn2+ Zn2+ Mg2+ at pH 7.3.The monovalent cations(Na+ and K+) had negligible effect on the photolysis of CTC.Fulvic acid(FA) decreased the photodegradation of CTC due to light screening effect.Hydrogen peroxide(H2O2) was formed concurrently with direct photodegradation of CTC.The generation rate of H2O2 increased from 0.027 to 0.086 μmol/(L.min) when the pH ranged from 6.0 to 9.0.The CTC solution was about three-fold more toxic to the Photobacterium phosphoreum bacteria after irradiation,suggesting that the photoproducts and H2O2 formed in the CTC solution exhibited high risk on the bacteria.By LC-ESI(+)-MS,the photoproducts of CTC were identified.The direct photodegradation of CTC was involved in hydroxylation and N-demethyl/dedismethyl processes.The main photoproducts included the iso-CTC analog containing hydroxyl groups(m/z 511.4 and 495.4),and the N-demethyl/dedismethyl products of the photoproduct m/z 495.4(m/z 481.3 and 467.4).In addition,the photochemical dechlorination of CTC led to tetracycline(m/z 445.5).
文摘The sunlight photodegradation half-lives of 20 mg/L acetochlor were 151, 154 and 169 days in de-ionized water, river water and paddy water, respectively. When exposed to ultraviolet (UV) light, acetochlor in aqueous solution was rapidly degraded. The half-lives were 7.1, 10.1, and 11.5 min in de-ionized water, river water and paddy water, respectively. Photoproducts of acetochlor were identified by gas chromatography/mass spectrometry(GC/MS) and found at least twelve photoproducts resulted from dechlorination with subsequent hydroxylation and cyclization processes. The chemical structures of ten photoproducts were presumed on the basis of mass spectrum interpretation and literature data. Photoproducts are identified as 2-ethyl-6-methylaniline; N,N-diethylaniline; 4,8-dimethyl-2-oxo-1,2,3,4- tetrahydroquino-line; 2-oxo-N-(2-ethyl-6-methylphenyl)-N-(ethoxymethyl)acetamide; N-(ethoxymethyl)-2′-ethyl-6′-methylformanilide;1-hydroxyacetyl-2-ethoxyl-7-ethylind ole; 8-ethyl-1-ethoxymethyl-2-oxo-1,2,3,4-tetrahydroquinoline; 4,8-dimethyl-1-ethoxymethyl-2-oxo-1,2,3,4-tetrahydroquinoline; 2-hydroxy-2′-ethyl-6′-methyl-N-(ethoxymethyl)acetanilide and a compound related to acetochlor. The other two photoproducts were detected by GC/MS although their chemical structure was unknown.
基金sponsored by Shandong Cynda Chemical Co.Ltd.(Shandong+1 种基金China)the Project of Pesticide Registration Residue of Ministry of Agriculture of China(FRF-SD-12-010B)
文摘The hydrolysis and photolysis of clomazone in aqueous solutions and natural water were assessed under natural and controlled conditions. Kinetics of hydrolysis and photolysis of clomazone were determined by HPLC-DAD. Photoproducts were identiifed by HPLC-MS. No noticeable hydrolysis occurred in aqueous buffer solutions ((25±2)°C, pH (4.5±0.1), pH (7.4±0.1), pH (9.0±0.1);(50±2)°C, pH (4.5±0.1), pH (7.4±0.1)) or in natural water up to 90 d. At pH (9.0±0.1) and (50±2)°C the half-life of clomazone was 50.2 d. Clomazone photodecomposition rate in aqueous solutions under UV radiation and natural sunlight followed ifrst-order kinetics. Degradation rates were faster under UV light (half-life of 51-59 min) compared to sunlight (half-life of 87-136 d). Under UV light, four major photoproducts were detected and tentatively identiifed according to HPLC-MS spectral information such as 2-chlorobenzamide, N-hydroxy-(2-benzyl)-2-methylpropan-amide, 2-[2-phenol]-4,4-dimethyl-3-isoxazolidinone and 2-[(4,6-dihydroxyl-2-chlorine phenol)]-4,4-dimethyl-3-isoxazolidinone. These results suggested that clomazone photodegradation proceeds via several reaction pathways:1) dehalogenation;2) substitution of chlorine group by hydroxyl;3) cleavage of the side chain. Photosensitizers, such as H2O2 and ribolfavin, could enhance photolysis of clomazone in natural sunlight. In summary, we found that photoreaction is an important dissipation pathway of clomazone in natural water systems.
文摘Direct photochemical degradations of progesterone (PR) and testosterone (TR), two naturally produced hormones, have been conducted in non-buffered aqueous solution (pH ranging between 5.5 and 6.0). The irradiation experiments were carried out in a batch reactor upon monochromatic (254 nm) and polychromatic (λ > 290 nm) at 25°C. GLC/MS and LC/UV-DAD/MS analyses were performed to investigate phototransformation products after a solid phase extraction (SPE) step for analytes concentration. For each compound several by-products have been identified and are the same ones under both irradiation conditions. Because of the presence of the same chromophore (α, β-unsaturated group) absorbing UV radiations in both hormones, the majority of chromatographic peaks correspond to by-products formed according to identical mechanisms involving isomerization, enolization, oxidation and hydration to lead to the generation of lumiketone, cyclopentenone, spiro-hydration, oxidation and hydroxylation photoproducts.
文摘Atorvastatin, widely prescribed hypolipidemic drug, undergoes rapid, probably self-sensitised, degradation (less than 20% left after 25-minute irradiation) if irradiated by wavelengths 300 - 350 nm in aqueous solution. When ferric ions are added to the reaction mixture, the degradation follows first order kinetics with a rate constant of 0.130 min<sup><span style="white-space:nowrap;"><span style="white-space:nowrap;">−</span></span>1</sup>. Photochemical degradation may thus represent a significant way of environmental transformation of this pharmaceutical. Toxicity testing of atorvastatin and atorvastatin photoproducts performed on the water plant <em>Lemna minor</em> revealed that atorvastatin itself exhibited no observable toxic effect measured as leaf area growth inhibition, while the photoproducts showed a significant toxicity to the plant, which shows the extreme importance of investigating not only toxicity of drugs themselves on aquatic organisms but also effects of their transformation products.
文摘The photochemical degradation of triadimefon in seawater was investigated under different reaction conditions in this study. The results showed that triadimefon could be effectively degraded by the irradiation of a high-pressure mercury lamp and the photodegradation rates were influenced by aquatic media, heavy metal ions and photosensitizers. The photochemical degradation of triadimefon followed the first-order reaction kinetic behavior, with the rate constants ranging from 0.0027 to 0.0128 min-1 under the studied conditions. The photolysis of triadimefon was slower in natural seawater than in distilled water or synthetic seawater. All the heavy metal ions studied in this paper had inhibition effects on the photolysis of triadimefon. Acetone, as a common photosensitizer, could accelerate the photolysis of triadimefon. Three photoproducts were identified by GC-MS analysis. Our study confirmed that photochemical degradation is an effective pathway to remove triadimefon in seawater.
文摘DNA damage in the form of cyclobutane pyrimidine dimers(CPDs) and (6-4) photoproducts(6-4PPs) induced by UV-B radiation in Arabidopsis thaliana at different temperatures was investigated using ELISA with specific monoclonal antibodies. CPDs and 6-4PPs increased during 3 h UV-B exposure, but further exposure led to decreases. Contrary to the commonly accepted view that DNA damage induced by UV-B radiation is temperature-independent because of its photochemical nature, we found UV-B-induction of CPDs and 6-4PPs in Arabidopsis to be slower at a low than at a high temperature. Photorepair of CPDs at 24℃ was much faster than that at 0℃ and 12℃, with 50% CPDs removal during 1 h exposure to white light. Photorepair of 6-4PPs at 12℃ was very slow as compared with that at 24℃, and almost no removal of 6-4PPs was detected after 4 h exposure to white light at 0℃. There was evidence to suggest that temperature-dependent DNA damage and photorepair could have important ecological implications.
基金financially supported by the National Natural Science Foundation of China (No. 40976043)the Science and Technology Key Project of Shandong Province (2006GG2205024)+2 种基金the Changjiang Scholars Program, Ministry of Education of Chinathe Taishan Scholars Program of Shandong Provincethe Scholar Foundation of Qingdao Agricultural University (631102)
文摘Carbon monoxide(CO) plays a significant role in global warming and atmospheric chemistry. Global oceans are net natural sources of atmospheric CO. CO at surface ocean is primarily produced from the photochemical degradation of chromophoric dissolved organic matter(CDOM). In this study, the effects of photobleaching, temperature and the origin(terrestrial or marine) of CDOM on the apparent quantum yields(AQY) of CO were studied for seawater samples collected from Jiaozhou Bay. Our results demonstrat that photobleaching, temperature and the origin of CDOM strongly affected the efficiency of CO photoproduction. The concentration, absorbance and fluorescence of CDOM exponentially decreased with increasing light dose. Terrestrial riverine organic matter could be more prone to photodegradation than the marine algae-derived one. The relationships between CO AQY and the dissolved organic carbon-specific absorption coefficient at 254 nm for the photobleaching study were nonlinear, whereas those of the original samples were strongly linear. This suggests that: 1) terrestrial riverine CDOM was more efficient than marine algae-derived CDOM for CO photoproduction; 2) aromatic and olefinic moieties of the CDOM pool were affected more strongly by degradation processes than by aliphatic ones. Water temperature and the origin of CDOM strongly affected the efficiency of CO photoproduction. The photoproduction rate of CO in autumn was estimated to be 31.98 μmol m-2 d-1 and the total DOC photomineralization was equivalent to 3.25%- 6.35% of primary production in Jiaozhou Bay. Our results indicate that CO photochemistry in coastal areas is important for oceanic carbon cycle.
基金Partially supported by the National Natural Science Foundation of China(12175240,12147153,11635009,12305097,12305137)the Fundamental Research Funds for the Central Universitiesthe China Postdoctoral Science Foundation(2021M693141,2021M693142)。
文摘The photoproduction of the f1(1285)meson off the proton target is investigated within an effective Lagrangian approach.The t-channelρ-andω-exchange diagrams,u-channel nucleon-exchange diagram,generalized contact term,and s-channel pole diagrams of the nucleon and a minimal number of nucleon resonances are taken into account in constructing the reaction amplitudes to describe the experimental data.Three different models,that is,the Feynman,Regge,and interpolated Regge models,are employed,where the t-channel reaction amplitudes are constructed in Feynman,Regge,and interpolated Regge types,respectively.The results show that neither the Feynman model with two nucleon resonances nor the interpolated Regge model with one nucleon resonance can satisfactorily reproduce the available data forγp→f1(1285)p.Nevertheless,in the Regge model,when any one of the N(1990)7/2^(+),N(2000)5/2^(+),N(2040)3/2^(+),N(2060)5/2^(-),N(2100)1/2^(+),N(2120)3/2^(-),N(2190)7/2^(-),N(2300)1/2^(+),and N(2570)5/2^(-)resonances is considered,the data can be well described.The resulting resonance parameters are consistent with those advocated in the Particle Data Group(PDG)review.Further analysis shows that,in the high-energy region,the peaks of γp→f1(1285)p differential cross sections at forward angles are dominated by the contributions from t-channelρ-andω-exchange diagrams,while in low-energy region,the s-channel pole diagrams of resonances also provide significant contributions to theγp→f1(1285)p cross sections.