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
After exposure of one-year old seedlings of Swietenia macrophylla to an overnight temperature (13 C, 19 C, 25 C, 31 C or 35 C), the leaf net photosynthetic rate (Pn) was researched through measuring photosynthetic lig...After exposure of one-year old seedlings of Swietenia macrophylla to an overnight temperature (13 C, 19 C, 25 C, 31 C or 35 C), the leaf net photosynthetic rate (Pn) was researched through measuring photosynthetic light-response curves at 360 mmolmol-1 CO2, and photosynthetic CO2-response curves at light-saturated intensity (1500 mmolm-2 s-1). The optimal temperature for photosynthesis measured at 360 mmol穖ol-1 CO2 was from 25 C to 31 C, but which was from 31C to 35 C at saturating CO2 concentration. At temperature of below 25 C, the decline in Pn was mainly due to the drop in carboxylation efficiency (Ce), while as temperature was over 31 C, the reduction in Pn resulted from both decrease in Ce and increase in leaf respiration. The CO2-induced stimulation of photosynthesis was strongly inhibited at temperatures below 13 C. The results showed that, the leaf photosynthesis of tropical evergreen plants should not be accelerated at low temperature in winter season with elevated CO2 concentration in the future.展开更多
CdS quantum dots(QDs)have been extensively studied as photocatalysts and sensitizers for visible-light-driven water reduction.However,their efficiencies are limited by the need to accumulate sufficient redox equivalen...CdS quantum dots(QDs)have been extensively studied as photocatalysts and sensitizers for visible-light-driven water reduction.However,their efficiencies are limited by the need to accumulate sufficient redox equivalents to produce_(H2)and consequent photocorrosion associated with slow hole-transfer rates.To address these limitations,we report the formation of CdS QD assemblies(aerogels,AGs)capable of facilitating energy/charge transport between individual QDs,and evaluate their performance as photocatalysts for hydrogen evolution as a function of structure,wurtzite(w-)vs.zincblende(zb-),and different annealing temperatures.The formation of AGs from QDs resulted in increased rates of_(H2)production under visible light illumination:from 1458(QD)to 6650(AG)μmol_(H2)·h^(-1)·g^(-1)on zbCdS and from 1221(QD)to 3325(AG)μmol_(H2)·h^(-1)·g^(-1)on wCdS.This is attributed to exciton delocalization between adjacent QDs facilitating charge/energy transport.Thermal processing of CdS AGs up to 250℃ improved their activity,increasing the degree of exciton delocalization,while annealing them to 300℃ caused sintering of the primary QD particles within the AGs and a decrease in activity associated with loss in surface area.The best photocatalyst,zbCdS AG annealed at 250℃,had an average_(H2)production rate of 13,604±2017μmol_(H2)·h^(-1)·g^(-1),an apparent quantum yield of 2.8%at 425±12.5 nm,and was stable for 2 h before beginning to deactivate due to photocorrosion.This study confirms the potential of CdS AGs as matrixes for the design of more active and stable composite photocatalysts for water splitting.展开更多
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.
文摘After exposure of one-year old seedlings of Swietenia macrophylla to an overnight temperature (13 C, 19 C, 25 C, 31 C or 35 C), the leaf net photosynthetic rate (Pn) was researched through measuring photosynthetic light-response curves at 360 mmolmol-1 CO2, and photosynthetic CO2-response curves at light-saturated intensity (1500 mmolm-2 s-1). The optimal temperature for photosynthesis measured at 360 mmol穖ol-1 CO2 was from 25 C to 31 C, but which was from 31C to 35 C at saturating CO2 concentration. At temperature of below 25 C, the decline in Pn was mainly due to the drop in carboxylation efficiency (Ce), while as temperature was over 31 C, the reduction in Pn resulted from both decrease in Ce and increase in leaf respiration. The CO2-induced stimulation of photosynthesis was strongly inhibited at temperatures below 13 C. The results showed that, the leaf photosynthesis of tropical evergreen plants should not be accelerated at low temperature in winter season with elevated CO2 concentration in the future.
基金supported by NSF Award No.1427926,and the Talos F200X G2 S/TEM that is funded in part through NSF MRI Award No.2018587supported by the U.S.Department of Energy,Office of Science,Office of Basic Energy Sciences,under Award Number SC0023324.
文摘CdS quantum dots(QDs)have been extensively studied as photocatalysts and sensitizers for visible-light-driven water reduction.However,their efficiencies are limited by the need to accumulate sufficient redox equivalents to produce_(H2)and consequent photocorrosion associated with slow hole-transfer rates.To address these limitations,we report the formation of CdS QD assemblies(aerogels,AGs)capable of facilitating energy/charge transport between individual QDs,and evaluate their performance as photocatalysts for hydrogen evolution as a function of structure,wurtzite(w-)vs.zincblende(zb-),and different annealing temperatures.The formation of AGs from QDs resulted in increased rates of_(H2)production under visible light illumination:from 1458(QD)to 6650(AG)μmol_(H2)·h^(-1)·g^(-1)on zbCdS and from 1221(QD)to 3325(AG)μmol_(H2)·h^(-1)·g^(-1)on wCdS.This is attributed to exciton delocalization between adjacent QDs facilitating charge/energy transport.Thermal processing of CdS AGs up to 250℃ improved their activity,increasing the degree of exciton delocalization,while annealing them to 300℃ caused sintering of the primary QD particles within the AGs and a decrease in activity associated with loss in surface area.The best photocatalyst,zbCdS AG annealed at 250℃,had an average_(H2)production rate of 13,604±2017μmol_(H2)·h^(-1)·g^(-1),an apparent quantum yield of 2.8%at 425±12.5 nm,and was stable for 2 h before beginning to deactivate due to photocorrosion.This study confirms the potential of CdS AGs as matrixes for the design of more active and stable composite photocatalysts for water splitting.