Natural hydrocarbon seeps in the marine environment are important contributors to greenhouse gases in the atmosphere. Such gases include methane, which plays a significant role in global carbon cycling and climate cha...Natural hydrocarbon seeps in the marine environment are important contributors to greenhouse gases in the atmosphere. Such gases include methane, which plays a significant role in global carbon cycling and climate change. To accurately quantify the methane flux from hydrocarbon seeps on the seafloor, a specialized in situ and online gas flux measuring(GFM) device was designed to obtain high-resolution time course gas fluxes using the process of equal volume exchange. The device consists of a 1.0-m diameter, 0.9-m tall, inverted conical tent and a GFM instrument that contains a solenoid valve, level transducer, and gas collection chamber. Rising gas bubbles from seeps were measured by laboratory-calibrated GFM instruments attached to the top of the tent. According to the experimental data, the optimal anti-shake time interval was 5 s. The measurement range of the device was 0–15 L min^(-1), and the relative error was ± 1.0%. The device was initially deployed at an active seep site in the Lingtou Promontory seep field in South China Sea. The amount of gas released from a single gas vent was 30.5 m^3 during the measurement period, and the gas flow rate ranged from 22 to 72 Lh^(-1), depending on tidal period, and was strongly negatively correlated with water depth. The measurement results strongly suggest that oceanic tides and swells had a significant forcing effect on gas flux. Low flow rates were associated with high tides and vice versa. The changes in gas volume escaping from the seafloor seeps could be attributed to the hydrostatic pressure induced by water depth. Our findings suggest that in the marine environment, especially in the shallow shelf area, sea level variation may play an important role in controlling methane release into the ocean. Such releases probably also affect atmospheric methane levels.展开更多
Ball milling modification was performed on Cs/X catalysts before or after cesium ion exchange.Multiple characterization results(such as pyridine-FTIR,XPS,and solid-state NMR)demonstrated that ball milling played a dis...Ball milling modification was performed on Cs/X catalysts before or after cesium ion exchange.Multiple characterization results(such as pyridine-FTIR,XPS,and solid-state NMR)demonstrated that ball milling played a distinct role in these two different preparation procedures of the catalyst.Ball milling performed after the cesium modification has a strong influence on the Cs/X structure and acid-base properties,which results in the enhancement of the catalytic performance for side-chain methylation of toluene with methanol.Detailed studies revealed that ball milling intensified the interactions between oxides and molecular sieves,which not only increased the dispersion of the Cs species but also generated some weaker basic centers.It is proposed that the new basic centers could be Si-O-Cs and Al-O-Cs,which are produced by breaking of the Si-O-Al bonds of the zeolite framework under the synergetic effect of ball milling and alkali treatment.These new active sites may help to promote the side-chain methylation reaction.However,excessive ball milling will lead to the vanishing of zeolite micropores,thus deactivating side-chain methylation activity,which indicates that microporosity plays a key role in side-chain methylation and individual basic centers cannot catalyze this reaction.展开更多
基金provided by the National Scientific Foundation of China (Nos. 41676046 and 41306045)the Knowledge Innovation Project of the Chinese Academy of Sciences (Nos. SIDSSE-201208 and SQ201110)+1 种基金the 'Hundred Talents Program' of the Chinese Academy of Sciencesfinancial support from China Scholarship Council
文摘Natural hydrocarbon seeps in the marine environment are important contributors to greenhouse gases in the atmosphere. Such gases include methane, which plays a significant role in global carbon cycling and climate change. To accurately quantify the methane flux from hydrocarbon seeps on the seafloor, a specialized in situ and online gas flux measuring(GFM) device was designed to obtain high-resolution time course gas fluxes using the process of equal volume exchange. The device consists of a 1.0-m diameter, 0.9-m tall, inverted conical tent and a GFM instrument that contains a solenoid valve, level transducer, and gas collection chamber. Rising gas bubbles from seeps were measured by laboratory-calibrated GFM instruments attached to the top of the tent. According to the experimental data, the optimal anti-shake time interval was 5 s. The measurement range of the device was 0–15 L min^(-1), and the relative error was ± 1.0%. The device was initially deployed at an active seep site in the Lingtou Promontory seep field in South China Sea. The amount of gas released from a single gas vent was 30.5 m^3 during the measurement period, and the gas flow rate ranged from 22 to 72 Lh^(-1), depending on tidal period, and was strongly negatively correlated with water depth. The measurement results strongly suggest that oceanic tides and swells had a significant forcing effect on gas flux. Low flow rates were associated with high tides and vice versa. The changes in gas volume escaping from the seafloor seeps could be attributed to the hydrostatic pressure induced by water depth. Our findings suggest that in the marine environment, especially in the shallow shelf area, sea level variation may play an important role in controlling methane release into the ocean. Such releases probably also affect atmospheric methane levels.
文摘Ball milling modification was performed on Cs/X catalysts before or after cesium ion exchange.Multiple characterization results(such as pyridine-FTIR,XPS,and solid-state NMR)demonstrated that ball milling played a distinct role in these two different preparation procedures of the catalyst.Ball milling performed after the cesium modification has a strong influence on the Cs/X structure and acid-base properties,which results in the enhancement of the catalytic performance for side-chain methylation of toluene with methanol.Detailed studies revealed that ball milling intensified the interactions between oxides and molecular sieves,which not only increased the dispersion of the Cs species but also generated some weaker basic centers.It is proposed that the new basic centers could be Si-O-Cs and Al-O-Cs,which are produced by breaking of the Si-O-Al bonds of the zeolite framework under the synergetic effect of ball milling and alkali treatment.These new active sites may help to promote the side-chain methylation reaction.However,excessive ball milling will lead to the vanishing of zeolite micropores,thus deactivating side-chain methylation activity,which indicates that microporosity plays a key role in side-chain methylation and individual basic centers cannot catalyze this reaction.
