The CO2reforming of CH4is studied over MgO‐promoted Ni catalysts,which were supported on alumina prepared from hydrotalcite.This presents an improved stability compared with non‐promoted catalysts.The introduction o...The CO2reforming of CH4is studied over MgO‐promoted Ni catalysts,which were supported on alumina prepared from hydrotalcite.This presents an improved stability compared with non‐promoted catalysts.The introduction of the MgO promoter was achieved through the‘‘memory effect’’of the Ni‐Al hydrotalcite structure,and ICP‐MS confirmed that only0.42wt.%of Mg2+ions were added into the Ni‐Mg/Al catalyst.Although no differences in the Ni particle size and basicity strength were observed,the Ni‐Mg/Al catalyst showed a higher catalytic stability than the Ni/Al catalyst.A series of surface reaction experiments were used and showed that the addition of a MgO promoter with low concentration can promote CO2dissociation to form active surface oxygen arising from the formation of the Ni‐MgO interface sites.Therefore,the carbon‐resistance promotion by nature was suggested to contribute to an oxidative environment around Ni particles,which would increase the conversion of carbon residues from CH4cracking to yield CO on the Ni metal surface.?2018,Dalian Institute of Chemical Physics,Chinese Academy of Sciences.Published by Elsevier B.V.All rights reserved.展开更多
COphotoreduction is an attractive process which allows the storage of solar energy and synthesis of solar fuels. Many different photocatalytic systems have been developed, while the alternative photo-reactors are stil...COphotoreduction is an attractive process which allows the storage of solar energy and synthesis of solar fuels. Many different photocatalytic systems have been developed, while the alternative photo-reactors are still insufficiently investigated. In this work, photoreduction of COwith HO into CHwas investigated in a modified concentrating solar reactor, using TiOand Pt/TiOas the catalysts. The TiOand Pt/TiOsamples were extensively characterized by different techniques including powder X-ray diffraction（XRD）, Nadsorption/desorption and UV–vis absorption. The catalytic performance of the TiOand Pt/TiOsamples in the gas phase was evaluated under unconcentrated and concentrated Xe-lamp light and nature solar light with different concentrating ratios. Various parameters of the reaction system and the catalysts were investigated and optimized to maximize the catalytic performance of COreduction system. Compared with the normal light irradiation, the TiOand Pt/TiOsamples show higher photocatalytic activity（about 6–7 times） for reducing COinto CHunder concentrated Xe-lamp light and nature solar light. In the range of experimental light intensity, it is found that the concentration of the light makes it suitable for the catalytic reaction, and increases the utilization efficiency of the TiOand Pt/TiOsamples while does not decrease the quantum efficiency.展开更多
During the 2nd Chinese Arctic Research Expedition, 20 pair of atmospheric samples were collected on the cruising route from Shanghai to Arctic Ocean using NOAA/ESRL flask sampling unit. Mean concentration of CO2 and C...During the 2nd Chinese Arctic Research Expedition, 20 pair of atmospheric samples were collected on the cruising route from Shanghai to Arctic Ocean using NOAA/ESRL flask sampling unit. Mean concentration of CO2 and CH4 were analyzed in different latitude zone from 30°N to 80°N and the distribution characteristics were studied. Mean concentration of CO2 decrease toward high latitude which indicates the uptake effect of CO2 by ocean. Coinciding with the CH4 global distribution character, mean CH4 concentration increase from 45°N to the North Pole region. Regional or local air mass may influence the greenhouse gas concentrations near seashore in the middle latitude （30°N-45°N）.展开更多
(CH_3C_5H_4)Zr(S_2CNBz_2)_3, Mr=987.55, space group P1, a=13.002(4), b=13.659(3), c=29.685(8); α=100.72(2)~o,β=97.23(2)~o, γ=105.36(2)~o; V=4909(2)~3, Z=4, Dc=1.34gcm^(-3), Mo-K(λ=0.71073A) radiation, μ=5.0cm^(-1...(CH_3C_5H_4)Zr(S_2CNBz_2)_3, Mr=987.55, space group P1, a=13.002(4), b=13.659(3), c=29.685(8); α=100.72(2)~o,β=97.23(2)~o, γ=105.36(2)~o; V=4909(2)~3, Z=4, Dc=1.34gcm^(-3), Mo-K(λ=0.71073A) radiation, μ=5.0cm^(-1), R=0.069, Rw=0.078 for 6100 reflections. The title complex has pentagonal bipyramid configuration in which the zirconium atom is coordinated by one CH_3C_5H_4 group and three bidentate dibenzyldithiocarbamate ligands.展开更多
In this study, by analyzing CH4 concentration and 613CCH4 in soil-gas profiles, the potentials of CH4 gas transfer from ground to atmosphere were studied at four representative sectors in the Yakela condensed gas fiel...In this study, by analyzing CH4 concentration and 613CCH4 in soil-gas profiles, the potentials of CH4 gas transfer from ground to atmosphere were studied at four representative sectors in the Yakela condensed gas field in the Tarim Basin, Xinjiang, China. These are： 1） the oil-gas interface sector, 2） fault sector, 3） oil-water interface sector, 4） an external area. Variation in CH4 in soil-gas profiles showed that CH4 microseepage resulted from the migration of subsurface hydrocarbon from deep-buried reservoirs to the earth＇s surface. It was found that CH4 from deep-buried reservoirs could migrate upwards to the surface through faults, fissures and permeable rocks, during which some CH4 was oxidized and the unoxidized methane remained in the soil or was emitted into the atmosphere. The lowest level of CH4 at the soil-gas profile was found at the CH4 gas-phase equilibrium point at which the CH4 migration upwards from deep-buried reservoirs and the CH4 diffusion downwards from the atmosphere met. The 613CcH4 and ethane, propane in soil gas exhibited thermogenic characteristics, suggesting the occurrence of CH4 microseepage from deep-buried reservoirs. A linear correlation analysis between CH4 concentrations in soil gas and temperature, moisture, pH, Eh, Ec and particle size of soil indicated that both soil Eh and soil temperature could affect CH4 concentration in soil gas while soil pH could indirectly influence soil methanotrophic oxidation via impacting soil Eh.展开更多
Since the industrial revolution,enhancement of atmospheric greenhouse gas concentrations as a result of human activities has been the primary cause of global warming.The monitoring and evaluation of greenhouse gases a...Since the industrial revolution,enhancement of atmospheric greenhouse gas concentrations as a result of human activities has been the primary cause of global warming.The monitoring and evaluation of greenhouse gases are significant prerequisites for carbon emission control.Using monthly data of global atmospheric carbon dioxide(CO_(2))and methane(CH4)column concentrations(hereinafter XCO_(2) and XCH_(4),respectively)retrieved by the Greenhouse Gas Observation Satellite(GOSAT),we analyzed the variations in XCO_(2)and XCH_(4)in China during 2010-2022 after confirming the reliability of the data.Then,the influence of a strong El Niño event in 2015-2016 on XCO_(2) and XCH_(4) variations in China was further studied.The results show that the retrieved XCO_(2) and XCH_(4) from GOSAT have similar temporal variation trends and significant correlations with the ground observation and emission inventory data of an atmospheric background station,which could be used to assess the variations in XCO_(2) and XCH_(4) in China.XCO_(2) is high in spring and winter while XCH_(4) is high in autumn.Both XCO_(2) and XCH_(4) gradually declined from Southeast China to Northwest and Northeast China,with variation ranges of 401-406 and 1.81-1.88 ppmv,respectively;and the high value areas are located in the middle-lower Yangtze River basin.XCO_(2) and XCH_(4) in China increased as a whole during 2010-2022,with rapid enhancement and high levels of XCO_(2) and XCH_(4) in several areas.The significant increases in XCO_(2) and XCH_(4) over China in 2016 might be closely related to the strong El Niño-Southern Oscillation(ENSO)event during 2015-2016.Under a global warming background in 2015,XCO_(2) and XCH_(4) increased by 0.768%and 0.657%in 2016 in China.Data analysis reveals that both the XCO_(2) and XCH_(4) variations might reflect the significant impact of the ENSO event on glacier melting in the Tibetan Plateau.展开更多
GREENHOUSE gases such as CH<sub>4</sub> in the ancient atmospheric concentration can be reconstructed by extracting and analyzing the gases trapped in polar ice core bubbles. It is a new attempt to extract...GREENHOUSE gases such as CH<sub>4</sub> in the ancient atmospheric concentration can be reconstructed by extracting and analyzing the gases trapped in polar ice core bubbles. It is a new attempt to extract and analyze the CH<sub>4</sub> concentration in Dunde ice core for the study of mountain glacier. Samples were taken from the about 140-m ice core drilled in 1987 in Dunde ice cap in Qilian Mountain. The ice core has been well preserved in cold room. 12 samples were taken from the upper 95 m, and cut to 15 cm in length and 5cm in diameter. CH<sub>4</sub> concentrations were measured in CNRS Laboratory of Glaciology, Grenoble, France.展开更多
基金supported by the National Natural Science Fundation of China(U1361202,51276120)~~
文摘The CO2reforming of CH4is studied over MgO‐promoted Ni catalysts,which were supported on alumina prepared from hydrotalcite.This presents an improved stability compared with non‐promoted catalysts.The introduction of the MgO promoter was achieved through the‘‘memory effect’’of the Ni‐Al hydrotalcite structure,and ICP‐MS confirmed that only0.42wt.%of Mg2+ions were added into the Ni‐Mg/Al catalyst.Although no differences in the Ni particle size and basicity strength were observed,the Ni‐Mg/Al catalyst showed a higher catalytic stability than the Ni/Al catalyst.A series of surface reaction experiments were used and showed that the addition of a MgO promoter with low concentration can promote CO2dissociation to form active surface oxygen arising from the formation of the Ni‐MgO interface sites.Therefore,the carbon‐resistance promotion by nature was suggested to contribute to an oxidative environment around Ni particles,which would increase the conversion of carbon residues from CH4cracking to yield CO on the Ni metal surface.?2018,Dalian Institute of Chemical Physics,Chinese Academy of Sciences.Published by Elsevier B.V.All rights reserved.
文摘COphotoreduction is an attractive process which allows the storage of solar energy and synthesis of solar fuels. Many different photocatalytic systems have been developed, while the alternative photo-reactors are still insufficiently investigated. In this work, photoreduction of COwith HO into CHwas investigated in a modified concentrating solar reactor, using TiOand Pt/TiOas the catalysts. The TiOand Pt/TiOsamples were extensively characterized by different techniques including powder X-ray diffraction（XRD）, Nadsorption/desorption and UV–vis absorption. The catalytic performance of the TiOand Pt/TiOsamples in the gas phase was evaluated under unconcentrated and concentrated Xe-lamp light and nature solar light with different concentrating ratios. Various parameters of the reaction system and the catalysts were investigated and optimized to maximize the catalytic performance of COreduction system. Compared with the normal light irradiation, the TiOand Pt/TiOsamples show higher photocatalytic activity（about 6–7 times） for reducing COinto CHunder concentrated Xe-lamp light and nature solar light. In the range of experimental light intensity, it is found that the concentration of the light makes it suitable for the catalytic reaction, and increases the utilization efficiency of the TiOand Pt/TiOsamples while does not decrease the quantum efficiency.
文摘During the 2nd Chinese Arctic Research Expedition, 20 pair of atmospheric samples were collected on the cruising route from Shanghai to Arctic Ocean using NOAA/ESRL flask sampling unit. Mean concentration of CO2 and CH4 were analyzed in different latitude zone from 30°N to 80°N and the distribution characteristics were studied. Mean concentration of CO2 decrease toward high latitude which indicates the uptake effect of CO2 by ocean. Coinciding with the CH4 global distribution character, mean CH4 concentration increase from 45°N to the North Pole region. Regional or local air mass may influence the greenhouse gas concentrations near seashore in the middle latitude （30°N-45°N）.
文摘(CH_3C_5H_4)Zr(S_2CNBz_2)_3, Mr=987.55, space group P1, a=13.002(4), b=13.659(3), c=29.685(8); α=100.72(2)~o,β=97.23(2)~o, γ=105.36(2)~o; V=4909(2)~3, Z=4, Dc=1.34gcm^(-3), Mo-K(λ=0.71073A) radiation, μ=5.0cm^(-1), R=0.069, Rw=0.078 for 6100 reflections. The title complex has pentagonal bipyramid configuration in which the zirconium atom is coordinated by one CH_3C_5H_4 group and three bidentate dibenzyldithiocarbamate ligands.
基金supported by the National Natural Science Foundation of China(Grant No.40973076 and 41072099)
文摘In this study, by analyzing CH4 concentration and 613CCH4 in soil-gas profiles, the potentials of CH4 gas transfer from ground to atmosphere were studied at four representative sectors in the Yakela condensed gas field in the Tarim Basin, Xinjiang, China. These are： 1） the oil-gas interface sector, 2） fault sector, 3） oil-water interface sector, 4） an external area. Variation in CH4 in soil-gas profiles showed that CH4 microseepage resulted from the migration of subsurface hydrocarbon from deep-buried reservoirs to the earth＇s surface. It was found that CH4 from deep-buried reservoirs could migrate upwards to the surface through faults, fissures and permeable rocks, during which some CH4 was oxidized and the unoxidized methane remained in the soil or was emitted into the atmosphere. The lowest level of CH4 at the soil-gas profile was found at the CH4 gas-phase equilibrium point at which the CH4 migration upwards from deep-buried reservoirs and the CH4 diffusion downwards from the atmosphere met. The 613CcH4 and ethane, propane in soil gas exhibited thermogenic characteristics, suggesting the occurrence of CH4 microseepage from deep-buried reservoirs. A linear correlation analysis between CH4 concentrations in soil gas and temperature, moisture, pH, Eh, Ec and particle size of soil indicated that both soil Eh and soil temperature could affect CH4 concentration in soil gas while soil pH could indirectly influence soil methanotrophic oxidation via impacting soil Eh.
基金Supported by the Natural Science Foundation of Liaoning Province(2022-MS-098)Joint Open Fund of the Institute of Atmospheric Environment,China Meteorological Administration,Shenyang and Key Laboratory of Agro-Meteorological Disasters of Liaoning Province(2024SYIAEKFZD05 and 2023SYIAEKFZD06)+3 种基金Open Research Project of Shangdianzi Atmospheric Background Station(SDZ20220912)Joint Research Project for Meteorological Capacity Improvement(23NLTSZ006)Applied Basic Research Program of Liaoning Province(2022JH2/101300193)National Natural Science Foundation of China(42105159 and 42005040).
文摘Since the industrial revolution,enhancement of atmospheric greenhouse gas concentrations as a result of human activities has been the primary cause of global warming.The monitoring and evaluation of greenhouse gases are significant prerequisites for carbon emission control.Using monthly data of global atmospheric carbon dioxide(CO_(2))and methane(CH4)column concentrations(hereinafter XCO_(2) and XCH_(4),respectively)retrieved by the Greenhouse Gas Observation Satellite(GOSAT),we analyzed the variations in XCO_(2)and XCH_(4)in China during 2010-2022 after confirming the reliability of the data.Then,the influence of a strong El Niño event in 2015-2016 on XCO_(2) and XCH_(4) variations in China was further studied.The results show that the retrieved XCO_(2) and XCH_(4) from GOSAT have similar temporal variation trends and significant correlations with the ground observation and emission inventory data of an atmospheric background station,which could be used to assess the variations in XCO_(2) and XCH_(4) in China.XCO_(2) is high in spring and winter while XCH_(4) is high in autumn.Both XCO_(2) and XCH_(4) gradually declined from Southeast China to Northwest and Northeast China,with variation ranges of 401-406 and 1.81-1.88 ppmv,respectively;and the high value areas are located in the middle-lower Yangtze River basin.XCO_(2) and XCH_(4) in China increased as a whole during 2010-2022,with rapid enhancement and high levels of XCO_(2) and XCH_(4) in several areas.The significant increases in XCO_(2) and XCH_(4) over China in 2016 might be closely related to the strong El Niño-Southern Oscillation(ENSO)event during 2015-2016.Under a global warming background in 2015,XCO_(2) and XCH_(4) increased by 0.768%and 0.657%in 2016 in China.Data analysis reveals that both the XCO_(2) and XCH_(4) variations might reflect the significant impact of the ENSO event on glacier melting in the Tibetan Plateau.
文摘GREENHOUSE gases such as CH<sub>4</sub> in the ancient atmospheric concentration can be reconstructed by extracting and analyzing the gases trapped in polar ice core bubbles. It is a new attempt to extract and analyze the CH<sub>4</sub> concentration in Dunde ice core for the study of mountain glacier. Samples were taken from the about 140-m ice core drilled in 1987 in Dunde ice cap in Qilian Mountain. The ice core has been well preserved in cold room. 12 samples were taken from the upper 95 m, and cut to 15 cm in length and 5cm in diameter. CH<sub>4</sub> concentrations were measured in CNRS Laboratory of Glaciology, Grenoble, France.
