The challenge of establishing top-down constraints for regional emissions of fossil fuel CO_(2)(FFCO_(2))arises from the difficulty in distinguishing between atmospheric CO_(2)concentrations released from fossil fuels...The challenge of establishing top-down constraints for regional emissions of fossil fuel CO_(2)(FFCO_(2))arises from the difficulty in distinguishing between atmospheric CO_(2)concentrations released from fossil fuels and background variability,particularly owing to the influence of terrestrial biospheric fluxes.This necessitates the development of a regional inversion methodology based on atmospheric CO_(2)observations to verify bottom-up estimations independently.This study presents a promising approach for estimating China's FFCO_(2)emissions by incorporating the model residual errors(MREs)of the column-averaged dry-air mole fractions of CO_(2)(XCO_(2))from FFCO_(2)emissions(MREff)retained in the analysis of natural flux optimization.China's FFCO_(2)emissions during the COVID-19 lockdown in 2020 are estimated using the GEOS-Chem adjoint model.The relationship between the MREff and FFCO_(2)is determined using the model based on a regional FFCO_(2)anomaly suggested by posterior NOx emissions from air-quality data assimilation.The MREff is typically one-tenth in magnitude,but some positively skewed outliers exceed 1 ppm because the prior emissions lack lockdown impacts,thereby exerting considerable observation forcing given the satellite retrieval uncertainties.We initialize the FFCO_(2)with posterior NOx emissions and optimize the colinear emission ratio.Synthetic data experiments demonstrate that this approach reduces the FFCO_(2)bias to less than 10%.The real-data experiments estimate 19%lower FFCO_(2)with GOSAT XCO_(2)and 26%lower with OCO-2 XCO_(2)than the bottom-up estimations.This study proves the feasibility of our regional FFCO_(2)inversion,highlighting the importance of addressing the outlier behaviors observed in satellite XCO_(2)retrievals.展开更多
There is a worldwide consensus that excessive anthropogenic carbon dioxide emissions will lead to global warming and other environmental problems.Supports from regulations and policies have gradually implemented in th...There is a worldwide consensus that excessive anthropogenic carbon dioxide emissions will lead to global warming and other environmental problems.Supports from regulations and policies have gradually implemented in this area.As one of the most discussed policies,the carbon emissions trading schemes(CETS)has an advantage in its price-oriented and cost-saving characteristics.In this paper,we analyze and assess the CETS effect from static and dynamic perspectives by applying provincial panel data covering a period ranging from 2004 to 2017.The CETS policy has a significant constraining effect on both carbon emissions and primary energy consumption.Compared to the other two uncertainties,namely the energy price uncertainty and the technology uncertainty,the carbon permit price uncertainty has a relatively smooth impact on the economy,which is being pursued consistently by the policymakers.展开更多
Examining the contribution of fossil fuel CO_(2) to the total CO_(2) changes in the atmosphere is of primary concern due to its alarming levels of fossil fuel emissions over the globe,specifically developing countries...Examining the contribution of fossil fuel CO_(2) to the total CO_(2) changes in the atmosphere is of primary concern due to its alarming levels of fossil fuel emissions over the globe,specifically developing countries.Atmospheric radiocarbon represents an important observational constraint and utilized to trace fossil fuel derived CO_(2)(CO_(2ff))in the atmosphere.For the first time,we have presented a detailed analysis on the spatial distribution of fossil fuel derived CO_(2)(CO_(2ff))over India using radiocarbon(Δ14C)measurements during three-year period.Analysis shows that theΔ14C values are varying between 29.33‰ to-34.06‰ across India in the year 2017,where highest value belongs to a location from Gujarat while lowest value belongs to a location from Chhattisgarh.Based on the14C patterns,spatial distributions of CO_(2ff) mole fractions have been determined over India and the calculated values of CO_(2ff) mole fractions are varying between 4.85 ppm to 26.59 ppm across India.It is also noticed that the highest CO_(2ff) mole fraction is observed as 26.59 ppm from a site in Chhattisgarh.CO_(2ff) mole fraction values from four high altitude sites are found to be varied between 4.85 ppm to 14.87 ppm.Effect of sampling different crop plants from the same growing season and different crop plant organs(grains,leaves,stems)on theΔ14C and CO_(2ff) have been studied.Annual and intra seasonal variations in theΔ14C and CO_(2ff) mole fractions have also been analyzed from a rural location(Dholpur,Rajasthan).展开更多
Developing an anthropogenic carbon dioxides(CO_(2))emissions monitoring and verification support(MVS)capacity is essential to support the Global Stocktake(GST)and ratchet up Nationally Determined Contributions(NDCs).T...Developing an anthropogenic carbon dioxides(CO_(2))emissions monitoring and verification support(MVS)capacity is essential to support the Global Stocktake(GST)and ratchet up Nationally Determined Contributions(NDCs).The 2019 IPCC refinement proposes top-down inversed CO_(2)emissions,primarily from fossil fuel(FFCO_(2)),as a viable emission dataset.Despite substantial progress in directly inferring FFCO_(2)emissions from CO_(2)observations,substantial challenges remain,particularly in distinguishing local CO_(2)enhancements from the high background due to the long atmospheric lifetime.Alternatively,using short-lived and co-emitted nitrogen dioxide(NO_(2))as a proxy in FFCO_(2)emission inversion has gained prominence.This methodology is broadly categorized into plume-based and emission ratios(ERs)-based inversion methods.In the plume-based methods,NO_(2)observations act as locators,constraints,and validators for deciphering CO_(2)plumes downwind of sources,typically at point source and city scales.The ERs-based inversion approach typically consists of two steps:inferring NO_(2)-based nitrogen oxides(NO_(x))emissions and converting NO_(x)to CO_(2)emissions using CO_(2)-to-NO_(x)ERs.While integrating NO_(2)observations into FFCO_(2)emission inversion offers advantages over the direct CO_(2)-based methods,uncertainties persist,including both structural and data-related uncertainties.Addressing these uncertainties is a primary focus for future research,which includes deploying nextgeneration satellites and developing advanced inversion systems.Besides,data caveats are necessary when releasing data to users to prevent potential misuse.Advancing NO_(2)-based CO_(2)emission inversion requires interdisciplinary collaboration across multiple communities of remote sensing,emission inventory,transport model improvement,and atmospheric inversion algorithm development.展开更多
Novel technologies in consideration of industrial sustainability(IS)are in urgent need to satisfy the increasing demands from the society.IS realizes the production of materials while maintaining environmental and res...Novel technologies in consideration of industrial sustainability(IS)are in urgent need to satisfy the increasing demands from the society.IS realizes the production of materials while maintaining environmental and resource sustainability.The chemical materials used in CO2 capture and storage(CCS)technologies play a significant role in the disposal of greenhouse gas emissions coming from large stationary fossil-fired power plants,which breaks the principle of IS and brings severe environmental problems.This study aims at providing a detailed review of first-principles modeling(density functional theory,DFT)of materials in CO2 capture technologies.DFT analysis provides insight into the atomic properties of the studied systems and builds an efficient guidance of the future design of the materials used in CO2 capture technologies.Major materials including oxygen carriers,metal organic frameworks,membranes,zeolites,ionic liquids and some other promising candidates are considered.The computational studies bring the outcomes of the adsorption behaviors,structural characteristics and accurate force fields of the studied materials in short turn-around times at low cost.This review can stimulate the design of novel materials with specific target of CO2 capture and promote the industrial sustainability of fossil fuel combustion technologies.展开更多
In this article, we calculate China's Mainland’s CO2 emission of fossil fuel consumption from 1991 to 2010 following the apparent consumption method recommend by IPCC： （i） the scale of CO2 emissions has increa...In this article, we calculate China's Mainland’s CO2 emission of fossil fuel consumption from 1991 to 2010 following the apparent consumption method recommend by IPCC： （i） the scale of CO2 emissions has increased nearly to 4 times as that in 1991; （ii） coal consumption constitutes the highest proportion due to the richness of coal resources in China; （iii） per capita CO2 emission has increased from 1.98 to 5.57 t CO2 ; （iv） carbon emission intensity declined significantly from 6.66 to 1.07 kg CO2 USD -1 , but recently it tends to be stable; and （v） regional develop gaps remain in China's Mainland, for according to the provincial data, in many developing regions economic increase over-reliance on fossil fuel consumption. China has made the promises and already taken actions to deal with the high carbon emission. Comprehensively considering the sustainability of development and the uncertainties remaining in global climate change, healthier structures of industry, intensive usage of fossil fuel, and a more balanced development pattern among the southern, central and western China should be put more emphasis.展开更多
Carbon dioxide rise, swing and spread (seasonal fluctuations) are addressed in this study. Actual CO<sub>2</sub> concentrations were used rather than dry values. The dry values are artificially higher beca...Carbon dioxide rise, swing and spread (seasonal fluctuations) are addressed in this study. Actual CO<sub>2</sub> concentrations were used rather than dry values. The dry values are artificially higher because water vapor must be removed in order for the NDIR instrument to work and is not factored back into the reported numbers. Articles addressing these observations express opinions that are divergent and often conflicting. This investigation resolves many of those inconsistencies. The data were obtained from many measuring stations at various latitudes since 1972 and then graphical compared to changes in sea temperatures, fossil fuel emissions, humidity, and seasonal ice and snow changes. In analyzing the data, various parameters were addressed including: variability, R squared curve values, correlations between curves, residence times, absorption percentages, and Troposphere effects. Mass balance calculations were also made to corroborate viability. The CO<sub>2</sub> “rise” over a 33-year period from a slight ocean temperature increase (0.7°F) contributed 2.3 percent of the total rise while fossil fuel emissions contributed 1.5 percent. The overwhelming majority (60 ppmv, 96%+) was caused by other factors including ocean and land biology as well potential errors in fundamental hypotheses. With respect to “spread” (seasonal CO<sub>2</sub> fluctuations) at the Polar Circles, graphical analysis with high correlations supported by mass balance calculations confirm that ice and snow are the primary cause and explain why the concentrations are the highest at these cold locations. The global variations in “swing” remain uncertain.展开更多
If substantial amounts of CO_(2),which according to actual scenarios may in the future be captured from industrial processes and power generation,shall be utilized effectively,scalable energy efficient technologies wi...If substantial amounts of CO_(2),which according to actual scenarios may in the future be captured from industrial processes and power generation,shall be utilized effectively,scalable energy efficient technologies will be required.Thus,a survey was performed to assess a large variety of applications utilizing CO_(2) chemically(e.g.,production of synthesis-gas,methanol synthesis),biologically(e.g.,CO_(2) as fertilizer in green houses,production of algae),or physically(enhancement of fossil fuel recovery,use as refrigerant).For each of the processes,material and energy balances were set up.Starting with pure CO_(2) at standard conditions,expenditure for transport and further process specific treatment were included.Based on these calculations,the avoidance of greenhouse gas emissions by applying the discussed technologies was evaluated.Based on the currently available technologies,applications for enhanced fossil fuel recovery turn out to be most attractive regarding the potential of utilizing large quantities of CO_(2)(total capacity>1000 Gt CO_(2))and producing significant amounts of marketable products on one hand and having good energy and material balances on the other hand(t_(CO_(2)-emitted)/t_(CO_(2)-utilized)<0.2-0.4).Nevertheless,large scale chemical fixation of CO_(2)providing valuable products like fuels is worth considering,if carbon-free energy sources are used to provide the process energy and H2 being essential as a reactant in a lot of chemical processes(e.g.,production of DME:t_(CO_(2)-emitted)/t_(CO_(2)-utilized)>0.34).Biological processes such as CO_(2) fixation using microalgae look attractive as long as energy and CO_(2) balance are considered.However,the development of effective photobioreactors for growing algae with low requirements for footprint area is a challenge.展开更多
基金jointly supported by the National Key Research and Development Plan(Grant No.2023YFB3907405)the National Natural Science Foundation of China(Grant No.42175132)the Chinese Academy of Sciences Project for Young Scientists in Basic Research(Grant No.YSBR-037)。
文摘The challenge of establishing top-down constraints for regional emissions of fossil fuel CO_(2)(FFCO_(2))arises from the difficulty in distinguishing between atmospheric CO_(2)concentrations released from fossil fuels and background variability,particularly owing to the influence of terrestrial biospheric fluxes.This necessitates the development of a regional inversion methodology based on atmospheric CO_(2)observations to verify bottom-up estimations independently.This study presents a promising approach for estimating China's FFCO_(2)emissions by incorporating the model residual errors(MREs)of the column-averaged dry-air mole fractions of CO_(2)(XCO_(2))from FFCO_(2)emissions(MREff)retained in the analysis of natural flux optimization.China's FFCO_(2)emissions during the COVID-19 lockdown in 2020 are estimated using the GEOS-Chem adjoint model.The relationship between the MREff and FFCO_(2)is determined using the model based on a regional FFCO_(2)anomaly suggested by posterior NOx emissions from air-quality data assimilation.The MREff is typically one-tenth in magnitude,but some positively skewed outliers exceed 1 ppm because the prior emissions lack lockdown impacts,thereby exerting considerable observation forcing given the satellite retrieval uncertainties.We initialize the FFCO_(2)with posterior NOx emissions and optimize the colinear emission ratio.Synthetic data experiments demonstrate that this approach reduces the FFCO_(2)bias to less than 10%.The real-data experiments estimate 19%lower FFCO_(2)with GOSAT XCO_(2)and 26%lower with OCO-2 XCO_(2)than the bottom-up estimations.This study proves the feasibility of our regional FFCO_(2)inversion,highlighting the importance of addressing the outlier behaviors observed in satellite XCO_(2)retrievals.
基金The authors are grateful for the financial supportive from the National Natural Science Foundation of China(71473010)and(41701635).
文摘There is a worldwide consensus that excessive anthropogenic carbon dioxide emissions will lead to global warming and other environmental problems.Supports from regulations and policies have gradually implemented in this area.As one of the most discussed policies,the carbon emissions trading schemes(CETS)has an advantage in its price-oriented and cost-saving characteristics.In this paper,we analyze and assess the CETS effect from static and dynamic perspectives by applying provincial panel data covering a period ranging from 2004 to 2017.The CETS policy has a significant constraining effect on both carbon emissions and primary energy consumption.Compared to the other two uncertainties,namely the energy price uncertainty and the technology uncertainty,the carbon permit price uncertainty has a relatively smooth impact on the economy,which is being pursued consistently by the policymakers.
文摘Examining the contribution of fossil fuel CO_(2) to the total CO_(2) changes in the atmosphere is of primary concern due to its alarming levels of fossil fuel emissions over the globe,specifically developing countries.Atmospheric radiocarbon represents an important observational constraint and utilized to trace fossil fuel derived CO_(2)(CO_(2ff))in the atmosphere.For the first time,we have presented a detailed analysis on the spatial distribution of fossil fuel derived CO_(2)(CO_(2ff))over India using radiocarbon(Δ14C)measurements during three-year period.Analysis shows that theΔ14C values are varying between 29.33‰ to-34.06‰ across India in the year 2017,where highest value belongs to a location from Gujarat while lowest value belongs to a location from Chhattisgarh.Based on the14C patterns,spatial distributions of CO_(2ff) mole fractions have been determined over India and the calculated values of CO_(2ff) mole fractions are varying between 4.85 ppm to 26.59 ppm across India.It is also noticed that the highest CO_(2ff) mole fraction is observed as 26.59 ppm from a site in Chhattisgarh.CO_(2ff) mole fraction values from four high altitude sites are found to be varied between 4.85 ppm to 14.87 ppm.Effect of sampling different crop plants from the same growing season and different crop plant organs(grains,leaves,stems)on theΔ14C and CO_(2ff) have been studied.Annual and intra seasonal variations in theΔ14C and CO_(2ff) mole fractions have also been analyzed from a rural location(Dholpur,Rajasthan).
基金supported by the National Natural Science Foundation of China(No.42105094).
文摘Developing an anthropogenic carbon dioxides(CO_(2))emissions monitoring and verification support(MVS)capacity is essential to support the Global Stocktake(GST)and ratchet up Nationally Determined Contributions(NDCs).The 2019 IPCC refinement proposes top-down inversed CO_(2)emissions,primarily from fossil fuel(FFCO_(2)),as a viable emission dataset.Despite substantial progress in directly inferring FFCO_(2)emissions from CO_(2)observations,substantial challenges remain,particularly in distinguishing local CO_(2)enhancements from the high background due to the long atmospheric lifetime.Alternatively,using short-lived and co-emitted nitrogen dioxide(NO_(2))as a proxy in FFCO_(2)emission inversion has gained prominence.This methodology is broadly categorized into plume-based and emission ratios(ERs)-based inversion methods.In the plume-based methods,NO_(2)observations act as locators,constraints,and validators for deciphering CO_(2)plumes downwind of sources,typically at point source and city scales.The ERs-based inversion approach typically consists of two steps:inferring NO_(2)-based nitrogen oxides(NO_(x))emissions and converting NO_(x)to CO_(2)emissions using CO_(2)-to-NO_(x)ERs.While integrating NO_(2)observations into FFCO_(2)emission inversion offers advantages over the direct CO_(2)-based methods,uncertainties persist,including both structural and data-related uncertainties.Addressing these uncertainties is a primary focus for future research,which includes deploying nextgeneration satellites and developing advanced inversion systems.Besides,data caveats are necessary when releasing data to users to prevent potential misuse.Advancing NO_(2)-based CO_(2)emission inversion requires interdisciplinary collaboration across multiple communities of remote sensing,emission inventory,transport model improvement,and atmospheric inversion algorithm development.
基金support provided by the Chinese Scholarship Council to develop this research
文摘Novel technologies in consideration of industrial sustainability(IS)are in urgent need to satisfy the increasing demands from the society.IS realizes the production of materials while maintaining environmental and resource sustainability.The chemical materials used in CO2 capture and storage(CCS)technologies play a significant role in the disposal of greenhouse gas emissions coming from large stationary fossil-fired power plants,which breaks the principle of IS and brings severe environmental problems.This study aims at providing a detailed review of first-principles modeling(density functional theory,DFT)of materials in CO2 capture technologies.DFT analysis provides insight into the atomic properties of the studied systems and builds an efficient guidance of the future design of the materials used in CO2 capture technologies.Major materials including oxygen carriers,metal organic frameworks,membranes,zeolites,ionic liquids and some other promising candidates are considered.The computational studies bring the outcomes of the adsorption behaviors,structural characteristics and accurate force fields of the studied materials in short turn-around times at low cost.This review can stimulate the design of novel materials with specific target of CO2 capture and promote the industrial sustainability of fossil fuel combustion technologies.
基金the National Natural Science Foundation of China (31070384)
文摘In this article, we calculate China's Mainland’s CO2 emission of fossil fuel consumption from 1991 to 2010 following the apparent consumption method recommend by IPCC： （i） the scale of CO2 emissions has increased nearly to 4 times as that in 1991; （ii） coal consumption constitutes the highest proportion due to the richness of coal resources in China; （iii） per capita CO2 emission has increased from 1.98 to 5.57 t CO2 ; （iv） carbon emission intensity declined significantly from 6.66 to 1.07 kg CO2 USD -1 , but recently it tends to be stable; and （v） regional develop gaps remain in China's Mainland, for according to the provincial data, in many developing regions economic increase over-reliance on fossil fuel consumption. China has made the promises and already taken actions to deal with the high carbon emission. Comprehensively considering the sustainability of development and the uncertainties remaining in global climate change, healthier structures of industry, intensive usage of fossil fuel, and a more balanced development pattern among the southern, central and western China should be put more emphasis.
文摘Carbon dioxide rise, swing and spread (seasonal fluctuations) are addressed in this study. Actual CO<sub>2</sub> concentrations were used rather than dry values. The dry values are artificially higher because water vapor must be removed in order for the NDIR instrument to work and is not factored back into the reported numbers. Articles addressing these observations express opinions that are divergent and often conflicting. This investigation resolves many of those inconsistencies. The data were obtained from many measuring stations at various latitudes since 1972 and then graphical compared to changes in sea temperatures, fossil fuel emissions, humidity, and seasonal ice and snow changes. In analyzing the data, various parameters were addressed including: variability, R squared curve values, correlations between curves, residence times, absorption percentages, and Troposphere effects. Mass balance calculations were also made to corroborate viability. The CO<sub>2</sub> “rise” over a 33-year period from a slight ocean temperature increase (0.7°F) contributed 2.3 percent of the total rise while fossil fuel emissions contributed 1.5 percent. The overwhelming majority (60 ppmv, 96%+) was caused by other factors including ocean and land biology as well potential errors in fundamental hypotheses. With respect to “spread” (seasonal CO<sub>2</sub> fluctuations) at the Polar Circles, graphical analysis with high correlations supported by mass balance calculations confirm that ice and snow are the primary cause and explain why the concentrations are the highest at these cold locations. The global variations in “swing” remain uncertain.
文摘If substantial amounts of CO_(2),which according to actual scenarios may in the future be captured from industrial processes and power generation,shall be utilized effectively,scalable energy efficient technologies will be required.Thus,a survey was performed to assess a large variety of applications utilizing CO_(2) chemically(e.g.,production of synthesis-gas,methanol synthesis),biologically(e.g.,CO_(2) as fertilizer in green houses,production of algae),or physically(enhancement of fossil fuel recovery,use as refrigerant).For each of the processes,material and energy balances were set up.Starting with pure CO_(2) at standard conditions,expenditure for transport and further process specific treatment were included.Based on these calculations,the avoidance of greenhouse gas emissions by applying the discussed technologies was evaluated.Based on the currently available technologies,applications for enhanced fossil fuel recovery turn out to be most attractive regarding the potential of utilizing large quantities of CO_(2)(total capacity>1000 Gt CO_(2))and producing significant amounts of marketable products on one hand and having good energy and material balances on the other hand(t_(CO_(2)-emitted)/t_(CO_(2)-utilized)<0.2-0.4).Nevertheless,large scale chemical fixation of CO_(2)providing valuable products like fuels is worth considering,if carbon-free energy sources are used to provide the process energy and H2 being essential as a reactant in a lot of chemical processes(e.g.,production of DME:t_(CO_(2)-emitted)/t_(CO_(2)-utilized)>0.34).Biological processes such as CO_(2) fixation using microalgae look attractive as long as energy and CO_(2) balance are considered.However,the development of effective photobioreactors for growing algae with low requirements for footprint area is a challenge.
