Precise measurements of the CO2 gas transfer across the air-sea interface provide a better under- standing of the global carbon cycle. The air-sea CO2 fluxes are obtained by the eddy covariance method and the bulk met...Precise measurements of the CO2 gas transfer across the air-sea interface provide a better under- standing of the global carbon cycle. The air-sea CO2 fluxes are obtained by the eddy covariance method and the bulk method from a buoy observation in the northern Huanghai sea. The effects of buoy motion on flux calculated by the eddy covariance method are demonstrated. The research shows that a motion correction can improve the correlation coefficient between the C02 fluxes esti- mated from two different levels. Without the CO2-H20 cross-correlation correction which is termed as PKT correction, the air-sea CO2 fluxes estimated by eddy covariance method using the motion corrected data are nearly an order of magnitude larger than those estimated by the bulk method. After the CO2-H20 cross-correlation correction, some eddy covariance CO2 fluxes indeed become closer to the bulk CO2 flux, whereas some are overcorrected which are in response to small water vapor flux.展开更多
In the continuous development of electrochemical CO_(2) reduction (ECR), Cu-based electrocatalysts have received great attention, due to their unique ability to produce high value-added multicarbon products. Of partic...In the continuous development of electrochemical CO_(2) reduction (ECR), Cu-based electrocatalysts have received great attention, due to their unique ability to produce high value-added multicarbon products. Of particular interest are various Cu-comprising nanocrystals, not only because they usually show better catalytic properties than bulk materials, but also because their well-defined structures and highly tunable compositions facilitate in-depth mechanistic studies. This review aims to summarize the latest developments of electrocatalysts for ECR, with a focus on systems using Cu-comprising nanocrystals. We first give a general introduction to the field of ECR, covering the significance of this process, reaction mechanisms, catalyst evaluation criteria, and electrolytic cell configurations. Next, we discuss Cu-comprising nanocrystals developed for ECR by categorizing them into four groups: monometallic copper, copper-containing bimetals/multimetals, copper compounds, and copper–metal oxide hybrids;among these groups, we choose representative examples for detailed discussion on the synthetic methods, structural and compositional reaction sensitivities, and catalyst evolution during ECR. In the last section, we outline the challenges in this field from the fundamental and applicative aspects, and give perspectives on the expansion of catalyst varieties, the identification and preservation of active sites, and the exploration of industrially relevant operations for these nanocrystals. We hope the insights provided in this review will inspire the design and development of next-generation catalysts for ECR.展开更多
Recently, as a direct consequence of the dwindling world oil reserves and the growing awareness of the environmental problems associated with the use of coal as energy source, there is growing interest in cheaper, abu...Recently, as a direct consequence of the dwindling world oil reserves and the growing awareness of the environmental problems associated with the use of coal as energy source, there is growing interest in cheaper, abundant and cleaner burning methane. The Gas-to-Liquid technology offers perhaps the most attractive routes for the exploitation of the world huge and growing natural gas resources. Using this process the erstwhile stranded gas is converted to premium grade liquid fuels and chemicals that are easily transported. However, a widespread application of the GTL process is being hampered by economical and technical challenges. The high cost of synthesis gas, for instance, weighs heavily on the economics and competitiveness of the process limiting its wider application. This work presented a modified Gas-to-Liquid process that eliminates the costly synthesis gas production step. The proposed process utilized an alternative pathway for methane activation via the production of chloromethane derivatives which are then converted to hydrocarbons. It established that hydrocarbons mainly olefins can be economically produced from di- and tri-chloro- methanes over a typical iron-based Fischer Tropsch catalysts in a moving bed reactor at industrially relevant conditions. Some of the attractions of the proposed process include a) the elimination of the costly air separation plant requirement b) high process selectivity and c) significant reduction of carbon dioxide emissions thereby saving on feedstock loss and the costly CO2 removal and isolation processes.展开更多
The persistent rise in concentrations of greenhouse gases (GHGs) in the earth’s atmosphere is responsible for global warming and climate change. Besides the known source of GHGs emissions like energy, industry, and a...The persistent rise in concentrations of greenhouse gases (GHGs) in the earth’s atmosphere is responsible for global warming and climate change. Besides the known source of GHGs emissions like energy, industry, and agriculture, intrinsic emissions from natural inland water bodies like wetland, rivers, reservoirs, estuaries, etc. have also been identified as other hotspots of GHGs emission and gaining the attention of the scientific communities in recent times. Inland fisheries in India are threatened by climate changes such as a change in temperature, precipitation, droughts, storm, sea-level rise, saltwater intrusion, floods that affect mostly the production, productivity and ultimately affect the fishers’ livelihood. There are, however, different mitigation and adaptation strategies to cope with the effects of climate change. Carbon sequestration and other related management interventions are one of the options available minimizing GHGs emissions from inland open waters, particularly the wetlands and coastal mangroves which are well known worldwide for their significant role in the storage of carbon. Assessment of C efflux from exposed sediments in dry streams, reservoirs, lakes, rivers, and ponds into the atmosphere can be considered imperative for a better understanding of their role as a C-sink or as a C-source to the atmosphere.展开更多
The tight tuff reservoir is an unusual type of unconventional reservoir with strong heterogeneity.However,there is a lack of research on the microscopic pore structure that causes the heterogeneity of tuff reservoirs....The tight tuff reservoir is an unusual type of unconventional reservoir with strong heterogeneity.However,there is a lack of research on the microscopic pore structure that causes the heterogeneity of tuff reservoirs.Using the Chang 7 Formation in Ordos Basin,China as a case study,carbon-dioxide gas adsorption,nitrogen gas adsorption and high-pressure mercury injection are integrated to investigate the multi-scale pore structure characteristics of tuff reservoirs.Meanwhile,the fractal dimension is introduced to characterize the complexity of pore structure in tuff reservoirs.By this multi-experimental method,the quantitative characterizations of the full-range pore size distribution of four tuff types were obtained and compared in the size ranges of micropores,mesopores and macropores.Fractal dimension curves derived from full-range pores are divided into six segments as D1,D2,D3,D4,D5 and D6 corresponding to fractal characteristics of micropores,smaller mesopores,larger mesopores,smaller macropores,medium macropores and larger macropores,respectively.The macropore volume,average macropore radius and fractal dimension D5 significantly control petrophysical properties.The larger macropore volume,average macropore radius and D5 correspond to favorable pore structure and good reservoir quality,which provides new indexes for the tuff reservoir evaluation.This study enriches the understanding of the heterogeneity of pore structures and contributes to unconventional oil and gas exploration and development.展开更多
Active-phase engineering is regularly utilized to tune the selectivity of metal nanoparticles (NPs) in heterogeneous catalysis. However, the lack of understanding of the active phase in electrocatalysis has hampered...Active-phase engineering is regularly utilized to tune the selectivity of metal nanoparticles (NPs) in heterogeneous catalysis. However, the lack of understanding of the active phase in electrocatalysis has hampered the development of efficient catalysts for CO2 electroreduction. Herein, we report the systematic engineering of active phases of Pd NPs, which are exploited to select reaction pathways for CO2 electroreduction. In situ X-ray absorption spectroscopy, in situ attenuated total reflection-infrared spectroscopy, and density functional theory calculations suggest that the formation of a hydrogen-adsorbed Pd surface on a mixture of the α- and β-phases of a palladium-hydride core (α+β PdHx@PdHx) above -0.2 V (vs. a reversible hydrogen electrode) facilitates formate production via the HCOO intermediate, whereas the formation of a metallic Pd surface on the β-phase Pd hydride core (β PdHx@Pd) below -0.5 V promotes CO production via the COOH" intermediate. The main product, which is either formate or CO, can be selectively produced with high Faradaic efficiencies (〉90%) and mass activities in the potential window of 0.05 to -0.9 V with scalable application demonstration.展开更多
基金The National Basic Research Program of China under contract No. 2011CB403501the Public Science and Technology Research Funds Projects of Ocean of the State oceanic Administration of China under contract No. 200905012-9+1 种基金the Fund for Creative Research Groups by the National Natural Science Foundation of China under contract No. 41121064the Open Research Foundation for the key Laboratory of Ocean Circulation and Waves.Institute of Oceanology,Chinese Academy of Sciences of China under contract No.KLOCAW1207
文摘Precise measurements of the CO2 gas transfer across the air-sea interface provide a better under- standing of the global carbon cycle. The air-sea CO2 fluxes are obtained by the eddy covariance method and the bulk method from a buoy observation in the northern Huanghai sea. The effects of buoy motion on flux calculated by the eddy covariance method are demonstrated. The research shows that a motion correction can improve the correlation coefficient between the C02 fluxes esti- mated from two different levels. Without the CO2-H20 cross-correlation correction which is termed as PKT correction, the air-sea CO2 fluxes estimated by eddy covariance method using the motion corrected data are nearly an order of magnitude larger than those estimated by the bulk method. After the CO2-H20 cross-correlation correction, some eddy covariance CO2 fluxes indeed become closer to the bulk CO2 flux, whereas some are overcorrected which are in response to small water vapor flux.
基金This work was supported by the Thousand Talents Program for Distinguished Young Scholars,the Fundamental Research Funds for the Central Universities(2020CDJQY-A072)the Venture and Innovation Support Program for Chongqing Overseas Returnees(cx2020107).
文摘In the continuous development of electrochemical CO_(2) reduction (ECR), Cu-based electrocatalysts have received great attention, due to their unique ability to produce high value-added multicarbon products. Of particular interest are various Cu-comprising nanocrystals, not only because they usually show better catalytic properties than bulk materials, but also because their well-defined structures and highly tunable compositions facilitate in-depth mechanistic studies. This review aims to summarize the latest developments of electrocatalysts for ECR, with a focus on systems using Cu-comprising nanocrystals. We first give a general introduction to the field of ECR, covering the significance of this process, reaction mechanisms, catalyst evaluation criteria, and electrolytic cell configurations. Next, we discuss Cu-comprising nanocrystals developed for ECR by categorizing them into four groups: monometallic copper, copper-containing bimetals/multimetals, copper compounds, and copper–metal oxide hybrids;among these groups, we choose representative examples for detailed discussion on the synthetic methods, structural and compositional reaction sensitivities, and catalyst evolution during ECR. In the last section, we outline the challenges in this field from the fundamental and applicative aspects, and give perspectives on the expansion of catalyst varieties, the identification and preservation of active sites, and the exploration of industrially relevant operations for these nanocrystals. We hope the insights provided in this review will inspire the design and development of next-generation catalysts for ECR.
文摘Recently, as a direct consequence of the dwindling world oil reserves and the growing awareness of the environmental problems associated with the use of coal as energy source, there is growing interest in cheaper, abundant and cleaner burning methane. The Gas-to-Liquid technology offers perhaps the most attractive routes for the exploitation of the world huge and growing natural gas resources. Using this process the erstwhile stranded gas is converted to premium grade liquid fuels and chemicals that are easily transported. However, a widespread application of the GTL process is being hampered by economical and technical challenges. The high cost of synthesis gas, for instance, weighs heavily on the economics and competitiveness of the process limiting its wider application. This work presented a modified Gas-to-Liquid process that eliminates the costly synthesis gas production step. The proposed process utilized an alternative pathway for methane activation via the production of chloromethane derivatives which are then converted to hydrocarbons. It established that hydrocarbons mainly olefins can be economically produced from di- and tri-chloro- methanes over a typical iron-based Fischer Tropsch catalysts in a moving bed reactor at industrially relevant conditions. Some of the attractions of the proposed process include a) the elimination of the costly air separation plant requirement b) high process selectivity and c) significant reduction of carbon dioxide emissions thereby saving on feedstock loss and the costly CO2 removal and isolation processes.
文摘The persistent rise in concentrations of greenhouse gases (GHGs) in the earth’s atmosphere is responsible for global warming and climate change. Besides the known source of GHGs emissions like energy, industry, and agriculture, intrinsic emissions from natural inland water bodies like wetland, rivers, reservoirs, estuaries, etc. have also been identified as other hotspots of GHGs emission and gaining the attention of the scientific communities in recent times. Inland fisheries in India are threatened by climate changes such as a change in temperature, precipitation, droughts, storm, sea-level rise, saltwater intrusion, floods that affect mostly the production, productivity and ultimately affect the fishers’ livelihood. There are, however, different mitigation and adaptation strategies to cope with the effects of climate change. Carbon sequestration and other related management interventions are one of the options available minimizing GHGs emissions from inland open waters, particularly the wetlands and coastal mangroves which are well known worldwide for their significant role in the storage of carbon. Assessment of C efflux from exposed sediments in dry streams, reservoirs, lakes, rivers, and ponds into the atmosphere can be considered imperative for a better understanding of their role as a C-sink or as a C-source to the atmosphere.
基金supported by the Strategic Cooperation Technology Projects of CNPC and CUPB(No.ZLZX2020-02)the National Science and Technology Special(No.2017ZX05049-006-001)+1 种基金the National Natural Science Foundation of China(No.41602137)Science Foundation of China University of Petroleum,Beijing(No.2462020YXZZ022).
文摘The tight tuff reservoir is an unusual type of unconventional reservoir with strong heterogeneity.However,there is a lack of research on the microscopic pore structure that causes the heterogeneity of tuff reservoirs.Using the Chang 7 Formation in Ordos Basin,China as a case study,carbon-dioxide gas adsorption,nitrogen gas adsorption and high-pressure mercury injection are integrated to investigate the multi-scale pore structure characteristics of tuff reservoirs.Meanwhile,the fractal dimension is introduced to characterize the complexity of pore structure in tuff reservoirs.By this multi-experimental method,the quantitative characterizations of the full-range pore size distribution of four tuff types were obtained and compared in the size ranges of micropores,mesopores and macropores.Fractal dimension curves derived from full-range pores are divided into six segments as D1,D2,D3,D4,D5 and D6 corresponding to fractal characteristics of micropores,smaller mesopores,larger mesopores,smaller macropores,medium macropores and larger macropores,respectively.The macropore volume,average macropore radius and fractal dimension D5 significantly control petrophysical properties.The larger macropore volume,average macropore radius and D5 correspond to favorable pore structure and good reservoir quality,which provides new indexes for the tuff reservoir evaluation.This study enriches the understanding of the heterogeneity of pore structures and contributes to unconventional oil and gas exploration and development.
文摘Active-phase engineering is regularly utilized to tune the selectivity of metal nanoparticles (NPs) in heterogeneous catalysis. However, the lack of understanding of the active phase in electrocatalysis has hampered the development of efficient catalysts for CO2 electroreduction. Herein, we report the systematic engineering of active phases of Pd NPs, which are exploited to select reaction pathways for CO2 electroreduction. In situ X-ray absorption spectroscopy, in situ attenuated total reflection-infrared spectroscopy, and density functional theory calculations suggest that the formation of a hydrogen-adsorbed Pd surface on a mixture of the α- and β-phases of a palladium-hydride core (α+β PdHx@PdHx) above -0.2 V (vs. a reversible hydrogen electrode) facilitates formate production via the HCOO intermediate, whereas the formation of a metallic Pd surface on the β-phase Pd hydride core (β PdHx@Pd) below -0.5 V promotes CO production via the COOH" intermediate. The main product, which is either formate or CO, can be selectively produced with high Faradaic efficiencies (〉90%) and mass activities in the potential window of 0.05 to -0.9 V with scalable application demonstration.