1.Challenges circular methane energy systems In recent decades,methane-based energy systems have rapidly gained traction across the globe because of the increasing availability of low-cost methane production capacity....1.Challenges circular methane energy systems In recent decades,methane-based energy systems have rapidly gained traction across the globe because of the increasing availability of low-cost methane production capacity.However,fossil methane production and combustion lead to large greenhouse gas emissions,contributing to climate change[1].展开更多
Electrochemical reduction of CO_(2)into high-value hydrocarbons and alcohols by using Cu-based catalysts is a promising and attractive technology for CO_(2)capture and utilization,resulting from their high catalytic a...Electrochemical reduction of CO_(2)into high-value hydrocarbons and alcohols by using Cu-based catalysts is a promising and attractive technology for CO_(2)capture and utilization,resulting from their high catalytic activity and selectivity.The mobility and accessibility of active sites in Cubased catalysts significantly hinder the development of efficient Cu-based catalysts for CO_(2)electrochemical reduction reaction(CO_(2)RR).Herein,a facile and effective strategy is developed to engineer accessible and structural stable Cu sites by incorporating single atomic Cu into the nitrogen cavities of the host graphitic carbon nitride(g-C_(3)N_(4))as the active sites for CO_(2)-to-CH_(4)conversion in CO_(2)RR.By regulating the coordination and density of Cu sites in g-C_(3)N_(4),an optimal catalyst corresponding to a one Cu atom in one nitrogen cavity reaches the highest CH_(4)Faraday efficiency of 49.04%and produces the products with a high CH_(4)/C_(2)H_(4)ratio over 9.This work provides the first experimental study on g-C_(3)N_(4)-supported single Cu atom catalyst for efficient CH_(4)production from CO_(2)RR and suggests a principle in designing highly stable and selective high-efficiency Cu-based catalysts for CO_(2)RR by engineering Cu active sites in 2D materials with porous crystal structures.展开更多
Long-term stability test of Mo/HZSM-5-N catalysts(HZSM-5-N stands for nano-sized HZSM-5) in methane dehydroaromatization(MDA)reaction has been performed with periodic CH4-H2 switch at 1033-1073 K for more than 100...Long-term stability test of Mo/HZSM-5-N catalysts(HZSM-5-N stands for nano-sized HZSM-5) in methane dehydroaromatization(MDA)reaction has been performed with periodic CH4-H2 switch at 1033-1073 K for more than 1000 h.During this test,methane conversion ranges from 13% to 16%,and mean yield to aromatics(i.e.benzene and naphthalene) exceeds 10%.N2-physisorption,XRD,NMR and TPO measurements were performed for the used Mo/HZSM-5 catalysts and coke deposition,and the results revealed that the periodic hydrogenation can effectively suppress coke deposition by removing the inert aromatic-type coke,thus ensuring Mo/HZSM-5 partly maintained its activity even in the presence of large amount of coke deposition.The effect of zeolite particle size on the catalytic activity was also explored,and the results showed that the nano-sized zeolite with low diffusion resistance performed better.It is recognized that the size effect was enhanced by reaction time,and it became more remarkable in a long-term MDA reaction even at a low space velocity.展开更多
Samples of methane molecules grade diameter channel CHA-type molecular sieves(Chabazite-K, SAPO-34 and SSZ-13) were investigated using the adsorption separation of CH4/N2 mixtures. The isotherms recorded for CH4 and N...Samples of methane molecules grade diameter channel CHA-type molecular sieves(Chabazite-K, SAPO-34 and SSZ-13) were investigated using the adsorption separation of CH4/N2 mixtures. The isotherms recorded for CH4 and N2 follow a typical type-Ι behavior, which were fitted well with the Sips model(R2>0.999) and the selectivity was calculated using IAST theory. The results reveal that Chabazite-K has the highest selectivity(SCH4/N= 5.5).2 SSZ-13 has the largest capacity, which can adsorb up to a maximum of 30.957 cm3·g-1(STP) of CH4, due to it having the largest pore volume and surface area, but the lowest selectivity(SCH4/N2= 2.5). From the breakthrough test, we can conclude that SSZ-13 may be a suitable candidate for the recovery of CH4 from low concentration methane(CH4<20%) based on its larger pore volume and higher CH4 capacity. Chabazite-K is more suited to the separation of high concentration methane(CH4>50%) due to its higher selectivity.展开更多
Adsorption isotherms of carbon dioxide (CO2), methane (CH4), and nitrogen (N2) on Hβand sodium exchanged β-zeolite (Naβ) were volumetrically measured at 273 and 303 K. The results show that all isotherms we...Adsorption isotherms of carbon dioxide (CO2), methane (CH4), and nitrogen (N2) on Hβand sodium exchanged β-zeolite (Naβ) were volumetrically measured at 273 and 303 K. The results show that all isotherms were of Brunauer type I and well correlated with Langmuir-Freundlich model. After sodium ions exchange, the adsorption amounts of three adsorbates increased, while the increase magnitude of CO2 adsorption capacity was much higher than that of CH4 and N2. The selectivities of CO2 over CH4 and CO2 over N2 enhanced after sodium exchange. Also, the initial heat of adsorption data implied a stronger interaction of CO2 molecules with Na+ ions in Naβ . These results can be attributed to the larger electrostatic interaction of CO2 with extraframework cations in zeolites. However, Naβ showed a decrease in the selectivity of CH4 over N2, which can be ascribed to the moderate affinity of N2 with Naβ. The variation of isosteric heats of adsorption as a function of loading indicates that the adsorption of CO2 in Naβ presents an energetically heterogeneous profile. On the contrary, the adsorption of CH4 was found to be essentially homogeneous, which suggests the dispersion interaction between CH4 and lattice oxygen atoms, and such interaction does not depend on the exchangeable cations of zeolite.展开更多
The methane(CH4) emissions from municipal solid waste(MSW) landfills in China in 2007 were estimated based on database of the three-dimensional emission factors matrix and point sources, by an IPCC recommended FOD(fir...The methane(CH4) emissions from municipal solid waste(MSW) landfills in China in 2007 were estimated based on database of the three-dimensional emission factors matrix and point sources, by an IPCC recommended FOD(firstorder decay) model. The location, capacity and age of landfills constitute the three dimensions of the emission factors matrix, which were obtained by laboratory analysis and in situ investigation. Key parameters such as waste composition,degradable organic carbon ratio, CH4 correction factor, oxidation factor and recovery rate, were carefully analyzed in terms of these three dimensions. The point sources database consists of 2,107 MSW landfills in cities and towns of China in 2007. The results show that the CH4 emissions from MSW landfills were 1.186 Mt in 2007. Compared with the CH4 emissions of 2.20 Mt in 2005, the significant discrepancy mainly comes from statistical data of landfills, e.g., number of landfills and amount of waste disposed in landfills. CH4 emissions were lower than 700 t for most of the landfills, whereas there were 279 landfills with emissions larger than 1,000 t, and only 10 landfills with emissions larger than 10,000 t.Jiangsu province ranks the largest emitter with 98,700 t while Tibet is the smallest emitter with 2,100 t. In general,the emissions from eastern provinces, such as Jiangsu, Guangdong and Zhejiang, were larger than those from western provinces, such as Ningxia, Tibet and Qinghai.展开更多
Methane (OH4), carbon dioxide (CO2) and nitrous oxide (N2O) are known to be major greenhouse gases that contribute to global warming. To identify the flux dynamics of these greenhouse gases is, therefore, of gre...Methane (OH4), carbon dioxide (CO2) and nitrous oxide (N2O) are known to be major greenhouse gases that contribute to global warming. To identify the flux dynamics of these greenhouse gases is, therefore, of great significance. In this paper, we conducted a comparative study on an alpine grassland and alpine wetland at the Bayinbuluk Grassland Eco-system Research Station, Chinese Academy of Sciences. By using opaque, static, manual stainless steel chambers and gas chromatography, we measured the fluxes of CH4, N2O and CO2 from the grassland and wetland through an in situ monitoring study from May 2010 to October 2012. The mean flux rates of CH4, N2O and CO2 for the experimental alpine wetland in the growing season (from May to October) were estimated at 322.4 μg/(m2.h), 16.7 μg/(m2.h) and 76.7 mg/(m2.h), respectively; and the values for the alpine grassland were -88.2 μg/(m2.h), 12.7 μg/(m2.h), 57.3 mg/(m2.h), respectively. The gas fluxes showed large seasonal and annual variations, suggesting weak fluxes in the non-growing season. The relationships between these gas fluxes and environmental factors were analyzed for the two alpine ecosystems. The results showed that air temperature, precipitation, soil temperature and soil moisture can greatly influence the fluxes of CH4, N2O and CO2, but the alpine grassland and alpine wetland showed different feedback mechanisms under the same climate and environmental conditions.展开更多
基金funding from the European Research Council (ERC)under grant agreement no.834134 (WATUSO)VLAIO for Moonshot funding (ARCLATH,No.HBC.2019.0110 and ARCLATH2,No.HBC.2021.0254)+3 种基金supported by the Flemish Government as an international research infrastructure (I001321N)infrastructure support by Department EWI via the Hermes Fund (AH.2016.134)the Hercules Foundation (AKUL/13/21)FWO Vlaanderen for an FWO-SB fellowship。
文摘1.Challenges circular methane energy systems In recent decades,methane-based energy systems have rapidly gained traction across the globe because of the increasing availability of low-cost methane production capacity.However,fossil methane production and combustion lead to large greenhouse gas emissions,contributing to climate change[1].
基金This work was supported by the Fundamental Research Funds for the Central Universities(2232021A-02 and 2232023Y-01)the National Natural Science Foundation of China(Nos.52122312,22209024 and 22202183).
文摘Electrochemical reduction of CO_(2)into high-value hydrocarbons and alcohols by using Cu-based catalysts is a promising and attractive technology for CO_(2)capture and utilization,resulting from their high catalytic activity and selectivity.The mobility and accessibility of active sites in Cubased catalysts significantly hinder the development of efficient Cu-based catalysts for CO_(2)electrochemical reduction reaction(CO_(2)RR).Herein,a facile and effective strategy is developed to engineer accessible and structural stable Cu sites by incorporating single atomic Cu into the nitrogen cavities of the host graphitic carbon nitride(g-C_(3)N_(4))as the active sites for CO_(2)-to-CH_(4)conversion in CO_(2)RR.By regulating the coordination and density of Cu sites in g-C_(3)N_(4),an optimal catalyst corresponding to a one Cu atom in one nitrogen cavity reaches the highest CH_(4)Faraday efficiency of 49.04%and produces the products with a high CH_(4)/C_(2)H_(4)ratio over 9.This work provides the first experimental study on g-C_(3)N_(4)-supported single Cu atom catalyst for efficient CH_(4)production from CO_(2)RR and suggests a principle in designing highly stable and selective high-efficiency Cu-based catalysts for CO_(2)RR by engineering Cu active sites in 2D materials with porous crystal structures.
基金financially supported by the"Strategic Priority Research Program"of Chinese Academy of Sciences(No.XDA09030101)the National Natural Science Foundation of China(No.21103181 and 21473185)+1 种基金DICP Fundamental Research Program for Clean Energy(DICP M201301)Shaanxi Yanchang Petroleum Group Co.Ltd
文摘Long-term stability test of Mo/HZSM-5-N catalysts(HZSM-5-N stands for nano-sized HZSM-5) in methane dehydroaromatization(MDA)reaction has been performed with periodic CH4-H2 switch at 1033-1073 K for more than 1000 h.During this test,methane conversion ranges from 13% to 16%,and mean yield to aromatics(i.e.benzene and naphthalene) exceeds 10%.N2-physisorption,XRD,NMR and TPO measurements were performed for the used Mo/HZSM-5 catalysts and coke deposition,and the results revealed that the periodic hydrogenation can effectively suppress coke deposition by removing the inert aromatic-type coke,thus ensuring Mo/HZSM-5 partly maintained its activity even in the presence of large amount of coke deposition.The effect of zeolite particle size on the catalytic activity was also explored,and the results showed that the nano-sized zeolite with low diffusion resistance performed better.It is recognized that the size effect was enhanced by reaction time,and it became more remarkable in a long-term MDA reaction even at a low space velocity.
基金financial support from the National Natural Science Foundation of China (Nos. 51672186, 21676175)
文摘Samples of methane molecules grade diameter channel CHA-type molecular sieves(Chabazite-K, SAPO-34 and SSZ-13) were investigated using the adsorption separation of CH4/N2 mixtures. The isotherms recorded for CH4 and N2 follow a typical type-Ι behavior, which were fitted well with the Sips model(R2>0.999) and the selectivity was calculated using IAST theory. The results reveal that Chabazite-K has the highest selectivity(SCH4/N= 5.5).2 SSZ-13 has the largest capacity, which can adsorb up to a maximum of 30.957 cm3·g-1(STP) of CH4, due to it having the largest pore volume and surface area, but the lowest selectivity(SCH4/N2= 2.5). From the breakthrough test, we can conclude that SSZ-13 may be a suitable candidate for the recovery of CH4 from low concentration methane(CH4<20%) based on its larger pore volume and higher CH4 capacity. Chabazite-K is more suited to the separation of high concentration methane(CH4>50%) due to its higher selectivity.
基金supported by the Doctoral Program of Higher Education(Project 200402910050)the Program for Changiiang Scholars and Innovative Research Team in University(No.IRT0732)Major Basic Research Project of Natural Science Foundation of Jiangsu Province Colleges(No.08KJA530001)
文摘Adsorption isotherms of carbon dioxide (CO2), methane (CH4), and nitrogen (N2) on Hβand sodium exchanged β-zeolite (Naβ) were volumetrically measured at 273 and 303 K. The results show that all isotherms were of Brunauer type I and well correlated with Langmuir-Freundlich model. After sodium ions exchange, the adsorption amounts of three adsorbates increased, while the increase magnitude of CO2 adsorption capacity was much higher than that of CH4 and N2. The selectivities of CO2 over CH4 and CO2 over N2 enhanced after sodium exchange. Also, the initial heat of adsorption data implied a stronger interaction of CO2 molecules with Na+ ions in Naβ . These results can be attributed to the larger electrostatic interaction of CO2 with extraframework cations in zeolites. However, Naβ showed a decrease in the selectivity of CH4 over N2, which can be ascribed to the moderate affinity of N2 with Naβ. The variation of isosteric heats of adsorption as a function of loading indicates that the adsorption of CO2 in Naβ presents an energetically heterogeneous profile. On the contrary, the adsorption of CH4 was found to be essentially homogeneous, which suggests the dispersion interaction between CH4 and lattice oxygen atoms, and such interaction does not depend on the exchangeable cations of zeolite.
基金funded by the Project Study on Key Issues of China City Carbon Emission Inventory (No. 41101500)supported by National Natural Science Foundation of China
文摘The methane(CH4) emissions from municipal solid waste(MSW) landfills in China in 2007 were estimated based on database of the three-dimensional emission factors matrix and point sources, by an IPCC recommended FOD(firstorder decay) model. The location, capacity and age of landfills constitute the three dimensions of the emission factors matrix, which were obtained by laboratory analysis and in situ investigation. Key parameters such as waste composition,degradable organic carbon ratio, CH4 correction factor, oxidation factor and recovery rate, were carefully analyzed in terms of these three dimensions. The point sources database consists of 2,107 MSW landfills in cities and towns of China in 2007. The results show that the CH4 emissions from MSW landfills were 1.186 Mt in 2007. Compared with the CH4 emissions of 2.20 Mt in 2005, the significant discrepancy mainly comes from statistical data of landfills, e.g., number of landfills and amount of waste disposed in landfills. CH4 emissions were lower than 700 t for most of the landfills, whereas there were 279 landfills with emissions larger than 1,000 t, and only 10 landfills with emissions larger than 10,000 t.Jiangsu province ranks the largest emitter with 98,700 t while Tibet is the smallest emitter with 2,100 t. In general,the emissions from eastern provinces, such as Jiangsu, Guangdong and Zhejiang, were larger than those from western provinces, such as Ningxia, Tibet and Qinghai.
基金funded by the National Basic Research Program of China (2009CB825103)the National Natural Science Foundation of China (41340041)the West Light Foundation of the Chinese Academy of Sciences (XBBS201206)
文摘Methane (OH4), carbon dioxide (CO2) and nitrous oxide (N2O) are known to be major greenhouse gases that contribute to global warming. To identify the flux dynamics of these greenhouse gases is, therefore, of great significance. In this paper, we conducted a comparative study on an alpine grassland and alpine wetland at the Bayinbuluk Grassland Eco-system Research Station, Chinese Academy of Sciences. By using opaque, static, manual stainless steel chambers and gas chromatography, we measured the fluxes of CH4, N2O and CO2 from the grassland and wetland through an in situ monitoring study from May 2010 to October 2012. The mean flux rates of CH4, N2O and CO2 for the experimental alpine wetland in the growing season (from May to October) were estimated at 322.4 μg/(m2.h), 16.7 μg/(m2.h) and 76.7 mg/(m2.h), respectively; and the values for the alpine grassland were -88.2 μg/(m2.h), 12.7 μg/(m2.h), 57.3 mg/(m2.h), respectively. The gas fluxes showed large seasonal and annual variations, suggesting weak fluxes in the non-growing season. The relationships between these gas fluxes and environmental factors were analyzed for the two alpine ecosystems. The results showed that air temperature, precipitation, soil temperature and soil moisture can greatly influence the fluxes of CH4, N2O and CO2, but the alpine grassland and alpine wetland showed different feedback mechanisms under the same climate and environmental conditions.