Solid sorbents with enhanced capacity and selectivity towards CO2 are crucial in the design of an efficient capture process.Among the possible alternatives,K2CO3-doped activated carbons have shown high CO2 capture cap...Solid sorbents with enhanced capacity and selectivity towards CO2 are crucial in the design of an efficient capture process.Among the possible alternatives,K2CO3-doped activated carbons have shown high CO2 capture capacity and rapid carbonation reaction rate.In this work,a sustainable and low-cost approach is developed with a biomass-based activated carbon or biocarbon as support.The CO2 capture performance in cyclic sorption–desorption operation and the sorption kinetics have been investigated under different scenarios in a purpose-built fixed-bed set-up.Independent of the H2O concentration in the flue gas,a constant relative humidity(~20%)in the K2CO3-doped biocarbon bed promoted the carbonation reaction and boosted the CO2 sorption capacity(1.92 mmol/g at 50℃ and 14 kPa partial pressure of CO2).Carbonation is slower than physical adsorption of CO2 but wise process design could tune the operation conditions and balance capture capacity and sorption kinetics.展开更多
As CO2 is injected into pore spaces of water-filled reservoir rocks, it displaces much of the pore fluids. In short terms (several to tens of years), the greater part of the injected CO2 is predicted to stay as free C...As CO2 is injected into pore spaces of water-filled reservoir rocks, it displaces much of the pore fluids. In short terms (several to tens of years), the greater part of the injected CO2 is predicted to stay as free CO2 , i.e. in a CO2 rich dense phase that may contain some water. This paper investigates the sorption characteristics for rocks (quartzose arenite, greywacke, shale, granite and serpentine) and minerals (quartz and albite) in the CO2 rich dense phase. The measurements were conducted at 50°C and 100°C, and pressures up to 20 MPa. Our results demonstrated that significant quantities of CO2 were sorbed with all the samples. Particularly, at 50°C and 100°C, quartzose arenite showed largest sorption capacity among the other samples in higher pressures (>10 MPa). Furthermore, comparison with model prediction based on the pore filling model, which assumed that CO2 acts as filling pore spaces of the rocks and minerals, suggested the importance of the sorption mechanism in the CO2 geological storage in addition to the pore-filling mechanism. The present results should be pointed out that the sorption characteristics may have significant and meaningful effect on the assessment of CO2 storage capacity in geological media.展开更多
For the assessment of the carbon dioxide (CO2) storage potential of water-filled reservoir rocks (i.e., saline aquifers), it should be first important step for a thorough understanding of the effect of water content o...For the assessment of the carbon dioxide (CO2) storage potential of water-filled reservoir rocks (i.e., saline aquifers), it should be first important step for a thorough understanding of the effect of water content on CO2/water/rock interactions during CO2 injection. The purpose of this study is to examine the CO2 sorption amount for Kimachi sandstone and Berea sandstone at different water content using the manometric method at temperature of 50?C and pressures of up to 20 MPa. Our results document that a significant quantity of CO2 was sorbed on the two types of sandstone on all water-saturated bases, which corresponded to the amount adsorbed on the air-dry basis. Also, all the wet samples had significantly higher sorption capacity than the theoretical values calculated from the solubility model based on dissolution of CO2 in pore water and the pore-filling model, which assumes that the pore volume unoccupied by water is filled with CO2. Furthermore, the observations indicated a certain degree of correlation between the sorbed amount and the water content, except at pressures below the critical point for Berea sandstone. This investigation points out that CO2 sorption is a possible mechanism in CO2 geological storage even under water-saturated conditions and that the mechanism of sorption on silica and silicate minerals plays an essential role in the reliable and accurate estimation of the CO2 storage capacity of water-saturated reservoirs.展开更多
Amine-silica composite materials for post-combustion COcapture have attracted considerable attention because of their high COuptake at low COconcentrations, excellent COcapture selectivity in the presence of moisture,...Amine-silica composite materials for post-combustion COcapture have attracted considerable attention because of their high COuptake at low COconcentrations, excellent COcapture selectivity in the presence of moisture, and lower energy requirements for sorbent regeneration. This review discusses the recent advances in amine-silica composites for COcapture, including adsorbent preparation and characterization, COcapture under dry and moisture conditions at different COpartial pressures, sorbent regeneration, and stability after many cyclic sorption-desorption runs.展开更多
在保持原有"层-柱"MOF,[Zn_4(bpta)_2(dipytz)2(H_2O)_2]·4DMF·H_2O(1)(H4bpta=2,2′,6,6′-联苯四羧酸,dipytz=3,6-二(4-吡啶基)-1,2,4,5-四嗪)主体结构不变的情况下,通过dipytz配体中四嗪环的原位水解反应将极性...在保持原有"层-柱"MOF,[Zn_4(bpta)_2(dipytz)2(H_2O)_2]·4DMF·H_2O(1)(H4bpta=2,2′,6,6′-联苯四羧酸,dipytz=3,6-二(4-吡啶基)-1,2,4,5-四嗪)主体结构不变的情况下,通过dipytz配体中四嗪环的原位水解反应将极性的二芳酰基联氨基团引入框架,成功构筑出配合物[Zn_4(bpta)_2(dipytzhydr)_2(H_2O)_2]·solvent(2)(dipytzhydr=1,2-二异烟酰基肼)。对配合物2的系统表征和气体吸附性质研究结果证实了功能化目标的实现:配合物2相比于配合物1展现出更高的二氧化碳吸附热(由28.8 k J·mol-1升高至30.3 k J·mol-1)和CO_2/CH_4吸附选择性。以上结果表明基于配体中四嗪基团的原位水解后修饰能够有效提高相关MOFs材料的CO_2吸附性能。展开更多
文摘Solid sorbents with enhanced capacity and selectivity towards CO2 are crucial in the design of an efficient capture process.Among the possible alternatives,K2CO3-doped activated carbons have shown high CO2 capture capacity and rapid carbonation reaction rate.In this work,a sustainable and low-cost approach is developed with a biomass-based activated carbon or biocarbon as support.The CO2 capture performance in cyclic sorption–desorption operation and the sorption kinetics have been investigated under different scenarios in a purpose-built fixed-bed set-up.Independent of the H2O concentration in the flue gas,a constant relative humidity(~20%)in the K2CO3-doped biocarbon bed promoted the carbonation reaction and boosted the CO2 sorption capacity(1.92 mmol/g at 50℃ and 14 kPa partial pressure of CO2).Carbonation is slower than physical adsorption of CO2 but wise process design could tune the operation conditions and balance capture capacity and sorption kinetics.
文摘As CO2 is injected into pore spaces of water-filled reservoir rocks, it displaces much of the pore fluids. In short terms (several to tens of years), the greater part of the injected CO2 is predicted to stay as free CO2 , i.e. in a CO2 rich dense phase that may contain some water. This paper investigates the sorption characteristics for rocks (quartzose arenite, greywacke, shale, granite and serpentine) and minerals (quartz and albite) in the CO2 rich dense phase. The measurements were conducted at 50°C and 100°C, and pressures up to 20 MPa. Our results demonstrated that significant quantities of CO2 were sorbed with all the samples. Particularly, at 50°C and 100°C, quartzose arenite showed largest sorption capacity among the other samples in higher pressures (>10 MPa). Furthermore, comparison with model prediction based on the pore filling model, which assumed that CO2 acts as filling pore spaces of the rocks and minerals, suggested the importance of the sorption mechanism in the CO2 geological storage in addition to the pore-filling mechanism. The present results should be pointed out that the sorption characteristics may have significant and meaningful effect on the assessment of CO2 storage capacity in geological media.
文摘For the assessment of the carbon dioxide (CO2) storage potential of water-filled reservoir rocks (i.e., saline aquifers), it should be first important step for a thorough understanding of the effect of water content on CO2/water/rock interactions during CO2 injection. The purpose of this study is to examine the CO2 sorption amount for Kimachi sandstone and Berea sandstone at different water content using the manometric method at temperature of 50?C and pressures of up to 20 MPa. Our results document that a significant quantity of CO2 was sorbed on the two types of sandstone on all water-saturated bases, which corresponded to the amount adsorbed on the air-dry basis. Also, all the wet samples had significantly higher sorption capacity than the theoretical values calculated from the solubility model based on dissolution of CO2 in pore water and the pore-filling model, which assumes that the pore volume unoccupied by water is filled with CO2. Furthermore, the observations indicated a certain degree of correlation between the sorbed amount and the water content, except at pressures below the critical point for Berea sandstone. This investigation points out that CO2 sorption is a possible mechanism in CO2 geological storage even under water-saturated conditions and that the mechanism of sorption on silica and silicate minerals plays an essential role in the reliable and accurate estimation of the CO2 storage capacity of water-saturated reservoirs.
基金supported financially by the National Natural Science Foundation of China (No. 21607121)by the National Research Foundation of Korea (NRF) (Grant number: NRF2015R1A4A1042434)
文摘Amine-silica composite materials for post-combustion COcapture have attracted considerable attention because of their high COuptake at low COconcentrations, excellent COcapture selectivity in the presence of moisture, and lower energy requirements for sorbent regeneration. This review discusses the recent advances in amine-silica composites for COcapture, including adsorbent preparation and characterization, COcapture under dry and moisture conditions at different COpartial pressures, sorbent regeneration, and stability after many cyclic sorption-desorption runs.
基金supported by the National Natural Science Foundation of China (Grants No.21531005,21421001,21671112)Natural Science Fund of Tianjin,China (Grant No.15JCZDJC38800)~~
文摘在保持原有"层-柱"MOF,[Zn_4(bpta)_2(dipytz)2(H_2O)_2]·4DMF·H_2O(1)(H4bpta=2,2′,6,6′-联苯四羧酸,dipytz=3,6-二(4-吡啶基)-1,2,4,5-四嗪)主体结构不变的情况下,通过dipytz配体中四嗪环的原位水解反应将极性的二芳酰基联氨基团引入框架,成功构筑出配合物[Zn_4(bpta)_2(dipytzhydr)_2(H_2O)_2]·solvent(2)(dipytzhydr=1,2-二异烟酰基肼)。对配合物2的系统表征和气体吸附性质研究结果证实了功能化目标的实现:配合物2相比于配合物1展现出更高的二氧化碳吸附热(由28.8 k J·mol-1升高至30.3 k J·mol-1)和CO_2/CH_4吸附选择性。以上结果表明基于配体中四嗪基团的原位水解后修饰能够有效提高相关MOFs材料的CO_2吸附性能。