Systematic optimization of the photocatalyst and investigation of the role of each component is important to maximizing catalytic activity and comprehending the photocatalytic conversion of CO_(2) reduction to solar f...Systematic optimization of the photocatalyst and investigation of the role of each component is important to maximizing catalytic activity and comprehending the photocatalytic conversion of CO_(2) reduction to solar fuels.A surface-modified Ag@Ru-P25 photocatalyst with H_(2)O_(2) treatment was designed in this study to convert CO_(2) and H_(2)O vapor into highly selective CH4.Ru doping followed by Ag nanoparticles(NPs)cocatalyst deposition on P25(TiO_(2))enhances visible light absorption and charge separation,whereas H_(2)O_(2) treatment modifies the surface of the photocatalyst with hydroxyl(–OH)groups and promotes CO_(2) adsorption.High-resonance transmission electron microscopy,X-ray photoelectron spectroscopy,X-ray absorption near-edge structure,and extended X-ray absorption fine structure techniques were used to analyze the surface and chemical composition of the photocatalyst,while thermogravimetric analysis,CO_(2) adsorption isotherm,and temperature programmed desorption study were performed to examine the significance of H_(2)O_(2) treatment in increasing CO_(2) reduction activity.The optimized Ag1.0@Ru1.0-P25 photocatalyst performed excellent CO_(2) reduction activity into CO,CH4,and C2H6 with a~95%selectivity of CH4,where the activity was~135 times higher than that of pristine TiO_(2)(P25).For the first time,this work explored the effect of H_(2)O_(2) treatment on the photocatalyst that dramatically increases CO_(2) reduction activity.展开更多
CO_(2) emulsions used for EOR have received a lot of interest because of its good performance on CO_(2)mobility reduction.However,most of them have been focusing on the high quality CO_(2) emulsion(high CO_(2) fractio...CO_(2) emulsions used for EOR have received a lot of interest because of its good performance on CO_(2)mobility reduction.However,most of them have been focusing on the high quality CO_(2) emulsion(high CO_(2) fraction),while CO_(2) emulsion with high water cut has been rarely researched.In this paper,we carried out a comprehensive experimental study of using high water cut CO_(2)/H_(2)O emulsion for enhancing oil recovery.Firstly,a nonionic surfactant,alkyl glycosides(APG),was selected to stabilize CO_(2)/H_(2)O emulsion,and the corresponding morphology and stability were evaluated with a transparent PVT cell.Subsequently,plugging capacity and apparent viscosity of CO_(2)/H_(2)O emulsion were measured systematically by a sand pack displacement apparatus connected with a 1.95-m long capillary tube.Furthermore,a high water cut(40 vol%) CO_(2)/H_(2)O emulsion was selected for flooding experiments in a long sand pack and a core sample,and the oil recovery,the rate of oil recovery,and the pressure gradients were analyzed.The results indicated that APG had a good performance on emulsifying and stabilizing CO_(2) emulsion.An inversion from H_(2)O/CO_(2) emulsion to CO_(2)/H_(2)O emulsion with the increase in water cut was confirmed.CO_(2)/H_(2)O emulsions with lower water cuts presented higher apparent viscosity,while the optimal plugging capacity of CO_(2)/H_(2)O emulsion occurred at a certain water cut.Eventually,the displacement using CO_(2)/H_(2)O emulsion provided 18.98% and 13.36% additional oil recovery than that using pure CO_(2) in long sand pack and core tests,respectively.This work may provide guidelines for EOR using CO_(2) emulsions with high water cut.展开更多
It is acknowledged that injecting CO_(2) into oil reservoirs and saline aquifers for storage is a practical and affordable method for CO_(2) sequestration.Most CO_(2) produced from industrial exhaust contains impurity...It is acknowledged that injecting CO_(2) into oil reservoirs and saline aquifers for storage is a practical and affordable method for CO_(2) sequestration.Most CO_(2) produced from industrial exhaust contains impurity gases such as H_(2)S that might impact CO_(2) sequestration due to competitive adsorption.This study makes a commendable effort to explore the adsorption behavior of CO_(2)/H_(2)S mixtures in calcite slit nanopores.Grand Canonical Monte Carlo(GCMC)simulation is employed to reveal the adsorption of CO_(2),H_(2)S as well as their binary mixtures in calcite nanopores.Results show that the increase in pressure and temperature can promote and inhibit the adsorption capacity of CO_(2) and H_(2)S in calcite nanopores,respectively.CO_(2)exhibits stronger adsorption on calcite surface than H_(2)S.Electrostatic energy plays the dominating role in the adsorption behavior.Electrostatic energy accounts for 97.11%of the CO_(2)-calcite interaction energy and 56.33%of the H_(2)S-calcite interaction energy at 10 MPa and 323.15 K.The presence of H_(2)S inhibits the CO_(2) adsorption in calcite nanopores due to competitive adsorption,and a higher mole fraction of H_(2)S leads to less CO_(2) adsorption.The quantity of CO_(2) adsorbed is lessened by approximately 33%when the mole fraction of H_(2)S reaches 0.25.CO_(2) molecules preferentially occupy the regions near the po re wall and H_(2)S molecules tend to reside at the center of nanopore even when the molar ratio of CO_(2) is low,indicating that CO_(2) has an adsorption priority on the calcite surface over H_(2)S.In addition,moisture can weaken the adsorption of both CO_(2) and H_(2)S,while CO_(2) is more affected.More interestingly,we find that pure CO_(2) is more suitable to be sequestrated in the shallower formations,i.e.,500-1500 m,whereas CO_(2)with H_(2)S impurity should be settled in the deeper reservoirs.展开更多
基金supported by the Ministry of Science and ICT in Korea(2021R1A2C2009459)X-ray absorption spectra were obtained from Pohang Accelerator Laboratory(PAL)10C beamlinesupported by the US Department of Energy,Office of Science,Office of Advanced Scientific Computing Research,and Scientific Discovery through Advanced Computing(SciDAC)program under Award Number DE-SC0022209.
文摘Systematic optimization of the photocatalyst and investigation of the role of each component is important to maximizing catalytic activity and comprehending the photocatalytic conversion of CO_(2) reduction to solar fuels.A surface-modified Ag@Ru-P25 photocatalyst with H_(2)O_(2) treatment was designed in this study to convert CO_(2) and H_(2)O vapor into highly selective CH4.Ru doping followed by Ag nanoparticles(NPs)cocatalyst deposition on P25(TiO_(2))enhances visible light absorption and charge separation,whereas H_(2)O_(2) treatment modifies the surface of the photocatalyst with hydroxyl(–OH)groups and promotes CO_(2) adsorption.High-resonance transmission electron microscopy,X-ray photoelectron spectroscopy,X-ray absorption near-edge structure,and extended X-ray absorption fine structure techniques were used to analyze the surface and chemical composition of the photocatalyst,while thermogravimetric analysis,CO_(2) adsorption isotherm,and temperature programmed desorption study were performed to examine the significance of H_(2)O_(2) treatment in increasing CO_(2) reduction activity.The optimized Ag1.0@Ru1.0-P25 photocatalyst performed excellent CO_(2) reduction activity into CO,CH4,and C2H6 with a~95%selectivity of CH4,where the activity was~135 times higher than that of pristine TiO_(2)(P25).For the first time,this work explored the effect of H_(2)O_(2) treatment on the photocatalyst that dramatically increases CO_(2) reduction activity.
基金The financial supports received from the National Natural Science Foundation of China(Nos.22178378,22127812)。
文摘CO_(2) emulsions used for EOR have received a lot of interest because of its good performance on CO_(2)mobility reduction.However,most of them have been focusing on the high quality CO_(2) emulsion(high CO_(2) fraction),while CO_(2) emulsion with high water cut has been rarely researched.In this paper,we carried out a comprehensive experimental study of using high water cut CO_(2)/H_(2)O emulsion for enhancing oil recovery.Firstly,a nonionic surfactant,alkyl glycosides(APG),was selected to stabilize CO_(2)/H_(2)O emulsion,and the corresponding morphology and stability were evaluated with a transparent PVT cell.Subsequently,plugging capacity and apparent viscosity of CO_(2)/H_(2)O emulsion were measured systematically by a sand pack displacement apparatus connected with a 1.95-m long capillary tube.Furthermore,a high water cut(40 vol%) CO_(2)/H_(2)O emulsion was selected for flooding experiments in a long sand pack and a core sample,and the oil recovery,the rate of oil recovery,and the pressure gradients were analyzed.The results indicated that APG had a good performance on emulsifying and stabilizing CO_(2) emulsion.An inversion from H_(2)O/CO_(2) emulsion to CO_(2)/H_(2)O emulsion with the increase in water cut was confirmed.CO_(2)/H_(2)O emulsions with lower water cuts presented higher apparent viscosity,while the optimal plugging capacity of CO_(2)/H_(2)O emulsion occurred at a certain water cut.Eventually,the displacement using CO_(2)/H_(2)O emulsion provided 18.98% and 13.36% additional oil recovery than that using pure CO_(2) in long sand pack and core tests,respectively.This work may provide guidelines for EOR using CO_(2) emulsions with high water cut.
基金financial support from the National Natural Science Foundation of China (Grant No.52004320)the Science Foundation of China University of Petroleum,Beijing (No.2462021QNXZ012,No.2462022BJRC001,and No.2462021YJRC012)the funding from the State Key Laboratory of Petroleum Resources and Engineering (No.PRP/indep-1-2103)。
文摘It is acknowledged that injecting CO_(2) into oil reservoirs and saline aquifers for storage is a practical and affordable method for CO_(2) sequestration.Most CO_(2) produced from industrial exhaust contains impurity gases such as H_(2)S that might impact CO_(2) sequestration due to competitive adsorption.This study makes a commendable effort to explore the adsorption behavior of CO_(2)/H_(2)S mixtures in calcite slit nanopores.Grand Canonical Monte Carlo(GCMC)simulation is employed to reveal the adsorption of CO_(2),H_(2)S as well as their binary mixtures in calcite nanopores.Results show that the increase in pressure and temperature can promote and inhibit the adsorption capacity of CO_(2) and H_(2)S in calcite nanopores,respectively.CO_(2)exhibits stronger adsorption on calcite surface than H_(2)S.Electrostatic energy plays the dominating role in the adsorption behavior.Electrostatic energy accounts for 97.11%of the CO_(2)-calcite interaction energy and 56.33%of the H_(2)S-calcite interaction energy at 10 MPa and 323.15 K.The presence of H_(2)S inhibits the CO_(2) adsorption in calcite nanopores due to competitive adsorption,and a higher mole fraction of H_(2)S leads to less CO_(2) adsorption.The quantity of CO_(2) adsorbed is lessened by approximately 33%when the mole fraction of H_(2)S reaches 0.25.CO_(2) molecules preferentially occupy the regions near the po re wall and H_(2)S molecules tend to reside at the center of nanopore even when the molar ratio of CO_(2) is low,indicating that CO_(2) has an adsorption priority on the calcite surface over H_(2)S.In addition,moisture can weaken the adsorption of both CO_(2) and H_(2)S,while CO_(2) is more affected.More interestingly,we find that pure CO_(2) is more suitable to be sequestrated in the shallower formations,i.e.,500-1500 m,whereas CO_(2)with H_(2)S impurity should be settled in the deeper reservoirs.
