"Carbon peaking and carbon neutrality"is an essential national strategy,and the geological storage and utilization of CO_(2)is a hot issue today.However,due to the scarcity of pure CO_(2)gas sources in China..."Carbon peaking and carbon neutrality"is an essential national strategy,and the geological storage and utilization of CO_(2)is a hot issue today.However,due to the scarcity of pure CO_(2)gas sources in China and the high cost of CO_(2)capture,CO_(2)-rich industrial waste gas(CO_(2)-rich IWG)is gradually emerging into the public's gaze.CO_(2)has good adsorption properties on shale surfaces,but acidic gases can react with shale,so the mechanism of the CO_(2)-rich IWG-water-shale reaction and the change in reservoir properties will determine the stability of geological storage.Therefore,based on the mineral composition of the Longmaxi Formation shale,this study constructs a thermodynamic equilibrium model of water-rock reactions and simulates the regularity of reactions between CO_(2)-rich IWG and shale minerals.The results indicate that CO_(2)consumed 12%after reaction,and impurity gases in the CO_(2)-rich IWG can be dissolved entirely,thus demonstrating the feasibility of treating IWG through water-rock reactions.Since IWG inhibits the dissolution of CO_(2),the optimal composition of CO_(2)-rich IWG is 95%CO_(2)and 5%IWG when CO_(2)geological storage is the main goal.In contrast,when the main goal is the geological storage of total CO_(2)-rich IWG or impurity gas,the optimal CO_(2)-rich IWG composition is 50%CO_(2)and 50%IWG.In the CO_(2)-rich IWG-water-shale reaction,temperature has less influence on the water-rock reaction,while pressure is the most important parameter.SO2 has the greatest impact on water-rock reaction in gas.For minerals,clay minerals such as illite and montmorillonite had a significant effect on water-rock reaction.The overall reaction is dominated by precipitation and the volume of the rock skeleton has increased by 0.74 cm3,resulting in a decrease in shale porosity,which enhances the stability of CO_(2)geological storage to some extent.During the reaction between CO_(2)-rich IWG-water-shale at simulated temperatures and pressures,precipitation is the main reaction,and shale porosity decreases.However,as the reservoir water content increases,the reaction will first dissolve and then precipitate before dissolving again.When the water content is less than 0.0005 kg or greater than 0.4 kg,it will lead to an increase in reservoir porosity,which ultimately reduces the long-term geological storage stability of CO_(2)-rich IWG.展开更多
Asphaltene deposition is a significant problem during gas injection processes,as it can block the porous medium,the wellbore,and the involved facilities,significantly impacting reservoir productivity and ultimate oil re...Asphaltene deposition is a significant problem during gas injection processes,as it can block the porous medium,the wellbore,and the involved facilities,significantly impacting reservoir productivity and ultimate oil recovery.Only a few studies have investigated the numerical modeling of this potential effect in porous media.This study focuses on asphaltene deposition due to natural gas and CO_(2) injection.Predictions of the effect of gas injection on asphaltene deposition behavior have been made using a 3D numerical simulation model.The results indicate that the injection of natural gas exacerbates asphaltene deposition,leading to a significant reduction in permeability near the injection well and throughout the reservoir.This reduction in permeability strongly affects the ability of gas toflow through the reservoir,resulting in an improvement of the displacement front.The displacement effi-ciency of the injection gas process increases by up to 1.40%when gas is injected at 5500 psi,compared to the scenario where the asphaltene model is not considered.CO_(2) injection leads to a miscible process with crude oil,extracting light and intermediate components,which intensifies asphaltene precipitation and increases the viscosity of the remaining crude oil,ultimately reducing the recovery rate.展开更多
CO_(2) dry fracturing is a promising alternative method to water fracturing in tight gas reservoirs,especially in water-scarce areas such as the Loess Plateau.The CO_(2) flowback efficiency is a critical factor that a...CO_(2) dry fracturing is a promising alternative method to water fracturing in tight gas reservoirs,especially in water-scarce areas such as the Loess Plateau.The CO_(2) flowback efficiency is a critical factor that affects the final gas production effect.However,there have been few studies focusing on the flowback characteristics after CO_(2) dry fracturing.In this study,an extensive core-to-field scale study was conducted to investigate CO_(2) flowback characteristics and CH_(4) production behavior.Firstly,to investigate the impact of core properties and production conditions on CO_(2) flowback,a series of laboratory experiments at the core scale were conducted.Then,the key factors affecting the flowback were analyzed using the grey correlation method based on field data.Finally,taking the construction parameters of Well S60 as an example,a dual-permeability model was used to characterize the different seepage fields in the matrix and fracture for tight gas reservoirs.The production parameters after CO_(2) dry fracturing were then optimized.Experimental results demonstrate that CO_(2) dry fracturing is more effective than slickwater fracturing,with a 9.2%increase in CH_(4) recovery.The increase in core permeability plays a positive role in improving CH_(4) production and CO_(2) flowback.The soaking process is mainly affected by CO_(2) diffusion,and the soaking time should be controlled within 12 h.Increasing the flowback pressure gradient results in a significant increase in both CH_(4) recovery and CO_(2) flowback efficiency.While,an increase in CO_(2) injection is not conducive to CH_(4) production and CO_(2) flowback.Based on the experimental and field data,the important factors affecting flowback and production were comprehensively and effectively discussed.The results show that permeability is the most important factor,followed by porosity and effective thickness.Considering flowback efficiency and the influence of proppant reflux,the injection volume should be the minimum volume that meets the requirements for generating fractures.The soaking time should be short which is 1 day in this study,and the optimal bottom hole flowback pressure should be set at 10 MPa.This study aims to improve the understanding of CO_(2) dry fracturing in tight gas reservoirs and provide valuable insights for optimizing the process parameters.展开更多
The overall photocatalytic CO_(2) reduction reaction(OPCRR)that can directly convert CO_(2) and H_(2)O into fuels represents a promising renewable energy conversion technology.As a typical redox reaction,the OPCRR inv...The overall photocatalytic CO_(2) reduction reaction(OPCRR)that can directly convert CO_(2) and H_(2)O into fuels represents a promising renewable energy conversion technology.As a typical redox reaction,the OPCRR involves two half-reactions:the CO_(2) reduction half-reaction(CRHR)and the water oxidation half-reaction(WOHR).Generally,both half-reactions can be promoted by adjusting the wettability of catalysts.However,there is a contradiction in wettability requirements for the two half-reactions.Specifically,CRHR prefers a hydrophobic surface that can accumulate more CO_(2) molecules on the active sites,ensuring the appropriate ratio of gas-phase(CO_(2))to liquid-phase(H_(2)O)reactants.Conversely,the WOHR prefers a hydrophilic surface that can promote the departure of the gaseous product(O_(2))from the catalyst surface,preventing isolation between active sites and the reactant(H_(2)O).Here,we successfully reconciled the contradictory wettability requirements for the CRHR and WOHR by creating an alternately hydrophobic catalyst.This was achieved through a selectively hydrophobic modification method and a charge-transfer-control strategy.Consequently,the collaboratively promoted CRHR and WOHR led to a significantly enhanced OPCRR with a solar-to-fuel conversion efficiency of 0.186%.Notably,in ethanol production,the catalyst exhibited a 10.64-fold increase in generation rate(271.44μmol g^(-1)h~(-1))and a 4-fold increase in selectivity(55.77%)compared to the benchmark catalyst.This innovative approach holds great potential for application in universal overall reactions involving gas participation.展开更多
The global concerns of energy crisis and climate change,primarily caused by carbon dioxide(CO_(2)),are of utmost importance.Recently,the electrocatalytic CO_(2) reduction reaction(CO_(2)RR) to high value-added multi-c...The global concerns of energy crisis and climate change,primarily caused by carbon dioxide(CO_(2)),are of utmost importance.Recently,the electrocatalytic CO_(2) reduction reaction(CO_(2)RR) to high value-added multi-carbon(C_(2+)) products driven by renewable electricity has emerged as a highly promising solution to alleviate energy shortages and achieve carbon neutrality.Among these C_(2+) products,ethylene(C_(2)H_(4))holds particular importance in the petrochemical industry.Accordingly,this review aims to establish a connection between the fundamentals of electrocatalytic CO_(2) reduction reaction to ethylene(CO_(2)RRto-C_(2)H_(4)) in laboratory-scale research(lab) and its potential applications in industrial-level fabrication(fab).The review begins by summarizing the fundamental aspects,including the design strategies of high-performance Cu-based electrocatalysts and advanced electrolyzer devices.Subsequently,innovative and value-added techniques are presented to address the inherent challenges encountered during the implementations of CO_(2)RR-to-C_(2)H_(4) in industrial scenarios.Additionally,case studies of the technoeconomic analysis of the CO_(2)RR-to-C_(2)H_(4) process are discussed,taking into factors such as costeffectiveness,scalability,and market potential.The review concludes by outlining the perspectives and challenges associated with scaling up the CO_(2)RR-to-C_(2)H_(4) process.The insights presented in this review are expected to make a valuable contribution in advancing the CO_(2)RR-to-C_(2)H_(4) process from lab to fab.展开更多
Undesirable gas channeling always occurs along the high-permeability layers in heterogeneous oil reservoirs during water-alternating-CO_(2)(WAG)flooding,and conventional polymer gels used for blocking the“channeling...Undesirable gas channeling always occurs along the high-permeability layers in heterogeneous oil reservoirs during water-alternating-CO_(2)(WAG)flooding,and conventional polymer gels used for blocking the“channeling”paths usually suffer from either low injectivity or poor gelation control.Herein,we for the first time developed an in-situ high-pressure CO_(2)-triggered gel system based on a smart surfactant,N-erucamidopropyl-N,N-dimethylamine(UC22AMPM),which was introduced into the aqueous slugs to control gas channeling inWAG processes.The water-like,low-viscosity UC22AMPM brine solution can be thickened by high-pressure CO_(2) owing to the formation of wormlike micelles(WLMs),as well as their growth and shear-induced structure buildup under shear flow.The thickening power can be further potentiated by the generation of denser WLMs resulting from either surfactant concentration augmentation or a certain range of heating,and can be impaired via pressurization above the critical pressure of CO_(2) because of its soaring solvent power.Core flooding tests using heterogeneous cores demonstrated that gas channeling was alleviated by plugging of high-capacity channels due to the in-situ gelation of UC22AMPM slugs upon their reaction with the pre-or post-injected CO_(2) slugs under shear flow,thereupon driving chase fluids into unrecovered low-permeability areas and producing an 8.0% higher oil recovery factor than the conventional WAG mode.This smart surfactant enabled high injectivity and satisfactory gelation control,attributable to low initial viscosity and the combined properties of one component and CO_(2)-triggered gelation,respectively.This work could provide a guide towards designing gels for reducing CO_(2) spillover and reinforcing the CO_(2) sequestration effect during CO_(2) enhanced oil recovery processes.展开更多
基金The work was supported by the National Natural Science Foundation of China(No.52074316)PetroChina Company Limited(No.2019E-2608).
文摘"Carbon peaking and carbon neutrality"is an essential national strategy,and the geological storage and utilization of CO_(2)is a hot issue today.However,due to the scarcity of pure CO_(2)gas sources in China and the high cost of CO_(2)capture,CO_(2)-rich industrial waste gas(CO_(2)-rich IWG)is gradually emerging into the public's gaze.CO_(2)has good adsorption properties on shale surfaces,but acidic gases can react with shale,so the mechanism of the CO_(2)-rich IWG-water-shale reaction and the change in reservoir properties will determine the stability of geological storage.Therefore,based on the mineral composition of the Longmaxi Formation shale,this study constructs a thermodynamic equilibrium model of water-rock reactions and simulates the regularity of reactions between CO_(2)-rich IWG and shale minerals.The results indicate that CO_(2)consumed 12%after reaction,and impurity gases in the CO_(2)-rich IWG can be dissolved entirely,thus demonstrating the feasibility of treating IWG through water-rock reactions.Since IWG inhibits the dissolution of CO_(2),the optimal composition of CO_(2)-rich IWG is 95%CO_(2)and 5%IWG when CO_(2)geological storage is the main goal.In contrast,when the main goal is the geological storage of total CO_(2)-rich IWG or impurity gas,the optimal CO_(2)-rich IWG composition is 50%CO_(2)and 50%IWG.In the CO_(2)-rich IWG-water-shale reaction,temperature has less influence on the water-rock reaction,while pressure is the most important parameter.SO2 has the greatest impact on water-rock reaction in gas.For minerals,clay minerals such as illite and montmorillonite had a significant effect on water-rock reaction.The overall reaction is dominated by precipitation and the volume of the rock skeleton has increased by 0.74 cm3,resulting in a decrease in shale porosity,which enhances the stability of CO_(2)geological storage to some extent.During the reaction between CO_(2)-rich IWG-water-shale at simulated temperatures and pressures,precipitation is the main reaction,and shale porosity decreases.However,as the reservoir water content increases,the reaction will first dissolve and then precipitate before dissolving again.When the water content is less than 0.0005 kg or greater than 0.4 kg,it will lead to an increase in reservoir porosity,which ultimately reduces the long-term geological storage stability of CO_(2)-rich IWG.
基金funded by CNOOC Production Research Project(CCL2022SZPS0076).
文摘Asphaltene deposition is a significant problem during gas injection processes,as it can block the porous medium,the wellbore,and the involved facilities,significantly impacting reservoir productivity and ultimate oil recovery.Only a few studies have investigated the numerical modeling of this potential effect in porous media.This study focuses on asphaltene deposition due to natural gas and CO_(2) injection.Predictions of the effect of gas injection on asphaltene deposition behavior have been made using a 3D numerical simulation model.The results indicate that the injection of natural gas exacerbates asphaltene deposition,leading to a significant reduction in permeability near the injection well and throughout the reservoir.This reduction in permeability strongly affects the ability of gas toflow through the reservoir,resulting in an improvement of the displacement front.The displacement effi-ciency of the injection gas process increases by up to 1.40%when gas is injected at 5500 psi,compared to the scenario where the asphaltene model is not considered.CO_(2) injection leads to a miscible process with crude oil,extracting light and intermediate components,which intensifies asphaltene precipitation and increases the viscosity of the remaining crude oil,ultimately reducing the recovery rate.
基金support from the National Natural Science Foundation of China(No.51904324,No.51974348)the Prospective Basic Major Science and Technology Projects for the 14th Five Year Plan(No.2021DJ2202).
文摘CO_(2) dry fracturing is a promising alternative method to water fracturing in tight gas reservoirs,especially in water-scarce areas such as the Loess Plateau.The CO_(2) flowback efficiency is a critical factor that affects the final gas production effect.However,there have been few studies focusing on the flowback characteristics after CO_(2) dry fracturing.In this study,an extensive core-to-field scale study was conducted to investigate CO_(2) flowback characteristics and CH_(4) production behavior.Firstly,to investigate the impact of core properties and production conditions on CO_(2) flowback,a series of laboratory experiments at the core scale were conducted.Then,the key factors affecting the flowback were analyzed using the grey correlation method based on field data.Finally,taking the construction parameters of Well S60 as an example,a dual-permeability model was used to characterize the different seepage fields in the matrix and fracture for tight gas reservoirs.The production parameters after CO_(2) dry fracturing were then optimized.Experimental results demonstrate that CO_(2) dry fracturing is more effective than slickwater fracturing,with a 9.2%increase in CH_(4) recovery.The increase in core permeability plays a positive role in improving CH_(4) production and CO_(2) flowback.The soaking process is mainly affected by CO_(2) diffusion,and the soaking time should be controlled within 12 h.Increasing the flowback pressure gradient results in a significant increase in both CH_(4) recovery and CO_(2) flowback efficiency.While,an increase in CO_(2) injection is not conducive to CH_(4) production and CO_(2) flowback.Based on the experimental and field data,the important factors affecting flowback and production were comprehensively and effectively discussed.The results show that permeability is the most important factor,followed by porosity and effective thickness.Considering flowback efficiency and the influence of proppant reflux,the injection volume should be the minimum volume that meets the requirements for generating fractures.The soaking time should be short which is 1 day in this study,and the optimal bottom hole flowback pressure should be set at 10 MPa.This study aims to improve the understanding of CO_(2) dry fracturing in tight gas reservoirs and provide valuable insights for optimizing the process parameters.
基金financially supported by the National Natural Science Foundation of China(22378204,22008121,51790492)the National Outstanding Youth Science Fund Project of National Natural Science Foundation of China(T2125004)+1 种基金the Funding of NJUST(No.TSXK2022D002)the Postgraduate Research&Practice Innovation Program of Jiangsu Province(KYCX23_0454)。
文摘The overall photocatalytic CO_(2) reduction reaction(OPCRR)that can directly convert CO_(2) and H_(2)O into fuels represents a promising renewable energy conversion technology.As a typical redox reaction,the OPCRR involves two half-reactions:the CO_(2) reduction half-reaction(CRHR)and the water oxidation half-reaction(WOHR).Generally,both half-reactions can be promoted by adjusting the wettability of catalysts.However,there is a contradiction in wettability requirements for the two half-reactions.Specifically,CRHR prefers a hydrophobic surface that can accumulate more CO_(2) molecules on the active sites,ensuring the appropriate ratio of gas-phase(CO_(2))to liquid-phase(H_(2)O)reactants.Conversely,the WOHR prefers a hydrophilic surface that can promote the departure of the gaseous product(O_(2))from the catalyst surface,preventing isolation between active sites and the reactant(H_(2)O).Here,we successfully reconciled the contradictory wettability requirements for the CRHR and WOHR by creating an alternately hydrophobic catalyst.This was achieved through a selectively hydrophobic modification method and a charge-transfer-control strategy.Consequently,the collaboratively promoted CRHR and WOHR led to a significantly enhanced OPCRR with a solar-to-fuel conversion efficiency of 0.186%.Notably,in ethanol production,the catalyst exhibited a 10.64-fold increase in generation rate(271.44μmol g^(-1)h~(-1))and a 4-fold increase in selectivity(55.77%)compared to the benchmark catalyst.This innovative approach holds great potential for application in universal overall reactions involving gas participation.
基金supported by Zhejiang Provincial Department of Science and Technology under its Provincial Key Laboratory Program(2020E10018)the financial support from Fundamental Research Funds for the Central Universities(2022LHJH01-03,2022ZFJH04,2022QZJH14)+5 种基金Pioneer R&D Program of Zhejiang Province(2022C03040)the financial aid from National Natural Science Foundation of China(22005266)Zhejiang Provincial Natural Science Foundation(LR21E020003)Fundamental Research Funds for the Central Universities(2021FZZX001-09)supported by the Royal Academy of Engineering under the Chairs in Emerging Technologies scheme(CiET2021_17)University of Nottingham Ningbo China for providing a full PhD scholarship。
文摘The global concerns of energy crisis and climate change,primarily caused by carbon dioxide(CO_(2)),are of utmost importance.Recently,the electrocatalytic CO_(2) reduction reaction(CO_(2)RR) to high value-added multi-carbon(C_(2+)) products driven by renewable electricity has emerged as a highly promising solution to alleviate energy shortages and achieve carbon neutrality.Among these C_(2+) products,ethylene(C_(2)H_(4))holds particular importance in the petrochemical industry.Accordingly,this review aims to establish a connection between the fundamentals of electrocatalytic CO_(2) reduction reaction to ethylene(CO_(2)RRto-C_(2)H_(4)) in laboratory-scale research(lab) and its potential applications in industrial-level fabrication(fab).The review begins by summarizing the fundamental aspects,including the design strategies of high-performance Cu-based electrocatalysts and advanced electrolyzer devices.Subsequently,innovative and value-added techniques are presented to address the inherent challenges encountered during the implementations of CO_(2)RR-to-C_(2)H_(4) in industrial scenarios.Additionally,case studies of the technoeconomic analysis of the CO_(2)RR-to-C_(2)H_(4) process are discussed,taking into factors such as costeffectiveness,scalability,and market potential.The review concludes by outlining the perspectives and challenges associated with scaling up the CO_(2)RR-to-C_(2)H_(4) process.The insights presented in this review are expected to make a valuable contribution in advancing the CO_(2)RR-to-C_(2)H_(4) process from lab to fab.
基金Financial support from the Natural Science Foundation of Sichuan Province(2022NSFSC0030)National Natural Science Foundation of China(U1762218)is gratefully acknowledged.
文摘Undesirable gas channeling always occurs along the high-permeability layers in heterogeneous oil reservoirs during water-alternating-CO_(2)(WAG)flooding,and conventional polymer gels used for blocking the“channeling”paths usually suffer from either low injectivity or poor gelation control.Herein,we for the first time developed an in-situ high-pressure CO_(2)-triggered gel system based on a smart surfactant,N-erucamidopropyl-N,N-dimethylamine(UC22AMPM),which was introduced into the aqueous slugs to control gas channeling inWAG processes.The water-like,low-viscosity UC22AMPM brine solution can be thickened by high-pressure CO_(2) owing to the formation of wormlike micelles(WLMs),as well as their growth and shear-induced structure buildup under shear flow.The thickening power can be further potentiated by the generation of denser WLMs resulting from either surfactant concentration augmentation or a certain range of heating,and can be impaired via pressurization above the critical pressure of CO_(2) because of its soaring solvent power.Core flooding tests using heterogeneous cores demonstrated that gas channeling was alleviated by plugging of high-capacity channels due to the in-situ gelation of UC22AMPM slugs upon their reaction with the pre-or post-injected CO_(2) slugs under shear flow,thereupon driving chase fluids into unrecovered low-permeability areas and producing an 8.0% higher oil recovery factor than the conventional WAG mode.This smart surfactant enabled high injectivity and satisfactory gelation control,attributable to low initial viscosity and the combined properties of one component and CO_(2)-triggered gelation,respectively.This work could provide a guide towards designing gels for reducing CO_(2) spillover and reinforcing the CO_(2) sequestration effect during CO_(2) enhanced oil recovery processes.
