In this study,an integrated technology is proposed for the absorption and utilization of CO_(2)in alkanolamine solution for the preparation of BaCO_(3)in a high-gravity environment.The effects of absorbent type,high-g...In this study,an integrated technology is proposed for the absorption and utilization of CO_(2)in alkanolamine solution for the preparation of BaCO_(3)in a high-gravity environment.The effects of absorbent type,high-gravity factor,gas/liquid ratio,and initial BaCl2concentration on the absorption rate and amount of CO_(2)and the preparation of BaCO_(3)are investigated.The results reveal that the absorption rate and amount of CO_(2)follow the order of ethyl alkanolamine(MEA)>diethanol amine(DEA)>N-methyldiethanolamine(MDEA),and thus MEA is the most effective absorbent for CO_(2)absorption.The absorption rate and amount of CO_(2)under high gravity are higher than that under normal gravity.Notably,the absorption rate at 75 min under high gravity is approximately 2 times that under normal gravity.This is because the centrifugal force resulting from the high-speed rotation of the packing can greatly increase gas-liquid mass transfer and micromixing.The particle size of BaCO_(3)prepared in the rotating packed bed is in the range of 57.2—89 nm,which is much smaller than that prepared in the bubbling reactor(>100.3 nm),and it also has higher purity(99.6%)and larger specific surface area(14.119 m^(2)·g^(-1)).It is concluded that the high-gravity technology has the potential to increase the absorption and utilization of CO_(2)in alkanolamine solution for the preparation of BaCO_(3).This study provides new insights into carbon emissions reduction and carbon utilization.展开更多
By employing metal oxides as oxygen carriers,chemical looping demonstrates its effectiveness in transferring oxygen between reduction and oxidation environments to partially oxidize fuels into syngas and convert CO_(2...By employing metal oxides as oxygen carriers,chemical looping demonstrates its effectiveness in transferring oxygen between reduction and oxidation environments to partially oxidize fuels into syngas and convert CO_(2) into CO.Generally,NiFe_(2_)O_(4) oxygen carriers have demonstrated remarkable efficiency in chemical looping CO_(2) conversion.Nevertheless,the intricate process of atomic migration and evolution within the internal structure of bimetallic oxygen carriers during continuous high‐temperature redox cycling remains unclear.Consequently,the lack of a fundamental understanding of the complex ionic migration and oxygen transfer associated with energy conversion processes hampers the design of high‐performance oxygen carriers.Thus,in this study,we employed in situ characterization techniques and theoretical calculations to investigate the ion migration behavior and structural evolution in the bulk of NiFe_(2_)O_(4) oxygen carriers during H_(2) reduction and CO_(2)/lab air oxidation cycles.We discovered that during the H_(2) reduction step,lattice oxygen rapidly migrates to vacancy layers to replenish consumed active oxygen species,while Ni leaches from the material and migrates to the surface.During the CO_(2) splitting step,Ni migrates toward the core of the bimetallic oxygen carrier,forming Fe–Ni alloys.During the air oxidation step,Fe–Ni migrates outward,creating a hollow structure owing to the Kirkendall effect triggered by the swift transfer of lattice oxygen.The metal atom migration paths depend on the oxygen transfer rates.These discoveries highlight the significance of regulating the release–recovery rate of lattice oxygen to uphold the structures and reactivity of oxygen carriers.This work offers a comprehensive understanding of the oxidation/reduction‐driven atomic interdiffusion behavior of bimetallic oxygen carriers.展开更多
Chemical looping combustion has the potential to be an efficient and low-cost technology capable of contributing to the reduction of the atmospheric concentration of CO_(2) in order to reach the 1.5/2°C goal and ...Chemical looping combustion has the potential to be an efficient and low-cost technology capable of contributing to the reduction of the atmospheric concentration of CO_(2) in order to reach the 1.5/2°C goal and mitigate climate change.In this process,a metal oxide is used as oxygen carrier in a dual fluidized bed to generate clean CO_(2) via combustion of biomass.Most commonly,natural ores or synthetic materials are used as oxygen carrier whereas both must meet special requirements for the conversion of solid fuels.Synthetic oxygen carriers are characterized by higher reactivity at the expense of higher costs versus the lower-cost natural ores.To determine the viability of both possibilities,a techno-economic comparison of a synthetic material based on manganese,iron,and copper to the natural ore ilmenite was conducted.The synthetic oxygen carrier was characterized and tested in a pilot plant,where high combustion efficiencies up to 98.4%and carbon capture rates up to 98.5%were reached.The techno-economic assessment resulted in CO_(2) capture costs of 75 and 40€/tCO_(2) for the synthetic and natural ore route respectively,whereas a sensitivity analysis showed the high impact of production costs and attrition rates of the synthetic material.The synthetic oxygen carrier could break even with the natural ore in case of lower production costs and attrition rates,which could be reached by adapting the production process and recycling material.By comparison to state-of-the-art technologies,it is demonstrated that both routes are viable and the capture cost of CO_(2) could be reduced by implementing the chemical looping combustion technology.展开更多
This work systematically reviews the complex mechanisms of CO_(2)-water-rock interactions,microscopic simulations of reactive transport(dissolution,precipitation and precipitate migration)in porous media,and microscop...This work systematically reviews the complex mechanisms of CO_(2)-water-rock interactions,microscopic simulations of reactive transport(dissolution,precipitation and precipitate migration)in porous media,and microscopic simulations of CO_(2)-water-rock system.The work points out the key issues in current research and provides suggestions for future research.After injection of CO_(2) into underground reservoirs,not only conventional pressure-driven flow and mass transfer processes occur,but also special physicochemical phenomena like dissolution,precipitation,and precipitate migration.The coupling of these processes causes complex changes in permeability and porosity parameters of the porous media.Pore-scale microscopic flow simulations can provide detailed information within the three-dimensional pore and throat space and explicitly observe changes in the fluid-solid interfaces of porous media during reactions.At present,the research has limitations in the decoupling of complex mechanisms,characterization of differential multi-mineral reactions,precipitation generation mechanisms and characterization(crystal nucleation and mineral detachment),simulation methods for precipitation-fluid interaction,and coupling mechanisms of multiple physicochemical processes.In future studies,it is essential to innovate experimental methods to decouple“dissolution-precipitation-precipitate migration”processes,improve the accuracy of experimental testing of minerals geochemical reaction-related parameters,build reliable characterization of various precipitation types,establish precipitation-fluid interaction simulation methods,coordinate the boundary conditions of different physicochemical processes,and,finally,achieve coupled flow simulation of“dissolution-precipitation-precipitate migration”within CO_(2)-water-rock systems.展开更多
Light olefins are important platform feedstocks in the petrochemical industry,and the ongoing global economic development has driven sustained growth in demand for these compounds.The dehydrogenation of alkanes,derive...Light olefins are important platform feedstocks in the petrochemical industry,and the ongoing global economic development has driven sustained growth in demand for these compounds.The dehydrogenation of alkanes,derived from shale gas,serves as an alternative olefins production route.Concurrently,the target of realizing carbon neutrality promotes the comprehensive utilization of greenhouse gas.The integrated process of light alkanes dehydrogenation and carbon dioxide reduction(CO_(2)-ODH)can produce light olefins and realize resource utilization of CO_(2),which has gained wide popularity.With the introduction of CO_(2),coke deposition and metal reduction encountered in alkanes dehydrogenation reactions can be effectively suppressed.CO_(2)-assisted alkanes dehydrogenation can also reduce the risk of potential explosion hazard associated with O_(2)-oxidative dehydrogenation reactions.Recent investigations into various metal-based catalysts including mono-and bi-metallic alloys and oxides have displayed promising performances due to their unique properties.This paper provides the comprehensive review and critical analysis of advancements in the CO_(2)-assisted oxidative dehydrogenation of light alkanes(C2-C4)on metal-based catalysts developed in recent years.Moreover,it offers a comparative summary of the structural properties,catalytic activities,and reaction mechanisms over various active sites,providing valuable insights for the future design of dehydrogenation catalysts.展开更多
The continuous and excessive emission of CO_(2)into the atmosphere presents a pressing challenge for global sustainable development.In response,researchers have been devoting significant efforts to develop methods for...The continuous and excessive emission of CO_(2)into the atmosphere presents a pressing challenge for global sustainable development.In response,researchers have been devoting significant efforts to develop methods for converting CO_(2)into valuable chemicals and fuels.These conversions have the potential to establish a closed artificial carbon cycle and provide an alternative resource to depleting fossil fuels.Among the various conversion routes,thermochemical CO_(2)reduction stands out as a promising candidate for industrialization.Within the realm of heterogeneous catalysis,single atom catalysts(SACs)have garnered significant attention.The utilization of SACs offers tremendous potential for enhancing catalytic performance.To achieve optimal activity and selectivity of SACs in CO_(2)thermochemical reduction reactions,a comprehensive understanding of key factors such as single atom metal-support interactions,chemical coordination,and accessibility of active sites is crucial.Despite extensive research in this field,the atomic-scale reaction mechanisms in different chemical environments remain largely unexplored.While SACs have been found successful applications in electrochemical and photochemical CO_(2)reduction reactions,their implementation in thermochemical CO_(2)reduction encounters challenges due to the sintering and/or agglomeration effects that occur at elevated temperatures.In this review,we present a unique approach that combines theoretical understanding with experimental strategies to guide researchers in the design of controlled and thermally stable SACs.By elucidating the underlying principles,we aim to enable the creation of SACs that exhibit stable and efficient catalytic activity for thermochemical CO_(2)reduction reactions.Subsequently,we provide a comprehensive overview of recent literature on noble metal-and transition metal-based SACs for thermochemical CO_(2)reduction.The current review is focused on certain CO_(2)-derived products involving one step reduction only for simplicity and for better understanding the SACs enhancement mechanism.We emphasize various synthesis methods employed and highlight the catalytic activity of these SACs.Finally,we delve into the perspectives and challenges associated with SACs in the context of thermochemical CO_(2)reduction reactions,providing valuable insights for future research endeavor.Through this review,we aim to contribute to the advancement of SACs in the field of thermochemical CO_(2)reduction,shedding light on their potential as effective catalysts and addressing the challenges that need to be overcome for their successful implementation as paradigm shift in catalysis.展开更多
Thermo-hydro-mechanical-chemical(THMC)interactions are prevalent during CO_(2)geological sequestration(CGS).In this study,a sequential coupling THMC numerical simulation program was constructed,which can be used to ex...Thermo-hydro-mechanical-chemical(THMC)interactions are prevalent during CO_(2)geological sequestration(CGS).In this study,a sequential coupling THMC numerical simulation program was constructed,which can be used to explore the following issues of CGS:fluid and heat flow,solute transport;stresses,displacements and rock failures related to geo-mechanical effects;equilibrium and kinetic chemical reactions;chemical damage to mechanical properties of the rock.Then,the coupling program was applied to the Ordos CGS Project to study the formation response under the multifield interaction caused by CO_(2)injection.The simulation results show that the mechanical process dominates the short CO_(2)injection period.Specifically,the formation’s permeability near the injection well increases by 43%,due to the reduction of effective stress,which significantly promotes the lateral migration of CO_(2).When the injection rate exceeds 0.15 million tons per year,the cohesion of the reservoir rock is not enough to resist the shear force inside the rock and rock failure may occur.During the subsequent long-term sequestration period(200 years),the influence of mineral reactions gradually increases.Due to calcite dissolution,the shear modulus of caprock is predicted to decrease by 7.6%,which will to some extent increase the risk of rock failure.展开更多
Copper(Cu)-based materials are known as the most attractive catalysts for electrochemical carbon dioxide reduction reaction(CO_(2)RR),especially the Cu^(+) species(e.g.,Cu_(2)O),which show excellent capability for cat...Copper(Cu)-based materials are known as the most attractive catalysts for electrochemical carbon dioxide reduction reaction(CO_(2)RR),especially the Cu^(+) species(e.g.,Cu_(2)O),which show excellent capability for catalyzing CO_(2) to C_(2+) chemicals because of their unique electronic structure.However,the active Cu^(+) species are prone to be reduced to metallic Cu under an electroreduction environment,thus resulting in fast deactivation and poor selectivity.Here,we developed an advanced surface modification strategy to maintain the active Cu^(+) species via assembling a protective layer of metal-organic framework(copper benzenetricarboxylate,CuBTC) on the surface of Cu_(2)O octahedron(Cu_(2)O@CuBTC).It's encouraging to see that the Cu_(2)O@CuBTC heterostructure outperforms the bare Cu_(2)O octahedron in catalyzing CO_(2) to C_(2+) chemicals and dramatically enhances the ratio of C_(2)H_(4)/CH_(4) products.A systematic study reveals that the introduced CuBTC shell plays a critical role in maintaining the active Cu^(+) species in Cu_(2)O@CuBTC heterostructure under reductive conditions.This work offers a practical strategy for improving the catalytic performance of CO_(2)RR over copper oxides and also establishes a route to maintain the state of valence-sensitive catalysts.展开更多
An essential technology of carbon capture, utilization and storage-enhanced oil recovery (CCUS-EOR) for tight oil reservoirs is CO_(2) huff-puff followed by associated produced gas reinjection. In this paper, the effe...An essential technology of carbon capture, utilization and storage-enhanced oil recovery (CCUS-EOR) for tight oil reservoirs is CO_(2) huff-puff followed by associated produced gas reinjection. In this paper, the effects of multi-component gas on the properties and components of tight oil are studied. First, the core displacement experiments using the CH_(4)/CO_(2) multi-component gas are conducted to determine the oil displacement efficiency under different CO_(2) and CH_(4) ratios. Then, a viscometer and a liquid density balance are used to investigate the change characteristics of oil viscosity and density after multi-component gas displacement with different CO_(2) and CH_(4) ratios. In addition, a laboratory scale numerical model is established to validate the experimental results. Finally, a composition model of multi-stage fractured horizontal well in tight oil reservoir considering nano-confinement effects is established to investigate the effects of multi-component gas on the components of produced dead oil and formation crude oil. The experimental results show that the oil displacement efficiency of multi-component gas displacement is greater than that of single-component gas displacement. The CH_(4) decreases the viscosity and density of light oil, while CO_(2) decreases the viscosity but increases the density. And the numerical simulation results show that CO_(2) extracts more heavy components from the liquid phase into the vapor phase, while CH_(4) extracts more light components from the liquid phase into the vapor phase during cyclic gas injection. The multi-component gas can extract both the light components and the heavy components from oil, and the balanced production of each component can be achieved by using multi-component gas huff-puff.展开更多
The development of catalytic materials for the recycling CO_(2) through a myriad of available processes is an attractive field,especially given the current climate change.While there is increasing publication in this ...The development of catalytic materials for the recycling CO_(2) through a myriad of available processes is an attractive field,especially given the current climate change.While there is increasing publication in this field,the reported catalysts rarely deviate from the traditionally supported metal nanoparticle morphology,with the most simplistic method of enhancement being the addition of more metals to an already complex composition.Encapsulated catalysts,especially yolk@shell catalysts with hollow voids,offer answers to the most prominent issues faced by this field,coking and sintering,and further potential for more advanced phenomena,for example,the confinement effect,to promote selectivity or offer greater protection against coking and sintering.This work serves to demonstrate the current position of catalyst development in the fields of thermal CO_(2) reforming and hydrogenation,summarizing the most recent work available and most common metals used for these reactions,and how yolk@shell catalysts can offer superior performance and survivability in thermal CO_(2) reforming and hydrogenation to the more traditional structure.Furthermore,this work will briefly demonstrate the bespoke nature and highly variable yolk@shell structure.Moreover,this review aims to illuminate the spatial confinement effect and how it enhances yolk@shell structured nanoreactors is presented.展开更多
基金supported by Research Project Supported by Horizon Europe Framework Programme(101183092)Shanxi Scholarship Council of China(2023-128)+2 种基金National Natural Science Foundation of China(22208328)Fundamental Research Program of Shanxi Province(20210302124618)Small and mediumsized oriented scientific and technological enterprises innovation ability improvement project of Shandong Province(2023TSGC0004)。
文摘In this study,an integrated technology is proposed for the absorption and utilization of CO_(2)in alkanolamine solution for the preparation of BaCO_(3)in a high-gravity environment.The effects of absorbent type,high-gravity factor,gas/liquid ratio,and initial BaCl2concentration on the absorption rate and amount of CO_(2)and the preparation of BaCO_(3)are investigated.The results reveal that the absorption rate and amount of CO_(2)follow the order of ethyl alkanolamine(MEA)>diethanol amine(DEA)>N-methyldiethanolamine(MDEA),and thus MEA is the most effective absorbent for CO_(2)absorption.The absorption rate and amount of CO_(2)under high gravity are higher than that under normal gravity.Notably,the absorption rate at 75 min under high gravity is approximately 2 times that under normal gravity.This is because the centrifugal force resulting from the high-speed rotation of the packing can greatly increase gas-liquid mass transfer and micromixing.The particle size of BaCO_(3)prepared in the rotating packed bed is in the range of 57.2—89 nm,which is much smaller than that prepared in the bubbling reactor(>100.3 nm),and it also has higher purity(99.6%)and larger specific surface area(14.119 m^(2)·g^(-1)).It is concluded that the high-gravity technology has the potential to increase the absorption and utilization of CO_(2)in alkanolamine solution for the preparation of BaCO_(3).This study provides new insights into carbon emissions reduction and carbon utilization.
基金National Natural Science Foundation of China,Grant/Award Numbers:52076209,52006224,52106285,22179027Foundation and Applied Foundation Research of Guangdong Province,Grant/Award Number:2022B1515020045+1 种基金Natural Science Foundation of Guangxi Province,Grant/Award Number:2021GXNSFAA075036Young Talent Support Project of Guangzhou Association for Science and Technology,Grant/Award Number:QT‐2023‐042。
文摘By employing metal oxides as oxygen carriers,chemical looping demonstrates its effectiveness in transferring oxygen between reduction and oxidation environments to partially oxidize fuels into syngas and convert CO_(2) into CO.Generally,NiFe_(2_)O_(4) oxygen carriers have demonstrated remarkable efficiency in chemical looping CO_(2) conversion.Nevertheless,the intricate process of atomic migration and evolution within the internal structure of bimetallic oxygen carriers during continuous high‐temperature redox cycling remains unclear.Consequently,the lack of a fundamental understanding of the complex ionic migration and oxygen transfer associated with energy conversion processes hampers the design of high‐performance oxygen carriers.Thus,in this study,we employed in situ characterization techniques and theoretical calculations to investigate the ion migration behavior and structural evolution in the bulk of NiFe_(2_)O_(4) oxygen carriers during H_(2) reduction and CO_(2)/lab air oxidation cycles.We discovered that during the H_(2) reduction step,lattice oxygen rapidly migrates to vacancy layers to replenish consumed active oxygen species,while Ni leaches from the material and migrates to the surface.During the CO_(2) splitting step,Ni migrates toward the core of the bimetallic oxygen carrier,forming Fe–Ni alloys.During the air oxidation step,Fe–Ni migrates outward,creating a hollow structure owing to the Kirkendall effect triggered by the swift transfer of lattice oxygen.The metal atom migration paths depend on the oxygen transfer rates.These discoveries highlight the significance of regulating the release–recovery rate of lattice oxygen to uphold the structures and reactivity of oxygen carriers.This work offers a comprehensive understanding of the oxidation/reduction‐driven atomic interdiffusion behavior of bimetallic oxygen carriers.
文摘Chemical looping combustion has the potential to be an efficient and low-cost technology capable of contributing to the reduction of the atmospheric concentration of CO_(2) in order to reach the 1.5/2°C goal and mitigate climate change.In this process,a metal oxide is used as oxygen carrier in a dual fluidized bed to generate clean CO_(2) via combustion of biomass.Most commonly,natural ores or synthetic materials are used as oxygen carrier whereas both must meet special requirements for the conversion of solid fuels.Synthetic oxygen carriers are characterized by higher reactivity at the expense of higher costs versus the lower-cost natural ores.To determine the viability of both possibilities,a techno-economic comparison of a synthetic material based on manganese,iron,and copper to the natural ore ilmenite was conducted.The synthetic oxygen carrier was characterized and tested in a pilot plant,where high combustion efficiencies up to 98.4%and carbon capture rates up to 98.5%were reached.The techno-economic assessment resulted in CO_(2) capture costs of 75 and 40€/tCO_(2) for the synthetic and natural ore route respectively,whereas a sensitivity analysis showed the high impact of production costs and attrition rates of the synthetic material.The synthetic oxygen carrier could break even with the natural ore in case of lower production costs and attrition rates,which could be reached by adapting the production process and recycling material.By comparison to state-of-the-art technologies,it is demonstrated that both routes are viable and the capture cost of CO_(2) could be reduced by implementing the chemical looping combustion technology.
基金Supported by the National Natural Science Foundation of China(52234003,52222402,52304044).
文摘This work systematically reviews the complex mechanisms of CO_(2)-water-rock interactions,microscopic simulations of reactive transport(dissolution,precipitation and precipitate migration)in porous media,and microscopic simulations of CO_(2)-water-rock system.The work points out the key issues in current research and provides suggestions for future research.After injection of CO_(2) into underground reservoirs,not only conventional pressure-driven flow and mass transfer processes occur,but also special physicochemical phenomena like dissolution,precipitation,and precipitate migration.The coupling of these processes causes complex changes in permeability and porosity parameters of the porous media.Pore-scale microscopic flow simulations can provide detailed information within the three-dimensional pore and throat space and explicitly observe changes in the fluid-solid interfaces of porous media during reactions.At present,the research has limitations in the decoupling of complex mechanisms,characterization of differential multi-mineral reactions,precipitation generation mechanisms and characterization(crystal nucleation and mineral detachment),simulation methods for precipitation-fluid interaction,and coupling mechanisms of multiple physicochemical processes.In future studies,it is essential to innovate experimental methods to decouple“dissolution-precipitation-precipitate migration”processes,improve the accuracy of experimental testing of minerals geochemical reaction-related parameters,build reliable characterization of various precipitation types,establish precipitation-fluid interaction simulation methods,coordinate the boundary conditions of different physicochemical processes,and,finally,achieve coupled flow simulation of“dissolution-precipitation-precipitate migration”within CO_(2)-water-rock systems.
文摘Light olefins are important platform feedstocks in the petrochemical industry,and the ongoing global economic development has driven sustained growth in demand for these compounds.The dehydrogenation of alkanes,derived from shale gas,serves as an alternative olefins production route.Concurrently,the target of realizing carbon neutrality promotes the comprehensive utilization of greenhouse gas.The integrated process of light alkanes dehydrogenation and carbon dioxide reduction(CO_(2)-ODH)can produce light olefins and realize resource utilization of CO_(2),which has gained wide popularity.With the introduction of CO_(2),coke deposition and metal reduction encountered in alkanes dehydrogenation reactions can be effectively suppressed.CO_(2)-assisted alkanes dehydrogenation can also reduce the risk of potential explosion hazard associated with O_(2)-oxidative dehydrogenation reactions.Recent investigations into various metal-based catalysts including mono-and bi-metallic alloys and oxides have displayed promising performances due to their unique properties.This paper provides the comprehensive review and critical analysis of advancements in the CO_(2)-assisted oxidative dehydrogenation of light alkanes(C2-C4)on metal-based catalysts developed in recent years.Moreover,it offers a comparative summary of the structural properties,catalytic activities,and reaction mechanisms over various active sites,providing valuable insights for the future design of dehydrogenation catalysts.
基金support by Khalifa University through CIRA-2020-077 and RC2-2018-024 grants。
文摘The continuous and excessive emission of CO_(2)into the atmosphere presents a pressing challenge for global sustainable development.In response,researchers have been devoting significant efforts to develop methods for converting CO_(2)into valuable chemicals and fuels.These conversions have the potential to establish a closed artificial carbon cycle and provide an alternative resource to depleting fossil fuels.Among the various conversion routes,thermochemical CO_(2)reduction stands out as a promising candidate for industrialization.Within the realm of heterogeneous catalysis,single atom catalysts(SACs)have garnered significant attention.The utilization of SACs offers tremendous potential for enhancing catalytic performance.To achieve optimal activity and selectivity of SACs in CO_(2)thermochemical reduction reactions,a comprehensive understanding of key factors such as single atom metal-support interactions,chemical coordination,and accessibility of active sites is crucial.Despite extensive research in this field,the atomic-scale reaction mechanisms in different chemical environments remain largely unexplored.While SACs have been found successful applications in electrochemical and photochemical CO_(2)reduction reactions,their implementation in thermochemical CO_(2)reduction encounters challenges due to the sintering and/or agglomeration effects that occur at elevated temperatures.In this review,we present a unique approach that combines theoretical understanding with experimental strategies to guide researchers in the design of controlled and thermally stable SACs.By elucidating the underlying principles,we aim to enable the creation of SACs that exhibit stable and efficient catalytic activity for thermochemical CO_(2)reduction reactions.Subsequently,we provide a comprehensive overview of recent literature on noble metal-and transition metal-based SACs for thermochemical CO_(2)reduction.The current review is focused on certain CO_(2)-derived products involving one step reduction only for simplicity and for better understanding the SACs enhancement mechanism.We emphasize various synthesis methods employed and highlight the catalytic activity of these SACs.Finally,we delve into the perspectives and challenges associated with SACs in the context of thermochemical CO_(2)reduction reactions,providing valuable insights for future research endeavor.Through this review,we aim to contribute to the advancement of SACs in the field of thermochemical CO_(2)reduction,shedding light on their potential as effective catalysts and addressing the challenges that need to be overcome for their successful implementation as paradigm shift in catalysis.
基金jointly supported by the National Natural Science Foundation of China(Grant No.42141013)the CNPC Innovation Found(2021 D002-1102)the China Postdoctoral Science Foundation(No.2021M701379)。
文摘Thermo-hydro-mechanical-chemical(THMC)interactions are prevalent during CO_(2)geological sequestration(CGS).In this study,a sequential coupling THMC numerical simulation program was constructed,which can be used to explore the following issues of CGS:fluid and heat flow,solute transport;stresses,displacements and rock failures related to geo-mechanical effects;equilibrium and kinetic chemical reactions;chemical damage to mechanical properties of the rock.Then,the coupling program was applied to the Ordos CGS Project to study the formation response under the multifield interaction caused by CO_(2)injection.The simulation results show that the mechanical process dominates the short CO_(2)injection period.Specifically,the formation’s permeability near the injection well increases by 43%,due to the reduction of effective stress,which significantly promotes the lateral migration of CO_(2).When the injection rate exceeds 0.15 million tons per year,the cohesion of the reservoir rock is not enough to resist the shear force inside the rock and rock failure may occur.During the subsequent long-term sequestration period(200 years),the influence of mineral reactions gradually increases.Due to calcite dissolution,the shear modulus of caprock is predicted to decrease by 7.6%,which will to some extent increase the risk of rock failure.
基金the Fundamental Research Funds for Central Universities (BLX202151)the National Natural Science Foundation of China (22208021, 52225003, 22109004)。
文摘Copper(Cu)-based materials are known as the most attractive catalysts for electrochemical carbon dioxide reduction reaction(CO_(2)RR),especially the Cu^(+) species(e.g.,Cu_(2)O),which show excellent capability for catalyzing CO_(2) to C_(2+) chemicals because of their unique electronic structure.However,the active Cu^(+) species are prone to be reduced to metallic Cu under an electroreduction environment,thus resulting in fast deactivation and poor selectivity.Here,we developed an advanced surface modification strategy to maintain the active Cu^(+) species via assembling a protective layer of metal-organic framework(copper benzenetricarboxylate,CuBTC) on the surface of Cu_(2)O octahedron(Cu_(2)O@CuBTC).It's encouraging to see that the Cu_(2)O@CuBTC heterostructure outperforms the bare Cu_(2)O octahedron in catalyzing CO_(2) to C_(2+) chemicals and dramatically enhances the ratio of C_(2)H_(4)/CH_(4) products.A systematic study reveals that the introduced CuBTC shell plays a critical role in maintaining the active Cu^(+) species in Cu_(2)O@CuBTC heterostructure under reductive conditions.This work offers a practical strategy for improving the catalytic performance of CO_(2)RR over copper oxides and also establishes a route to maintain the state of valence-sensitive catalysts.
基金supported by the National Natural Science Foundation of China(No.52174038 and No.52004307)China Petroleum Science and Technology Project-major project-Research on tight oil-shale oil reservoir engineering methods and key technologies in Ordos Basin(ZLZX2020-02-04)Science Foundation of China University of Petroleum,Beijing(No.2462018YJRC015).
文摘An essential technology of carbon capture, utilization and storage-enhanced oil recovery (CCUS-EOR) for tight oil reservoirs is CO_(2) huff-puff followed by associated produced gas reinjection. In this paper, the effects of multi-component gas on the properties and components of tight oil are studied. First, the core displacement experiments using the CH_(4)/CO_(2) multi-component gas are conducted to determine the oil displacement efficiency under different CO_(2) and CH_(4) ratios. Then, a viscometer and a liquid density balance are used to investigate the change characteristics of oil viscosity and density after multi-component gas displacement with different CO_(2) and CH_(4) ratios. In addition, a laboratory scale numerical model is established to validate the experimental results. Finally, a composition model of multi-stage fractured horizontal well in tight oil reservoir considering nano-confinement effects is established to investigate the effects of multi-component gas on the components of produced dead oil and formation crude oil. The experimental results show that the oil displacement efficiency of multi-component gas displacement is greater than that of single-component gas displacement. The CH_(4) decreases the viscosity and density of light oil, while CO_(2) decreases the viscosity but increases the density. And the numerical simulation results show that CO_(2) extracts more heavy components from the liquid phase into the vapor phase, while CH_(4) extracts more light components from the liquid phase into the vapor phase during cyclic gas injection. The multi-component gas can extract both the light components and the heavy components from oil, and the balanced production of each component can be achieved by using multi-component gas huff-puff.
基金Financial support was provided by the Chinese Academy of Sciences–The World Academy of Sciences(CAS-TWAS)president fellowship。
文摘The development of catalytic materials for the recycling CO_(2) through a myriad of available processes is an attractive field,especially given the current climate change.While there is increasing publication in this field,the reported catalysts rarely deviate from the traditionally supported metal nanoparticle morphology,with the most simplistic method of enhancement being the addition of more metals to an already complex composition.Encapsulated catalysts,especially yolk@shell catalysts with hollow voids,offer answers to the most prominent issues faced by this field,coking and sintering,and further potential for more advanced phenomena,for example,the confinement effect,to promote selectivity or offer greater protection against coking and sintering.This work serves to demonstrate the current position of catalyst development in the fields of thermal CO_(2) reforming and hydrogenation,summarizing the most recent work available and most common metals used for these reactions,and how yolk@shell catalysts can offer superior performance and survivability in thermal CO_(2) reforming and hydrogenation to the more traditional structure.Furthermore,this work will briefly demonstrate the bespoke nature and highly variable yolk@shell structure.Moreover,this review aims to illuminate the spatial confinement effect and how it enhances yolk@shell structured nanoreactors is presented.
