To enhance the separation selectivity of Mg-MOF-74 towards CO_(2) in a CO_(2)/N_(2) mixture,a series of Mg-MOF-74 and Ni_(x)/Mg_(1-x)-MOF-74 adsorbents were prepared by solvothermal synthesis in this paper.It was foun...To enhance the separation selectivity of Mg-MOF-74 towards CO_(2) in a CO_(2)/N_(2) mixture,a series of Mg-MOF-74 and Ni_(x)/Mg_(1-x)-MOF-74 adsorbents were prepared by solvothermal synthesis in this paper.It was found that the adsorption capacity of Mg-MOF-74 for CO_(2) could be effectively increased by optimizing the amount of acetic acid.On this basis,the bimetal MOF-74 adsorbent was prepared by metal modification.The multi-component dynamic adsorption penetration analysis was utilized to examine the CO_(2) adsorption capacity and CO_(2)/N_(2) selectivity of the diverse adsorbent materials.The results showed that Ni0.11/Mg0.89-MOF-74 showed a CO_(2) adsorption capacity of 7.02 mmol/g under pure CO_(2) atmosphere and had a selectivity of 20.50 for CO_(2)/N_(2) under 15% CO_(2)/85%N_(2) conditions,which was 10.2% and 18.02% higher than that of Mg-MOF-74 respectively.Combining XPS,SEM and N_(2) adsorption-desorption characterization analysis,it was attributed to the effect of the more stable unsaturated metal sites Ni into the Mg-MOF-74 on the pore structure and the synergistic interaction between the two metals.Density Functional Theory(DFT)simulations revealed that the synergistic interaction between modulated the electrostatic potential strength and gradient of the material,which was more favorable for the adsorption of CO_(2) molecules with small diameters and large quadrupole moment.In addition,the Ni0.11/Mg0.89-MOF-74 showed commendable cyclic stability,underscoring its promising potential for practical applications.展开更多
Utilizing sunlight to convert CO_(2) into chemical fuels could address the greenhouse effect and fossil fuel crisis,Heterojunction structure catalysts with oxygen vacancy are attractive in the field of photocatalytic ...Utilizing sunlight to convert CO_(2) into chemical fuels could address the greenhouse effect and fossil fuel crisis,Heterojunction structure catalysts with oxygen vacancy are attractive in the field of photocatalytic CO_(2) conversion.Herein,a modified TiO_(2)/In_(2)O_(3)(R-P2 5/In_(2)O_(3-x)) type Ⅱ heterojunction composite with oxygen vacancies is designed for photocatalytic CO_(2) reduction,which exhibits excellent CO_(2) reduction activity,with a C_(2) selectivity of 56.66%(in terms of R_(electron)).In situ Fourier-transform infrared spectroscopy(DRIFTS) and time-resolved photoluminescence(TR-PL) spectroscopy are used to reveal the intermediate formation of the photocatalytic mechanism and photogenerated electron lifetime,respectively.The experimental characterizations reveal that the R-P25/In_(2)O_(3-x) composite shows a remarkable behavior for coupling C-C bonds.Besides,efficient charge separation contributes to the improved CO_(2) conversion performance of photocatalysts.This work introduces a type Ⅱ heterojunction composite photocatalyst,which promotes understanding the CO_(2) reduction mechanisms on heterojunction composites and is valuable for the development of photocatalysts.展开更多
Mixed matrix membranes(MMMs)could combine the advantages of both polymeric membranes and porousfillers,making them an effective alternative to conventional polymer membranes.However,interfacial incompatibility issues,s...Mixed matrix membranes(MMMs)could combine the advantages of both polymeric membranes and porousfillers,making them an effective alternative to conventional polymer membranes.However,interfacial incompatibility issues,such as the presence of interfacial voids,hardening of polymer chains,and blockage of micropores by polymers between common MMMsfillers and the polymer matrix,currently limit the gas sep-aration performance of MMMs.Ternary phase MMMs(consisting of afiller,an additive,and a matrix)made by adding a third compound,usually functionalized additives,can overcome the structural problems of binary phase MMMs and positively impact membrane separation performance.This review introduces the structure and fabrication processes for ternary MMMs,categorizes various nanofillers and the third component,and summarizes and analyzes in detail the CO_(2) separation performance of newly developed ternary MMMs based on both rubbery and glassy polymers.Based on this separation data,the challenges of ternary MMMs are also discussed.Finally,future directions for ternary MMMs are proposed.展开更多
A novel system was proposed for the capture and separation of CO 2 from flue gas. In this method, a resin was employed to regenerate the amine capturing CO 2 from flue gas at room temperature. The feasibility for ...A novel system was proposed for the capture and separation of CO 2 from flue gas. In this method, a resin was employed to regenerate the amine capturing CO 2 from flue gas at room temperature. The feasibility for the resin to regenerate amines such as MEA, MAE, TEA, and ammonia was demonstrated. It was also discovered that the resin could be regenerated by hot water.展开更多
Rational design of ionic liquids(ILs),which is highly dependent on the accuracy of the model used,has always been crucial for CO_(2)separation from flue gas.In this study,a support vector machine(SVM)model which is a ...Rational design of ionic liquids(ILs),which is highly dependent on the accuracy of the model used,has always been crucial for CO_(2)separation from flue gas.In this study,a support vector machine(SVM)model which is a machine learning approach is established,so as to improve the prediction accuracy and range of IL melting points.Based on IL melting points data with 600 training data and 168 testing data,the estimated average absolute relative deviations(AARD)and squared correlation coefficients(R^(2))are 3.11%,0.8820 and 5.12%,0.8542 for the training set and testing set of the SVM model,respectively.Then,through the melting points model and other rational design processes including conductor-like screening model for real solvents(COSMO-RS)calculation and physical property constraints,cyano-based ILs are obtained,in which tetracyanoborate[TCB]-is often ruled out due to incorrect estimation of melting points model in the literature.Subsequently,by means of process simulation using Aspen Plus,optimal IL are compared with excellent IL reported in the literature.Finally,1-ethyl-3-methylimidazolium tricyanomethanide[EMIM][TCM]is selected as a most suitable solvent for CO_(2)separation from flue gas,the process of which leads to 12.9%savings on total annualized cost compared to that of 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)amide[EMIM][Tf_(2)N].展开更多
氮化硅是一种良好的载体,具有较高的水热稳定性和机械稳定性,其表面的氨基基团能够较好地锚定金属,显著提高金属分散度。但是,商品氮化硅比表面积较低,对金属分散作用仍然有限。因此,以自制的高比表面积氮化硅(Si_(3)N_(4))为载体,通过...氮化硅是一种良好的载体,具有较高的水热稳定性和机械稳定性,其表面的氨基基团能够较好地锚定金属,显著提高金属分散度。但是,商品氮化硅比表面积较低,对金属分散作用仍然有限。因此,以自制的高比表面积氮化硅(Si_(3)N_(4))为载体,通过浸渍法制备了不同Ru负载量(质量分数分别为0.5%、1.0%和2.0%)的催化剂(分别为0.5%Ru/Si_(3)N_(4)、1.0%Ru/Si_(3)N_(4)和2.0%Ru/Si_(3)N_(4)),并以商品氮化硅(Si_(3)N_(4)-C)为载体制备了2.0%Ru/Si_(3)N_(4)-C催化剂作为对照组。表征了催化剂的理化性质,测试了其在300℃、0.1 MPa下的CO_(2)加氢反应活性。结果显示,与Si_(3)N_(4)-C相比,Si_(3)N_(4)的比表面积较高(502 m^(2)/g),Si_(3)N_(4)作为载体显著提高了金属分散度,降低了金属粒径,催化剂暴露出更多的活性位点。0.5%Ru/Si_(3)N_(4)的金属粒径较小,展现出强的H_(2)吸附能力,H难以解吸,抑制了中间物种CO加氢生成CH_(4)。随着Ru负载量增加,金属粒径增大,催化剂的CH_(4)选择性更好。Ru/Si_(3)N_(4)系列催化剂中,2.0%Ru/Si_(3)N_(4)的CH_(4)选择性较高(98.8%)。空速为10000 m L/(g·h)时,0.5%Ru/Si_(3)N_(4)的CO选择性为88.2%。与2.0%Ru/Si_(3)N_(4)相比,2.0%Ru/Si_(3)N_(4)-C的金属粒径更大,活性位点较少,活性更低。2.0%Ru/Si_(3)N_(4)和2.0%Ru/Si_(3)N_(4)-C的CO_(2)转化率分别为53.1%和9.2%。Si_(3)N_(4)有效提高了金属分散度,提高了催化剂的CO_(2)加氢反应活性;通过调控Ru负载量控制催化剂金属粒径,可实现对产物CO或CH_(4)选择性的调控。展开更多
The CO2 separation from natural gas, syngas or flue gas represents an important industrial field of applications. An economic and energy-efficient CO2 separation from these gas streams is a prerequisite for sustainabl...The CO2 separation from natural gas, syngas or flue gas represents an important industrial field of applications. An economic and energy-efficient CO2 separation from these gas streams is a prerequisite for sustainable industry contributions to the megatrends resource efficiency and globalization of technologies. One way of reducing operational expenditure for these separation processes is the development of better performing CO2 absorbents. Although a number of absorbents for the separation of CO2 from process gas streams exist, the need for the development of CO2 absorbents with an improved absorption performance, less corrosion and foaming, no nitrosamine formation, lower energy requirement and therefore less operational expenditure remains. Recent industrial activities have led to the development of novel high-performance CO2 scrubbing agents that can be employed in numerous industrial processes such as natural gas treatment, purification of syngas and the scrubbing of flue gas. The objective of this paper is to introduce these new high-performance scrubbing agents and to compare their performance with other state-of-the-art absorbents. It turned out, that the evaluated absorbents offer high cyclic capacities in the range of 2.4 to 2.6 mol CO2/kg absorbent and low absorption enthalpies (–30 kJ/mol) allowing for distinctive savings in the regeneration energy of the absorbent. Calculations with the modified Kremser model resulted in a reduction of the specific reboiler heat duty of 55%. Furthermore, the absorbents are less corrosive than standard amines as indicated by the measured corrosion rates of 0.21 mm/y versus 1.18 mm/y for a piperazine/methyldiethanolamine mixture. Based on new experimental results it is shown how substantial savings in operational and capital expenditure can be realized due to favorable absorbent properties. The novel high-performance CO2 system solutions meet recent industrial absorbent requirements and allow for more efficient or new CO2 separation processes.展开更多
"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
Efficiently enriching low-concentration CH4 is pivotal for enhancing the utilization of unconventional energy sources and mitigating greenhouse gas emissions.This study focuses on modifying the overall performance of ...Efficiently enriching low-concentration CH4 is pivotal for enhancing the utilization of unconventional energy sources and mitigating greenhouse gas emissions.This study focuses on modifying the overall performance of CH_(4)/N_(2)separation membranes.A novel mixed matrix membrane(MMM)with a reinforced substrate structure was developed through a straightforward dip-coating technique.This MMM incorporates a polytetrafluoroethylene(PTFE)porous membrane as the supporting framework,while a composite of block polymer(styrene-butadiene-styrene)and metal-organic framework(Ni-MOF-74)forms the selective separation layer.Comprehensive characterization of Ni-MOF-74 and the fabricatedmembranes was conducted using X-rays diffraction,scanning electron microscope,Brunauer-Emmett-Teller analysis,and gas permeance tests.The findings indicate a robust integration of the PTFE porous support with the membrane layer,enhancing the mechanical stability of theMMM.Under optimal conditions,the mechanical strength of the PM20 membrane(containing 20%Ni-MOF-74)was observed to be 37.7 MPa,representing remarkable increase compared to the non-reinforcedMMM.Additionally,thePM20membrane exhibited an impressive CH4 permeation rate of 92 barrer(1 barrer﹦3.35×10^(-16)mol·m·m^(-2)·s^(-1)·Pa^(-1))alongside a CH_(4)/N_(2)selectivity of 4.18.These results underscore the MMM's substantial performance and its promising potential in methane enrichment applications.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
Zinc indium sulfide(ZnIn_(2)S_(4),ZIS),a novel photocatalyst with layered nanostructure,has drawn significant attention in the field of photocatalytic CO_(2)reduction in recent years due to various advantages,includin...Zinc indium sulfide(ZnIn_(2)S_(4),ZIS),a novel photocatalyst with layered nanostructure,has drawn significant attention in the field of photocatalytic CO_(2)reduction in recent years due to various advantages,including non-toxicity,structural stability,easy availability,and suitable band gap.We introduce the types of ZIS-based nanomaterials and their action mechanism in photocatalytic CO_(2)reduction.Moreover,we put forward prospects in the future development directions of ZIS-based nanomaterials for photocatalytic CO_(2)reduction.展开更多
Zinc indium sulfide(ZnIn_(2)S_(4),ZIS),a novel photocatalyst with layered nanostructure,has drawn significant attention in the field of photocatalytic CO_(2) reduction in recent years due to various advantages,includi...Zinc indium sulfide(ZnIn_(2)S_(4),ZIS),a novel photocatalyst with layered nanostructure,has drawn significant attention in the field of photocatalytic CO_(2) reduction in recent years due to various advantages,including non-toxicity,structural stability,easy availability,and suitable band gap.We introduced the types of ZISbased nanomaterials and their action mechanism in photocatalytic CO_(2) reduction.Moreover,we put forward prospects in the future development directions of ZIS-based nanomaterials for photocatalytic CO_(2) reduction.展开更多
基金supported by National Natural Science Foundation of China(U23A20100)the Strategic Priority Research Program(A)of the Chinese Academy of Sciences(XDA0390404)+5 种基金ICC CAS SCJC-DT-2023-03,the Foundation of State Key Laboratory of Coal Conversion(J24-25-619)Youth Innovation Promotion Association CAS(2018209,2020179)Key R&D Program of Shanxi Province(202102090301008,202202090301013)the special fund for S&T Innovation Team of Shanxi Province(202204051001012)Project of International Cooperation and Exchange NSFC-RFBR(22011530069)Tianjin Science and Technology Plan Project(22YFYSHZ00290)。
文摘To enhance the separation selectivity of Mg-MOF-74 towards CO_(2) in a CO_(2)/N_(2) mixture,a series of Mg-MOF-74 and Ni_(x)/Mg_(1-x)-MOF-74 adsorbents were prepared by solvothermal synthesis in this paper.It was found that the adsorption capacity of Mg-MOF-74 for CO_(2) could be effectively increased by optimizing the amount of acetic acid.On this basis,the bimetal MOF-74 adsorbent was prepared by metal modification.The multi-component dynamic adsorption penetration analysis was utilized to examine the CO_(2) adsorption capacity and CO_(2)/N_(2) selectivity of the diverse adsorbent materials.The results showed that Ni0.11/Mg0.89-MOF-74 showed a CO_(2) adsorption capacity of 7.02 mmol/g under pure CO_(2) atmosphere and had a selectivity of 20.50 for CO_(2)/N_(2) under 15% CO_(2)/85%N_(2) conditions,which was 10.2% and 18.02% higher than that of Mg-MOF-74 respectively.Combining XPS,SEM and N_(2) adsorption-desorption characterization analysis,it was attributed to the effect of the more stable unsaturated metal sites Ni into the Mg-MOF-74 on the pore structure and the synergistic interaction between the two metals.Density Functional Theory(DFT)simulations revealed that the synergistic interaction between modulated the electrostatic potential strength and gradient of the material,which was more favorable for the adsorption of CO_(2) molecules with small diameters and large quadrupole moment.In addition,the Ni0.11/Mg0.89-MOF-74 showed commendable cyclic stability,underscoring its promising potential for practical applications.
基金National Research Foundation (NRF) of Korea grant funded by the Korea Government (MSIT) (NRF-2022R1A2C2093415)partially funding from the Circle Foundation (Republic of Korea) (Grant Number: 2023 TCF Innovative Science Project-03))partially Korea Basic Science Institute (National Research Facilities and Equipment Center) grant funded by the Ministry of Education (2022R1A6C101A751)。
文摘Utilizing sunlight to convert CO_(2) into chemical fuels could address the greenhouse effect and fossil fuel crisis,Heterojunction structure catalysts with oxygen vacancy are attractive in the field of photocatalytic CO_(2) conversion.Herein,a modified TiO_(2)/In_(2)O_(3)(R-P2 5/In_(2)O_(3-x)) type Ⅱ heterojunction composite with oxygen vacancies is designed for photocatalytic CO_(2) reduction,which exhibits excellent CO_(2) reduction activity,with a C_(2) selectivity of 56.66%(in terms of R_(electron)).In situ Fourier-transform infrared spectroscopy(DRIFTS) and time-resolved photoluminescence(TR-PL) spectroscopy are used to reveal the intermediate formation of the photocatalytic mechanism and photogenerated electron lifetime,respectively.The experimental characterizations reveal that the R-P25/In_(2)O_(3-x) composite shows a remarkable behavior for coupling C-C bonds.Besides,efficient charge separation contributes to the improved CO_(2) conversion performance of photocatalysts.This work introduces a type Ⅱ heterojunction composite photocatalyst,which promotes understanding the CO_(2) reduction mechanisms on heterojunction composites and is valuable for the development of photocatalysts.
基金support from Sichuan Science and Technology Program(2021YFH0116)National Natural Science Foundation of China(No.52170112)DongFang Boiler Co.,Ltd.(3522015).
文摘Mixed matrix membranes(MMMs)could combine the advantages of both polymeric membranes and porousfillers,making them an effective alternative to conventional polymer membranes.However,interfacial incompatibility issues,such as the presence of interfacial voids,hardening of polymer chains,and blockage of micropores by polymers between common MMMsfillers and the polymer matrix,currently limit the gas sep-aration performance of MMMs.Ternary phase MMMs(consisting of afiller,an additive,and a matrix)made by adding a third compound,usually functionalized additives,can overcome the structural problems of binary phase MMMs and positively impact membrane separation performance.This review introduces the structure and fabrication processes for ternary MMMs,categorizes various nanofillers and the third component,and summarizes and analyzes in detail the CO_(2) separation performance of newly developed ternary MMMs based on both rubbery and glassy polymers.Based on this separation data,the challenges of ternary MMMs are also discussed.Finally,future directions for ternary MMMs are proposed.
文摘A novel system was proposed for the capture and separation of CO 2 from flue gas. In this method, a resin was employed to regenerate the amine capturing CO 2 from flue gas at room temperature. The feasibility for the resin to regenerate amines such as MEA, MAE, TEA, and ammonia was demonstrated. It was also discovered that the resin could be regenerated by hot water.
基金the financial support by the National Natural Science Foundation of China(Project No.21878054)the Natural Science Foundation of Fujian Province of China(2020J01515)
文摘Rational design of ionic liquids(ILs),which is highly dependent on the accuracy of the model used,has always been crucial for CO_(2)separation from flue gas.In this study,a support vector machine(SVM)model which is a machine learning approach is established,so as to improve the prediction accuracy and range of IL melting points.Based on IL melting points data with 600 training data and 168 testing data,the estimated average absolute relative deviations(AARD)and squared correlation coefficients(R^(2))are 3.11%,0.8820 and 5.12%,0.8542 for the training set and testing set of the SVM model,respectively.Then,through the melting points model and other rational design processes including conductor-like screening model for real solvents(COSMO-RS)calculation and physical property constraints,cyano-based ILs are obtained,in which tetracyanoborate[TCB]-is often ruled out due to incorrect estimation of melting points model in the literature.Subsequently,by means of process simulation using Aspen Plus,optimal IL are compared with excellent IL reported in the literature.Finally,1-ethyl-3-methylimidazolium tricyanomethanide[EMIM][TCM]is selected as a most suitable solvent for CO_(2)separation from flue gas,the process of which leads to 12.9%savings on total annualized cost compared to that of 1-ethyl-3-methylimidazolium bis(trifluoromethylsulfonyl)amide[EMIM][Tf_(2)N].
文摘氮化硅是一种良好的载体,具有较高的水热稳定性和机械稳定性,其表面的氨基基团能够较好地锚定金属,显著提高金属分散度。但是,商品氮化硅比表面积较低,对金属分散作用仍然有限。因此,以自制的高比表面积氮化硅(Si_(3)N_(4))为载体,通过浸渍法制备了不同Ru负载量(质量分数分别为0.5%、1.0%和2.0%)的催化剂(分别为0.5%Ru/Si_(3)N_(4)、1.0%Ru/Si_(3)N_(4)和2.0%Ru/Si_(3)N_(4)),并以商品氮化硅(Si_(3)N_(4)-C)为载体制备了2.0%Ru/Si_(3)N_(4)-C催化剂作为对照组。表征了催化剂的理化性质,测试了其在300℃、0.1 MPa下的CO_(2)加氢反应活性。结果显示,与Si_(3)N_(4)-C相比,Si_(3)N_(4)的比表面积较高(502 m^(2)/g),Si_(3)N_(4)作为载体显著提高了金属分散度,降低了金属粒径,催化剂暴露出更多的活性位点。0.5%Ru/Si_(3)N_(4)的金属粒径较小,展现出强的H_(2)吸附能力,H难以解吸,抑制了中间物种CO加氢生成CH_(4)。随着Ru负载量增加,金属粒径增大,催化剂的CH_(4)选择性更好。Ru/Si_(3)N_(4)系列催化剂中,2.0%Ru/Si_(3)N_(4)的CH_(4)选择性较高(98.8%)。空速为10000 m L/(g·h)时,0.5%Ru/Si_(3)N_(4)的CO选择性为88.2%。与2.0%Ru/Si_(3)N_(4)相比,2.0%Ru/Si_(3)N_(4)-C的金属粒径更大,活性位点较少,活性更低。2.0%Ru/Si_(3)N_(4)和2.0%Ru/Si_(3)N_(4)-C的CO_(2)转化率分别为53.1%和9.2%。Si_(3)N_(4)有效提高了金属分散度,提高了催化剂的CO_(2)加氢反应活性;通过调控Ru负载量控制催化剂金属粒径,可实现对产物CO或CH_(4)选择性的调控。
文摘The CO2 separation from natural gas, syngas or flue gas represents an important industrial field of applications. An economic and energy-efficient CO2 separation from these gas streams is a prerequisite for sustainable industry contributions to the megatrends resource efficiency and globalization of technologies. One way of reducing operational expenditure for these separation processes is the development of better performing CO2 absorbents. Although a number of absorbents for the separation of CO2 from process gas streams exist, the need for the development of CO2 absorbents with an improved absorption performance, less corrosion and foaming, no nitrosamine formation, lower energy requirement and therefore less operational expenditure remains. Recent industrial activities have led to the development of novel high-performance CO2 scrubbing agents that can be employed in numerous industrial processes such as natural gas treatment, purification of syngas and the scrubbing of flue gas. The objective of this paper is to introduce these new high-performance scrubbing agents and to compare their performance with other state-of-the-art absorbents. It turned out, that the evaluated absorbents offer high cyclic capacities in the range of 2.4 to 2.6 mol CO2/kg absorbent and low absorption enthalpies (–30 kJ/mol) allowing for distinctive savings in the regeneration energy of the absorbent. Calculations with the modified Kremser model resulted in a reduction of the specific reboiler heat duty of 55%. Furthermore, the absorbents are less corrosive than standard amines as indicated by the measured corrosion rates of 0.21 mm/y versus 1.18 mm/y for a piperazine/methyldiethanolamine mixture. Based on new experimental results it is shown how substantial savings in operational and capital expenditure can be realized due to favorable absorbent properties. The novel high-performance CO2 system solutions meet recent industrial absorbent requirements and allow for more efficient or new CO2 separation processes.
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financial support from the National Natural Science Foundation of China(52174229 and 52174230)the Natural Science Foundation of Liaoning Province(2022-KF-13-05)+1 种基金Fushun Revitalization Talents Program(FSYC202107010)the program funded by Liaoning Province Education Administration(LJKZ0411).
文摘Efficiently enriching low-concentration CH4 is pivotal for enhancing the utilization of unconventional energy sources and mitigating greenhouse gas emissions.This study focuses on modifying the overall performance of CH_(4)/N_(2)separation membranes.A novel mixed matrix membrane(MMM)with a reinforced substrate structure was developed through a straightforward dip-coating technique.This MMM incorporates a polytetrafluoroethylene(PTFE)porous membrane as the supporting framework,while a composite of block polymer(styrene-butadiene-styrene)and metal-organic framework(Ni-MOF-74)forms the selective separation layer.Comprehensive characterization of Ni-MOF-74 and the fabricatedmembranes was conducted using X-rays diffraction,scanning electron microscope,Brunauer-Emmett-Teller analysis,and gas permeance tests.The findings indicate a robust integration of the PTFE porous support with the membrane layer,enhancing the mechanical stability of theMMM.Under optimal conditions,the mechanical strength of the PM20 membrane(containing 20%Ni-MOF-74)was observed to be 37.7 MPa,representing remarkable increase compared to the non-reinforcedMMM.Additionally,thePM20membrane exhibited an impressive CH4 permeation rate of 92 barrer(1 barrer﹦3.35×10^(-16)mol·m·m^(-2)·s^(-1)·Pa^(-1))alongside a CH_(4)/N_(2)selectivity of 4.18.These results underscore the MMM's substantial performance and its promising potential in methane enrichment applications.
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.
文摘Zinc indium sulfide(ZnIn_(2)S_(4),ZIS),a novel photocatalyst with layered nanostructure,has drawn significant attention in the field of photocatalytic CO_(2)reduction in recent years due to various advantages,including non-toxicity,structural stability,easy availability,and suitable band gap.We introduce the types of ZIS-based nanomaterials and their action mechanism in photocatalytic CO_(2)reduction.Moreover,we put forward prospects in the future development directions of ZIS-based nanomaterials for photocatalytic CO_(2)reduction.
文摘Zinc indium sulfide(ZnIn_(2)S_(4),ZIS),a novel photocatalyst with layered nanostructure,has drawn significant attention in the field of photocatalytic CO_(2) reduction in recent years due to various advantages,including non-toxicity,structural stability,easy availability,and suitable band gap.We introduced the types of ZISbased nanomaterials and their action mechanism in photocatalytic CO_(2) reduction.Moreover,we put forward prospects in the future development directions of ZIS-based nanomaterials for photocatalytic CO_(2) reduction.
