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
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
Environment friendly and intelligent surfactants have attracted great attention in recent years.A bio-based CO_(2)responsive surfactant rosin acid dimaleimide choline(R-BMI-C)with an extremely rigid skeleton was prepa...Environment friendly and intelligent surfactants have attracted great attention in recent years.A bio-based CO_(2)responsive surfactant rosin acid dimaleimide choline(R-BMI-C)with an extremely rigid skeleton was prepared using rosin and choline as raw materials by Diels-Alder addition reaction and acid-base neutralization reactions.Its structure was confirmed by IR and^(1)H NMR spectra.The foams’properties of R-BMI-C could be adjusted by bubbling CO_(2)/N_(2)to change the structure of the surfactant.At pH 10.4,R-BMI-C forms an unstable foam with a half-life of 1.5 h.When the pH was reduced to 7.4 by bubbling CO_(2),R-BMI-C forms an extremely stable foam with a half-life of 336 h.The surfactant R-BMI-C changed from bola type to conventional type when bubbling CO_(2).And the internal aggregation structure of R-BMI-C aqueous solution changed from spherical micelles to laminar micelles according to the cryogenic-transmission electron microscope.We know that the lamellar structure tends to adsorb at the air/water interface or is trapped in the foam film,which slows down the foam coarsening and agglomeration process,resulting in a significant increase in foam stability.R-BMI-C could be used in oil extraction,fire-fighting and chemical decontamination due to its excellent foaming,stabilization and defoaming properties.展开更多
In this study, we developed a strategy for using the Scoggins procedure in the synthesis of acetamidines as novel C02-triggered switchable surfactants via acetimidates by effectively tuning the chemical equilibrium. T...In this study, we developed a strategy for using the Scoggins procedure in the synthesis of acetamidines as novel C02-triggered switchable surfactants via acetimidates by effectively tuning the chemical equilibrium. The as-synthesized N'-alkyl-N,Ndiethylacetamidines exhibit excellent CO_2/N_2 switchability and their bicarbonate salts have the ability to emulsify oil-water mixtures.展开更多
This article reports the development of a novel switchable Pickering emulsion with rapid CO_(2)/N_(2) respon-siveness,which is stabilized using alumina nanoparticles hydrophobized in situ with a trace amount of a swit...This article reports the development of a novel switchable Pickering emulsion with rapid CO_(2)/N_(2) respon-siveness,which is stabilized using alumina nanoparticles hydrophobized in situ with a trace amount of a switchable superamphiphile via electrostatic interactions.With the introduction of CO_(2) for 30 s,the Pickering emulsion can be spontaneously demulsified with complete phase separation;the emulsion can then be reconstructed in response to N_(2) purging for 10 min followed by homogenization.Moreover,the stable Pickering emulsion can be stored for more than 60 days at room temperature with-out any visible change.The CO_(2)/N_(2)-responsive behavior of the switchable Pickering emulsion is attribu-ted to the reversible desorption/adsorption of the switchable surfactants on the surfaces of the alumina nanoparticles upon the alternative bubbling of CO_(2)or N_(2).Thanks to the simple fabrication of the surfac-tant and the hydrophobization of the alumina nanoparticles,this research has developed an extremely facile and cost-efficient method for preparing a rapidly CO_(2)/N_(2)-responsive switchable Pickering emul-sion.The dosage of the switchable surfactants has been significantly reduced by nearly 1500 times(from 150 to 0.1 mmol·L^(-1))as compared with the dosage used in previous studies.Moreover,the as-prepared CO_(2)/N_(2)-responsive switchable Pickering emulsion is environmentally friendly,mild,and nontoxic;thus,it holds great potential for practical applications with considerable economic and environmental benefits,such as oil transport,fossil fuel production,environmental gases detection,and the encapsulation and release of active ingredients.展开更多
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。
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.
基金supported by the National Natural Science Foundation of China(32171734)the Scientific Research Funds of Huaqiao University(20BS201).
文摘Environment friendly and intelligent surfactants have attracted great attention in recent years.A bio-based CO_(2)responsive surfactant rosin acid dimaleimide choline(R-BMI-C)with an extremely rigid skeleton was prepared using rosin and choline as raw materials by Diels-Alder addition reaction and acid-base neutralization reactions.Its structure was confirmed by IR and^(1)H NMR spectra.The foams’properties of R-BMI-C could be adjusted by bubbling CO_(2)/N_(2)to change the structure of the surfactant.At pH 10.4,R-BMI-C forms an unstable foam with a half-life of 1.5 h.When the pH was reduced to 7.4 by bubbling CO_(2),R-BMI-C forms an extremely stable foam with a half-life of 336 h.The surfactant R-BMI-C changed from bola type to conventional type when bubbling CO_(2).And the internal aggregation structure of R-BMI-C aqueous solution changed from spherical micelles to laminar micelles according to the cryogenic-transmission electron microscope.We know that the lamellar structure tends to adsorb at the air/water interface or is trapped in the foam film,which slows down the foam coarsening and agglomeration process,resulting in a significant increase in foam stability.R-BMI-C could be used in oil extraction,fire-fighting and chemical decontamination due to its excellent foaming,stabilization and defoaming properties.
基金supported by the China National Petroleum Corporation (RIPED-2017-JS-87)
文摘In this study, we developed a strategy for using the Scoggins procedure in the synthesis of acetamidines as novel C02-triggered switchable surfactants via acetimidates by effectively tuning the chemical equilibrium. The as-synthesized N'-alkyl-N,Ndiethylacetamidines exhibit excellent CO_2/N_2 switchability and their bicarbonate salts have the ability to emulsify oil-water mixtures.
基金supported by the Natural Sciences and Engineering Research Council of Canada (NSERC)the Canada Research Chairs Program (Hongbo Zeng)the China Scholarship Council (CSC) (An Chen)
文摘This article reports the development of a novel switchable Pickering emulsion with rapid CO_(2)/N_(2) respon-siveness,which is stabilized using alumina nanoparticles hydrophobized in situ with a trace amount of a switchable superamphiphile via electrostatic interactions.With the introduction of CO_(2) for 30 s,the Pickering emulsion can be spontaneously demulsified with complete phase separation;the emulsion can then be reconstructed in response to N_(2) purging for 10 min followed by homogenization.Moreover,the stable Pickering emulsion can be stored for more than 60 days at room temperature with-out any visible change.The CO_(2)/N_(2)-responsive behavior of the switchable Pickering emulsion is attribu-ted to the reversible desorption/adsorption of the switchable surfactants on the surfaces of the alumina nanoparticles upon the alternative bubbling of CO_(2)or N_(2).Thanks to the simple fabrication of the surfac-tant and the hydrophobization of the alumina nanoparticles,this research has developed an extremely facile and cost-efficient method for preparing a rapidly CO_(2)/N_(2)-responsive switchable Pickering emul-sion.The dosage of the switchable surfactants has been significantly reduced by nearly 1500 times(from 150 to 0.1 mmol·L^(-1))as compared with the dosage used in previous studies.Moreover,the as-prepared CO_(2)/N_(2)-responsive switchable Pickering emulsion is environmentally friendly,mild,and nontoxic;thus,it holds great potential for practical applications with considerable economic and environmental benefits,such as oil transport,fossil fuel production,environmental gases detection,and the encapsulation and release of active ingredients.
