Magnetic resonance imaging (MRI) was used to probe the structure and flow velocity within the interparticle space of a packed bed of agar beads under water-saturated condition. The images of the velocity field at th...Magnetic resonance imaging (MRI) was used to probe the structure and flow velocity within the interparticle space of a packed bed of agar beads under water-saturated condition. The images of the velocity field at three different flow rates were obtained. To determine the pore-parameter of the porous media, the internal structure of the bed was also obtained using image processing technique. The results show that the porosity of the sample is 31.28% and the fitting curve for the distribution of pore equivalent diameter follows Gaussian distribution. The velocity profiles do shift as the flow rate varies and the solution flow through the void space is not a homogeneous flow in any pores. The velocity distributions within the pore are roughly parabolic with the local maximum being near the center. About half of the velocity components are in the class of 0-1 cm/s. The frequency of lower velocity components is lower at higher flow rate, but to higher velocity components, it is just the opposite.展开更多
To obtain the influence laws of the fine gangue rate on the properties of coal gangue cementitious paste, the slump, divergence, stratification, bleeding, setting time and mechanical strength with the change of fine g...To obtain the influence laws of the fine gangue rate on the properties of coal gangue cementitious paste, the slump, divergence, stratification, bleeding, setting time and mechanical strength with the change of fine gangue rate were studied on the basis of keeping the amount of cementing material and slurry concentration unchanged. The porosity and the distribution of pore diameter of the filling specimen for curing 28 d were tested by a mercury injection instrument under different fine gangue rate conditions. It was shown that the slump, divergence, setting time and compressive strength of the paste firstly increased and then decreased with increasing fine gangue rate. The stratification and bleeding rate decreased with increasing fine gangue rate. The smaller the critical pore size of the paste was, the smaller the porosity was, the smaller the average pore size was. When the fine gangue rate was 40%, the maximum critical pore diameter of the paste was 55.79 μm, and the corresponding porosity was 17.54%, and the properties of filling paste were the best. When the fine gangue rate further increased, the aggregate surface area increased, and the reaction product of cementitious materials could not effectively fill the pores. It weakened the agglomeration effect. The particles surface of coal gangue was fragmental and flake deposit with irregular shape and uneven fold morphology. It was easy to be bonded with the surface of other filling material. The hydration products of coal gangue cementitious material were a large number of C-S-H gel with fibrous shape and ettringite(AFt) with compact block structure. The theoretical reference was provided for the preparation of low cost gangue cemented filling materials in coal mines.展开更多
Coal seam CO_(2) sequestration is an important option to address global warming.A better knowledge on coal pore structure evolution during gas adsorption can provide guidance for coal seams CO_(2) seques-tration.Howev...Coal seam CO_(2) sequestration is an important option to address global warming.A better knowledge on coal pore structure evolution during gas adsorption can provide guidance for coal seams CO_(2) seques-tration.However,few investigations on the pore structure evolution differences between the deep and shallow coal were conducted during gas adsorption.In this study,based on the real-time synchrotron radiation small-angle X-ray scattering(SAXS)observation,the average pore diameter and pore surface fractal dimension evolution differences between deep and shallow coal were investigated from the as-pects of coal compositions and stress history.Two types of coal deformation(inner-swelling and outer-swelling)coexist during gas adsorption.Coal compositions have significant impact on the dominance of deformation type.The dominance of inner-swelling in deep coal is induced by the higher ash contents,and there is the decrease of average pore diameter during gas adsorption.The impact of stress-history(burial depth)on adsorption-induced deformation is more prominent than that of gas adsorption ca-pacity.In deep coal,the surface fractal dimension evolution presents a negative correlation with the evolution of pore diameters.In shallow coal,the surface fractal dimension evolution presents a Langmuir-type correlation with the adsorption time.展开更多
Heteroatom-doped carbon materials have demonstrated great potential in the electrochemical reduction reaction of CO_(2)(CO_(2)RR)due to their versatile structure and function.However,rational structure control remains...Heteroatom-doped carbon materials have demonstrated great potential in the electrochemical reduction reaction of CO_(2)(CO_(2)RR)due to their versatile structure and function.However,rational structure control remains one challenge.In this work,we reported a unique carbon precursor of soft template-containing porous poly(ionic liquid)(PIL)that was directly synthesized via free-radical self-polymerization of ionic liquid monomer in a soft template route.Variation of the carbonization temperature in a direct pyrolysis process without any additive yielded a series of carbon materials with facile adjustable textural properties and N species.Significantly,the integration of soft-template in the PIL precursor led to the formation of hierarchical porous carbon material with a higher surface area and larger pore size than that from the template-free precursor.In CO_(2)RR to CO,the champion catalyst gave a Faraday efficiency of 83.0%and a current density of 1.79 mA·cm^(-2)at-0.9 V vs.reversible hydrogen electrode(vs.RHE).The abundant graphite N species and hierarchical pore structure,especially the unique hierarchical small-/ultramicropores were revealed to enable better CO_(2)RR performance.展开更多
In order to study the influence of highland barley straw ash (HBSA) prepared under certain conditions on the durability of magnesium oxychloride cement mortar (MOCM) under freeze-thaw damage,rapid freeze-thaw cycle te...In order to study the influence of highland barley straw ash (HBSA) prepared under certain conditions on the durability of magnesium oxychloride cement mortar (MOCM) under freeze-thaw damage,rapid freeze-thaw cycle tests were carried out firstly.The relative mass evaluation parameters and the relative compressive strength evaluation parameters,which represent the degradation of freeze-thaw resistance,were used as the indices to study the degradation rule of MOCM.Secondly,nuclear magnetic resonance (NMR) tests were carried out on MOCM under different freeze-thaw cycles to analyze the pore diameter changes in the freeze-thaw process.The microstructure of MOCM was tested by Fourier transform infrared spectroscopy (FTIR),X-ray diffraction (XRD) and scanning electron microscopy (SEM),and then the effect mechanism of HBSA on the anti-freezing performance of MOCM was revealed.Finally,the two-parameter Weibull distribution function was used to analyze the reliability of durability degradation of MOCM added with HBSA under freeze-thaw cycles.The specific conclusions are as follows:With the increase of HBSA's addition,the freeze-thaw resistance of MOCM increase firstly and then decrease.When the addition of HBSA is 10%,the decay rate of relative mass evaluation parameters and relative compressive strength evaluation parameters is the slowest,and the frost resistance is the best.The proportion of harmful pores and more harmful pores in MOCM added with 10% HBSA decreases by 25.11% and 21.34%,compared with that without HBSA before and after freeze-thaw cycles.A lot of magnesium silicate hydrate (M-S-H) gels are generated in MOCM with HBSA content of 10%,which fills part of the pores,so that the proportion of harmful pores and more harmful pores is the lowest.The Weibull function can be effectively applied to the reliability analysis of the freeze-thaw cycle of MOCM added with HBSA,and the theoretical results are in good agreement with the experimental results.展开更多
tert-Butylation of toluene with tert-butanol used as the alkylating agent was investigated over the activated bentonite and HY zeolite used as the catalyst.The influences of various butylation reaction parameters,incl...tert-Butylation of toluene with tert-butanol used as the alkylating agent was investigated over the activated bentonite and HY zeolite used as the catalyst.The influences of various butylation reaction parameters,including the toluene/tert-butanol ratio,the reaction temperature,and the space velocity were discussed.The optimal results were obtained at a reaction temperature of 180 ℃,a space velocity of 4 h-1,and a mole ratio of toluene to tert-butanol equating to 2.The structure and acidic properties of catalyst were characterized by the BET method and the Fourier transform infrared (FTIR) spectroscopy.Compared with the HY zeolite,the activated bentonite possessed high activity for toluene conversion and high para-selectivity because it had larger pore diameter,smaller micropore surface area and higher ratio of total Lewis acids to total Br nsted acids.展开更多
Wormholelike mesoporous carbons (WMCs) with three different pore diameters (D-P), namely WMC-F7 (D-p = 8.5 nm), WMC-F30 (D-p =4.4 nm), and WMC-F0 (D-p =3.1 nm) are prepared via a modified sol-gel process. Then PtRu na...Wormholelike mesoporous carbons (WMCs) with three different pore diameters (D-P), namely WMC-F7 (D-p = 8.5 nm), WMC-F30 (D-p =4.4 nm), and WMC-F0 (D-p =3.1 nm) are prepared via a modified sol-gel process. Then PtRu nanoparticles with the particle size (40 of 3.2 nm supported on WMCs are synthesized with a modified pulse microwave-assisted polyol method. It is found that the pore diameter of WMCs plays an important role in the electrochemical activity of PtRu toward alcohol electrooxidation reaction. PtRu/WMC-F7 with D-p > 2d(pt) exhibits the largest electrochemical surface area (ESA) and the highest activity toward methanol electrooxidation. With the decrease in Dp, PtRu/WMC-F30 and PtRu/WMC-F0 have much lower ESA and electrochemical activity, especially for the isopropanol electrooxidation with a larger molecular size. When D-p is more than twice d(pt), the mass transfer of reactants and electrolyte are easier, and thus more PtRu nanoparticles can be utilized and the catalysts activity can be enhanced. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.展开更多
In this work,the effect of the textural property of activated carbons on desorption activation energy and adsorption capacity for benzothiophene(BT)was investigated.BET surface areas and the textural parameters of thr...In this work,the effect of the textural property of activated carbons on desorption activation energy and adsorption capacity for benzothiophene(BT)was investigated.BET surface areas and the textural parameters of three kinds of the activated carbons,namely SY-6,SY-13 and SY-19,were measured with an ASAP 2010 instrument.The desorption activation energies of BT on the activated carbons were determined by temperature-programmed desorption(TPD).Static adsorption experiments were carried out to determine the isotherms of BT on the activated carbons.The influence of the textural property of the activated carbons on desorption activation energy and the adsorption capacity for BT was discussed.Results showed that the BET surface areas of the activated carbons,SY-6,SY-13 and SY-19 were 1106,1070 and 689 m2·g^(-1),respectively,and their average pore diameters were 1.96,2.58 and 2.16 nm,respectively.The TPD results indicated that the desorption activation energy of BT on the activated carbons,SY-6,SY-19 and SY-13 were 58.84,53.02 and 42.57 KJ/mol,respectively.The isotherms showed that the amount of BT adsorbed on the activated carbons followed the order of SY-6>SY-19>SY-13.The smaller the average pore diameter of the activated carbon,the stronger its adsorption for BT and the higher the activation energy required for BT desorption on its surface.The Freundlich adsorption isotherm model can be properly used to formulate the adsorption behavior of BT on the activated carbons.展开更多
基金Project(51374035)supported by the National Natural Science Foundation of ChinaProject(2012BAB08B02)supported by the National Science&Technology Pillar Program During the Twelfth Five-year Plan PeriodProject(NCET-13-0669)supported by the New Century Excellent Talents in University of Ministry of Education of China
文摘Magnetic resonance imaging (MRI) was used to probe the structure and flow velocity within the interparticle space of a packed bed of agar beads under water-saturated condition. The images of the velocity field at three different flow rates were obtained. To determine the pore-parameter of the porous media, the internal structure of the bed was also obtained using image processing technique. The results show that the porosity of the sample is 31.28% and the fitting curve for the distribution of pore equivalent diameter follows Gaussian distribution. The velocity profiles do shift as the flow rate varies and the solution flow through the void space is not a homogeneous flow in any pores. The velocity distributions within the pore are roughly parabolic with the local maximum being near the center. About half of the velocity components are in the class of 0-1 cm/s. The frequency of lower velocity components is lower at higher flow rate, but to higher velocity components, it is just the opposite.
基金Funded by the National Science Foundation of China(No.51574055)the Key State Laboratory of Coastal and Offshore Engineering(No.LP1720)
文摘To obtain the influence laws of the fine gangue rate on the properties of coal gangue cementitious paste, the slump, divergence, stratification, bleeding, setting time and mechanical strength with the change of fine gangue rate were studied on the basis of keeping the amount of cementing material and slurry concentration unchanged. The porosity and the distribution of pore diameter of the filling specimen for curing 28 d were tested by a mercury injection instrument under different fine gangue rate conditions. It was shown that the slump, divergence, setting time and compressive strength of the paste firstly increased and then decreased with increasing fine gangue rate. The stratification and bleeding rate decreased with increasing fine gangue rate. The smaller the critical pore size of the paste was, the smaller the porosity was, the smaller the average pore size was. When the fine gangue rate was 40%, the maximum critical pore diameter of the paste was 55.79 μm, and the corresponding porosity was 17.54%, and the properties of filling paste were the best. When the fine gangue rate further increased, the aggregate surface area increased, and the reaction product of cementitious materials could not effectively fill the pores. It weakened the agglomeration effect. The particles surface of coal gangue was fragmental and flake deposit with irregular shape and uneven fold morphology. It was easy to be bonded with the surface of other filling material. The hydration products of coal gangue cementitious material were a large number of C-S-H gel with fibrous shape and ettringite(AFt) with compact block structure. The theoretical reference was provided for the preparation of low cost gangue cemented filling materials in coal mines.
基金supported by the National Natural Science Foundation of China (grant Nos.U1910206,52004293,52225402)Beijing Natural Science Foundation (grant No.8232057)+4 种基金the Open Project Program of State Key Laboratory of Coal and CBM Co-mining (grant No.2022KF21)Fundamental Research Funds for the Central Universities (grant No.FRF-TP-20-034A1)the Open Project Program of Key Laboratory of Deep Earth Science and Engineering (Sichuan University)Ministry of Education (grant No.DESE 202004)China Postdoctoral Science Foundation (grant No.2018M641526).
文摘Coal seam CO_(2) sequestration is an important option to address global warming.A better knowledge on coal pore structure evolution during gas adsorption can provide guidance for coal seams CO_(2) seques-tration.However,few investigations on the pore structure evolution differences between the deep and shallow coal were conducted during gas adsorption.In this study,based on the real-time synchrotron radiation small-angle X-ray scattering(SAXS)observation,the average pore diameter and pore surface fractal dimension evolution differences between deep and shallow coal were investigated from the as-pects of coal compositions and stress history.Two types of coal deformation(inner-swelling and outer-swelling)coexist during gas adsorption.Coal compositions have significant impact on the dominance of deformation type.The dominance of inner-swelling in deep coal is induced by the higher ash contents,and there is the decrease of average pore diameter during gas adsorption.The impact of stress-history(burial depth)on adsorption-induced deformation is more prominent than that of gas adsorption ca-pacity.In deep coal,the surface fractal dimension evolution presents a negative correlation with the evolution of pore diameters.In shallow coal,the surface fractal dimension evolution presents a Langmuir-type correlation with the adsorption time.
基金support from the National Natural Science Foundation of China(Nos.22072065,U1662107,and 21476109)Six talent peaks project in Jiangsu Province(JNHB035)+3 种基金State Key Laboratory of Materials-Oriented Chemical Engineering(KL17-04)Jiangsu Provincial Science Foundation for Youths(SBK2020044703)the Project of Priority Academic Program Development of Jiangsu Higher Education Institutions(PAPD)High-Performance Computing Center of Nanjing Tech University。
文摘Heteroatom-doped carbon materials have demonstrated great potential in the electrochemical reduction reaction of CO_(2)(CO_(2)RR)due to their versatile structure and function.However,rational structure control remains one challenge.In this work,we reported a unique carbon precursor of soft template-containing porous poly(ionic liquid)(PIL)that was directly synthesized via free-radical self-polymerization of ionic liquid monomer in a soft template route.Variation of the carbonization temperature in a direct pyrolysis process without any additive yielded a series of carbon materials with facile adjustable textural properties and N species.Significantly,the integration of soft-template in the PIL precursor led to the formation of hierarchical porous carbon material with a higher surface area and larger pore size than that from the template-free precursor.In CO_(2)RR to CO,the champion catalyst gave a Faraday efficiency of 83.0%and a current density of 1.79 mA·cm^(-2)at-0.9 V vs.reversible hydrogen electrode(vs.RHE).The abundant graphite N species and hierarchical pore structure,especially the unique hierarchical small-/ultramicropores were revealed to enable better CO_(2)RR performance.
基金Funded by the National Natural Science Foundation of China (No.51868044)Basic Research Program of Qinghai Province (No.2022-ZJ-921)。
文摘In order to study the influence of highland barley straw ash (HBSA) prepared under certain conditions on the durability of magnesium oxychloride cement mortar (MOCM) under freeze-thaw damage,rapid freeze-thaw cycle tests were carried out firstly.The relative mass evaluation parameters and the relative compressive strength evaluation parameters,which represent the degradation of freeze-thaw resistance,were used as the indices to study the degradation rule of MOCM.Secondly,nuclear magnetic resonance (NMR) tests were carried out on MOCM under different freeze-thaw cycles to analyze the pore diameter changes in the freeze-thaw process.The microstructure of MOCM was tested by Fourier transform infrared spectroscopy (FTIR),X-ray diffraction (XRD) and scanning electron microscopy (SEM),and then the effect mechanism of HBSA on the anti-freezing performance of MOCM was revealed.Finally,the two-parameter Weibull distribution function was used to analyze the reliability of durability degradation of MOCM added with HBSA under freeze-thaw cycles.The specific conclusions are as follows:With the increase of HBSA's addition,the freeze-thaw resistance of MOCM increase firstly and then decrease.When the addition of HBSA is 10%,the decay rate of relative mass evaluation parameters and relative compressive strength evaluation parameters is the slowest,and the frost resistance is the best.The proportion of harmful pores and more harmful pores in MOCM added with 10% HBSA decreases by 25.11% and 21.34%,compared with that without HBSA before and after freeze-thaw cycles.A lot of magnesium silicate hydrate (M-S-H) gels are generated in MOCM with HBSA content of 10%,which fills part of the pores,so that the proportion of harmful pores and more harmful pores is the lowest.The Weibull function can be effectively applied to the reliability analysis of the freeze-thaw cycle of MOCM added with HBSA,and the theoretical results are in good agreement with the experimental results.
文摘tert-Butylation of toluene with tert-butanol used as the alkylating agent was investigated over the activated bentonite and HY zeolite used as the catalyst.The influences of various butylation reaction parameters,including the toluene/tert-butanol ratio,the reaction temperature,and the space velocity were discussed.The optimal results were obtained at a reaction temperature of 180 ℃,a space velocity of 4 h-1,and a mole ratio of toluene to tert-butanol equating to 2.The structure and acidic properties of catalyst were characterized by the BET method and the Fourier transform infrared (FTIR) spectroscopy.Compared with the HY zeolite,the activated bentonite possessed high activity for toluene conversion and high para-selectivity because it had larger pore diameter,smaller micropore surface area and higher ratio of total Lewis acids to total Br nsted acids.
基金supported by the National Natural Science Foundation of China (no. 91434106)
文摘Wormholelike mesoporous carbons (WMCs) with three different pore diameters (D-P), namely WMC-F7 (D-p = 8.5 nm), WMC-F30 (D-p =4.4 nm), and WMC-F0 (D-p =3.1 nm) are prepared via a modified sol-gel process. Then PtRu nanoparticles with the particle size (40 of 3.2 nm supported on WMCs are synthesized with a modified pulse microwave-assisted polyol method. It is found that the pore diameter of WMCs plays an important role in the electrochemical activity of PtRu toward alcohol electrooxidation reaction. PtRu/WMC-F7 with D-p > 2d(pt) exhibits the largest electrochemical surface area (ESA) and the highest activity toward methanol electrooxidation. With the decrease in Dp, PtRu/WMC-F30 and PtRu/WMC-F0 have much lower ESA and electrochemical activity, especially for the isopropanol electrooxidation with a larger molecular size. When D-p is more than twice d(pt), the mass transfer of reactants and electrolyte are easier, and thus more PtRu nanoparticles can be utilized and the catalysts activity can be enhanced. (C) 2016 Science Press and Dalian Institute of Chemical Physics, Chinese Academy of Sciences. Published by Elsevier B.V. and Science Press. All rights reserved.
基金the National Natural Science Foundation of China(Grant No.20336020)for financial support.
文摘In this work,the effect of the textural property of activated carbons on desorption activation energy and adsorption capacity for benzothiophene(BT)was investigated.BET surface areas and the textural parameters of three kinds of the activated carbons,namely SY-6,SY-13 and SY-19,were measured with an ASAP 2010 instrument.The desorption activation energies of BT on the activated carbons were determined by temperature-programmed desorption(TPD).Static adsorption experiments were carried out to determine the isotherms of BT on the activated carbons.The influence of the textural property of the activated carbons on desorption activation energy and the adsorption capacity for BT was discussed.Results showed that the BET surface areas of the activated carbons,SY-6,SY-13 and SY-19 were 1106,1070 and 689 m2·g^(-1),respectively,and their average pore diameters were 1.96,2.58 and 2.16 nm,respectively.The TPD results indicated that the desorption activation energy of BT on the activated carbons,SY-6,SY-19 and SY-13 were 58.84,53.02 and 42.57 KJ/mol,respectively.The isotherms showed that the amount of BT adsorbed on the activated carbons followed the order of SY-6>SY-19>SY-13.The smaller the average pore diameter of the activated carbon,the stronger its adsorption for BT and the higher the activation energy required for BT desorption on its surface.The Freundlich adsorption isotherm model can be properly used to formulate the adsorption behavior of BT on the activated carbons.