Xenon/krypton(Xe/Kr)separation is an important task in industry,yet it remains challenging to develop adsorbents with high Xe/Kr selectivity and adsorption capacity of Xe,especially at low partial pressures.Herein,we ...Xenon/krypton(Xe/Kr)separation is an important task in industry,yet it remains challenging to develop adsorbents with high Xe/Kr selectivity and adsorption capacity of Xe,especially at low partial pressures.Herein,we report a series of microporous carbon molecular sieves(CMSs)for Xe/Kr separation.Those materials have ideal bimodal pore size distributions that not only provide substantial space for the accommodation of gas molecules,but also allow selective diffusion of gas molecules.Additionally,the carbon frameworks decorated with polar oxygen-containing functional groups afford higher affinity for Xe than Kr,which is proven by density functional theory(DFT)calculations and charge density difference analysis.The optimal CPVDC-700 exhibits a high selectivity of Xe/Kr and,more importantly,a record-high uptake of Xe(2.93 mmol g^(-1))at 0.2 bar and298 K,which is the highest among all the reported carbon adsorbents.Breakthrough experiments confirm the excellent performance of such CMSs for Xe/Kr separation,and the dynamic adsorption uptake of Xe and productivity of high-purity Kr are calculated to be 2.91 mmol g^(-1)and 208 m L g^(-1)(9.29 mmol g^(-1)),respectively,which also set up a new benchmark for Xe/Kr separation of carbon adsorbents.展开更多
In this paper,we present a new method for preparing γ-alumina nanoparticles with a bimodal pore size distribution by using an efficiently mixing membrane dispersion microreactor.NH4HCO3and AI2(SO4)3.18H2Owere reacted...In this paper,we present a new method for preparing γ-alumina nanoparticles with a bimodal pore size distribution by using an efficiently mixing membrane dispersion microreactor.NH4HCO3and AI2(SO4)3.18H2Owere reacted under vigorous mixing to give an ammonium aluminum carbonate hydroxide (AACH)precursor.γ-Alumina was obtained by calcination of AACH at 550℃ for 6h.The effects of NH4HCO3concentration,pH during aging,and reaction temperature were investigated.The mechanism of bimodal pore formation was clarified.The results showed that large pores (10-100nm) were mainly formed in the reactor and during aging,and small pores (0-10nm)were mainly formed during calcination.When the concentration of NH4HCO3was 1.5mol/L,the aging pH was 9.2,and the reaction temperature was 80℃,γ-alumina with a specific surface area of 504.7m^2/g and pore volume of 1.76mL/g was obtained.The average size of the large pores was about 30nm,and the average size of the small pores was about 4nm.展开更多
A series of macroporous silicates with zeolitic microporous frameworks have been successfully prepared by self assembly of discrete colloidal crystals of silicalite 1, titanium silicalite 1(TS 1) and ZSM 5 , using pol...A series of macroporous silicates with zeolitic microporous frameworks have been successfully prepared by self assembly of discrete colloidal crystals of silicalite 1, titanium silicalite 1(TS 1) and ZSM 5 , using polystyrene(PS) spheres as templates. The properties of these novel materials were characterized by means of XRD, IR, SEM, 29 Si MAS NMR and N 2 adsorption/desorption measurements. These materials show ordered spheroidal voids, which are interconnected in three dimensions through windows. The ordering of the macropores are mainly affected by the particle size of the colloidal zeolites. [WT5HZ]展开更多
为研究双峰孔隙结构对非饱和土力学特性的影响,以广西南宁和桂林2种典型双峰孔隙结构黏土为研究对象,分析了其在不同饱和度情况下的抗剪强度特性;辅以滤纸法及核磁共振(nuclear magnetic resonance,NMR)技术探究了2种土体在双峰孔隙结...为研究双峰孔隙结构对非饱和土力学特性的影响,以广西南宁和桂林2种典型双峰孔隙结构黏土为研究对象,分析了其在不同饱和度情况下的抗剪强度特性;辅以滤纸法及核磁共振(nuclear magnetic resonance,NMR)技术探究了2种土体在双峰孔隙结构情况下孔隙水分布状态对强度的影响机理。结果表明:饱和状态下,2种土体试样的T2分布曲线为双峰结构,且土样持水特性整体上均呈现双峰土水特征曲线;2种土体的应力-位移关系变化规律相似,抗剪强度与饱和度密切相关;在饱和度为40%前后土样黏聚力变化趋势发生改变,而内摩擦角则是在饱和度为80%时达到最小值。展开更多
Carbon materials have shown remarkable usefulness in facilitating the performance of insulating sulfur cathode for lithium–sulfur batteries owing to their excellent conductivity and porous structure. However,the anxi...Carbon materials have shown remarkable usefulness in facilitating the performance of insulating sulfur cathode for lithium–sulfur batteries owing to their excellent conductivity and porous structure. However,the anxiety is the poor affinity toward polar polysulfides due to the intrinsic nonpolar surface of carbon.Herein, we report a direct pyrolysis of the mixture urea and boric acid to synthesize B/N–codoped hierarchically porous carbon nanosheets(B–N–CSs) as efficient sulfur host for lithium–sulfur battery. The graphene–like B–N–CSs provides high specific surface area and porous structure with abundant micropores(1.1 nm) and low–range mesopores(2.3 nm), thereby constraining the sulfur active materials within the pores. More importantly, the codoped B/N elements can further enhance the polysulfide confinement through strong Li–N and B–S interaction based on the Lewis acid–base theory. These structural superiorities significantly suppress the shuttle effect by both physical confinement and chemical interaction, and promote the redox kinetics of polysulfide conversion. When evaluated as the cathode host, the S/B–N–CSs composite displays the excellent performance with a high reversible capacity up to 772 m A h g–1 at 0.5 C and a low fading rate of ^0.09% per cycle averaged upon 500 cycles. In particular, remarkable stability with a high capacity retention of 87.1% can be realized when augmenting the sulfur loading in the cathode up to 4.6 mg cm^(-2).展开更多
The catalytic property of AICl(3) catalyst immobilized on gamma -Al2O3 for isobutene polymerization has been studied. It was found that the activity, selectivity and stability of the catalyst are dependent greatly on ...The catalytic property of AICl(3) catalyst immobilized on gamma -Al2O3 for isobutene polymerization has been studied. It was found that the activity, selectivity and stability of the catalyst are dependent greatly on geometric characteristic pf the pore structure and size of catalyst. Although the activity and selectivity of the catalysts with micro- and meso-pore structure are all high in initial stage, but their stability is low, while those with bimodal meso- and macro-pore structure are excellent. Increasing granularity of the catalyst(particle become fine) brings about an increase in isobutene conversion, but a decrease in selectivity, resulting in lower average molecular weight and iis broader distribution.展开更多
Mesoporous silica with controllable bimodal pore size distribution was synthesized with cetyltrimethylammonium bromide （CTAB） as chemical template for small mesopores and silica gel as physical template for large me...Mesoporous silica with controllable bimodal pore size distribution was synthesized with cetyltrimethylammonium bromide （CTAB） as chemical template for small mesopores and silica gel as physical template for large mesopores. The structure of synthesized samples were characterized by Fourier transform infrared （FT-IR） spectroscopy, X-ray diffraction （XRD）, scanning electron microscopy （SEM）, transmission electron microscopy （TEM） and N2 adsorption-desorption measurements. The experimental results show that bimodal mesoporous silica consists of small mesopores of about 3 nm and large mesopores of about 45 nm. The small mesopores which were formed on the external surface and pore walls of the silica gel had similar characters with those of MCM-41, while large mesopores were inherited from parent silica gel material. The pore size distribution of the synthesized silica can be adjusted by changing the relative content of TEOS and silica gel or the feeding sequence of silica gel and NH4OH.展开更多
The synthesis of silica with bimodal, disordered mesopores structure, by template-mediated sol-gel processing and subsequent heat-treatment process, was investigated. In the presence of nonionic surfactant Tx-15, the ...The synthesis of silica with bimodal, disordered mesopores structure, by template-mediated sol-gel processing and subsequent heat-treatment process, was investigated. In the presence of nonionic surfactant Tx-15, the organically modified mesostructured nano-particles were synthesized by co-condensation of organosiloxane （RTES） and tetraethoxysilane （TEOS） in the first step, and then the bimodal porous silica was formed by the removal of the incorporated organic groups using programmed calcination. Here, RTES used was methyltriethoxysilane （MTES）, vinyltriethoxysilane （VTES） and phenyltriethoxysilane （PhTES）, respectively. Organotrialkoxysilane, TEOS and Tx-15 formed MSU-2-1iked assemblies, around which the nano-particles aggregated and cross-linked, considerably influencing the pore size distribution of both primary pores and secondary pores. By changing the type and amount of the organotrialkoxysilane added, a broad variety of silica with a controlled bimodal mesopore distribution could be easily synthesized. Textural and structural properties were determined by X-ray diffraction, high-resolution transmission electron microscopy, N2 adsorption/desorption, and thermogravimetric analysis.展开更多
基金supported by the National Natural Science Foundation of China(21878260,21978254,22141001)the Ministry of Education-Singapore(MOE2018-T2-2-148,MOE2019-T2-1-093)+4 种基金the Energy Market Authority of Singapore(EMA-EP009-SEGC-020)the Agency for ScienceTechnology and Research(U2102d2004,U2102d2012)the National Research Foundation(NRF-CRP26-2021RS-0002)the China Scholarship Council(CSC,202106310172)for a fellowship to support his study at National University of Singapore。
文摘Xenon/krypton(Xe/Kr)separation is an important task in industry,yet it remains challenging to develop adsorbents with high Xe/Kr selectivity and adsorption capacity of Xe,especially at low partial pressures.Herein,we report a series of microporous carbon molecular sieves(CMSs)for Xe/Kr separation.Those materials have ideal bimodal pore size distributions that not only provide substantial space for the accommodation of gas molecules,but also allow selective diffusion of gas molecules.Additionally,the carbon frameworks decorated with polar oxygen-containing functional groups afford higher affinity for Xe than Kr,which is proven by density functional theory(DFT)calculations and charge density difference analysis.The optimal CPVDC-700 exhibits a high selectivity of Xe/Kr and,more importantly,a record-high uptake of Xe(2.93 mmol g^(-1))at 0.2 bar and298 K,which is the highest among all the reported carbon adsorbents.Breakthrough experiments confirm the excellent performance of such CMSs for Xe/Kr separation,and the dynamic adsorption uptake of Xe and productivity of high-purity Kr are calculated to be 2.91 mmol g^(-1)and 208 m L g^(-1)(9.29 mmol g^(-1)),respectively,which also set up a new benchmark for Xe/Kr separation of carbon adsorbents.
基金This work was financially supported by the National Basic Research Foundation of China (grant number 2013CB733600)and the National Natural Science Foundation (grant numbers 21276140,20976096,and 21036002).
文摘In this paper,we present a new method for preparing γ-alumina nanoparticles with a bimodal pore size distribution by using an efficiently mixing membrane dispersion microreactor.NH4HCO3and AI2(SO4)3.18H2Owere reacted under vigorous mixing to give an ammonium aluminum carbonate hydroxide (AACH)precursor.γ-Alumina was obtained by calcination of AACH at 550℃ for 6h.The effects of NH4HCO3concentration,pH during aging,and reaction temperature were investigated.The mechanism of bimodal pore formation was clarified.The results showed that large pores (10-100nm) were mainly formed in the reactor and during aging,and small pores (0-10nm)were mainly formed during calcination.When the concentration of NH4HCO3was 1.5mol/L,the aging pH was 9.2,and the reaction temperature was 80℃,γ-alumina with a specific surface area of 504.7m^2/g and pore volume of 1.76mL/g was obtained.The average size of the large pores was about 30nm,and the average size of the small pores was about 4nm.
文摘A series of macroporous silicates with zeolitic microporous frameworks have been successfully prepared by self assembly of discrete colloidal crystals of silicalite 1, titanium silicalite 1(TS 1) and ZSM 5 , using polystyrene(PS) spheres as templates. The properties of these novel materials were characterized by means of XRD, IR, SEM, 29 Si MAS NMR and N 2 adsorption/desorption measurements. These materials show ordered spheroidal voids, which are interconnected in three dimensions through windows. The ordering of the macropores are mainly affected by the particle size of the colloidal zeolites. [WT5HZ]
基金supported by the National Natural Science Foundation of China(21337003,21477149)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDB05050200)~~
文摘为研究双峰孔隙结构对非饱和土力学特性的影响,以广西南宁和桂林2种典型双峰孔隙结构黏土为研究对象,分析了其在不同饱和度情况下的抗剪强度特性;辅以滤纸法及核磁共振(nuclear magnetic resonance,NMR)技术探究了2种土体在双峰孔隙结构情况下孔隙水分布状态对强度的影响机理。结果表明:饱和状态下,2种土体试样的T2分布曲线为双峰结构,且土样持水特性整体上均呈现双峰土水特征曲线;2种土体的应力-位移关系变化规律相似,抗剪强度与饱和度密切相关;在饱和度为40%前后土样黏聚力变化趋势发生改变,而内摩擦角则是在饱和度为80%时达到最小值。
基金financial support of the National Natural Science Foundation of China (Grant No. 21263016, 21363015, 51662029, 21863006)the Youth Science Foundation of Jiangxi Province (Grant No. 20192BAB216001)the Key Laboratory of Jiangxi Province for Environment and Energy Catalysis (20181BCD40004)。
文摘Carbon materials have shown remarkable usefulness in facilitating the performance of insulating sulfur cathode for lithium–sulfur batteries owing to their excellent conductivity and porous structure. However,the anxiety is the poor affinity toward polar polysulfides due to the intrinsic nonpolar surface of carbon.Herein, we report a direct pyrolysis of the mixture urea and boric acid to synthesize B/N–codoped hierarchically porous carbon nanosheets(B–N–CSs) as efficient sulfur host for lithium–sulfur battery. The graphene–like B–N–CSs provides high specific surface area and porous structure with abundant micropores(1.1 nm) and low–range mesopores(2.3 nm), thereby constraining the sulfur active materials within the pores. More importantly, the codoped B/N elements can further enhance the polysulfide confinement through strong Li–N and B–S interaction based on the Lewis acid–base theory. These structural superiorities significantly suppress the shuttle effect by both physical confinement and chemical interaction, and promote the redox kinetics of polysulfide conversion. When evaluated as the cathode host, the S/B–N–CSs composite displays the excellent performance with a high reversible capacity up to 772 m A h g–1 at 0.5 C and a low fading rate of ^0.09% per cycle averaged upon 500 cycles. In particular, remarkable stability with a high capacity retention of 87.1% can be realized when augmenting the sulfur loading in the cathode up to 4.6 mg cm^(-2).
文摘The catalytic property of AICl(3) catalyst immobilized on gamma -Al2O3 for isobutene polymerization has been studied. It was found that the activity, selectivity and stability of the catalyst are dependent greatly on geometric characteristic pf the pore structure and size of catalyst. Although the activity and selectivity of the catalysts with micro- and meso-pore structure are all high in initial stage, but their stability is low, while those with bimodal meso- and macro-pore structure are excellent. Increasing granularity of the catalyst(particle become fine) brings about an increase in isobutene conversion, but a decrease in selectivity, resulting in lower average molecular weight and iis broader distribution.
基金Funded by the National Natural Science Foundation of China (No. 20876113)
文摘Mesoporous silica with controllable bimodal pore size distribution was synthesized with cetyltrimethylammonium bromide （CTAB） as chemical template for small mesopores and silica gel as physical template for large mesopores. The structure of synthesized samples were characterized by Fourier transform infrared （FT-IR） spectroscopy, X-ray diffraction （XRD）, scanning electron microscopy （SEM）, transmission electron microscopy （TEM） and N2 adsorption-desorption measurements. The experimental results show that bimodal mesoporous silica consists of small mesopores of about 3 nm and large mesopores of about 45 nm. The small mesopores which were formed on the external surface and pore walls of the silica gel had similar characters with those of MCM-41, while large mesopores were inherited from parent silica gel material. The pore size distribution of the synthesized silica can be adjusted by changing the relative content of TEOS and silica gel or the feeding sequence of silica gel and NH4OH.
文摘The synthesis of silica with bimodal, disordered mesopores structure, by template-mediated sol-gel processing and subsequent heat-treatment process, was investigated. In the presence of nonionic surfactant Tx-15, the organically modified mesostructured nano-particles were synthesized by co-condensation of organosiloxane （RTES） and tetraethoxysilane （TEOS） in the first step, and then the bimodal porous silica was formed by the removal of the incorporated organic groups using programmed calcination. Here, RTES used was methyltriethoxysilane （MTES）, vinyltriethoxysilane （VTES） and phenyltriethoxysilane （PhTES）, respectively. Organotrialkoxysilane, TEOS and Tx-15 formed MSU-2-1iked assemblies, around which the nano-particles aggregated and cross-linked, considerably influencing the pore size distribution of both primary pores and secondary pores. By changing the type and amount of the organotrialkoxysilane added, a broad variety of silica with a controlled bimodal mesopore distribution could be easily synthesized. Textural and structural properties were determined by X-ray diffraction, high-resolution transmission electron microscopy, N2 adsorption/desorption, and thermogravimetric analysis.
