The external surface of HZSM-5 zeolite was passivated by liquid siliceous deposition and by acidic sites poisoning with lepidine, respectively. Then methanol-to-hydrocarbons (MTH) reaction was investigated over the ...The external surface of HZSM-5 zeolite was passivated by liquid siliceous deposition and by acidic sites poisoning with lepidine, respectively. Then methanol-to-hydrocarbons (MTH) reaction was investigated over the above as-prepared catalysts and the dissoluble coke on these used catalysts was analyzed by GC-MS, to study the role of the external surface of HZSM-5 in the catalytic reaction. Comparison with the experi- mental results based on parent ZSM-5 showed that the product distribution of MTH reaction was obviously influenced by the external surface. Evidences were listed as follows: (1) the final product on parent HZSM-5 showed higher aromatic selectivity, lower olefin selectivity, lower ra- tio of C2/C3+ aliphatics and higher ratio of C3/C4+ aliphatics than the reaction mixture produced by the sole catalysis of acidic sites in HZSM-5 channel; (2) a little of pentamethylbenzene and hexamethylbenzene in the product on parent HZSM-5, was produced via multi-methylation of methylbenzene on the external surface. The above conclusion may also be suitable for MTH reaction over other zeolites with 10-ring channel.展开更多
This study examined the thermal effects of building′s external wall surfaces, using observational data of spatial-temporal distribution of surface temperature, air temperature, and heat flux into and out of external ...This study examined the thermal effects of building′s external wall surfaces, using observational data of spatial-temporal distribution of surface temperature, air temperature, and heat flux into and out of external surface. Results indicate that external wall surface temperature and nearby air temperature vary with the change of orientation, height and season. In general, the external wall surface temperature is lower near the ground, and is higher near the roof, than nearby air temperature. But north wall surface temperature is mostly lower than nearby air temperature at the same height; south wall surface temperature during the daytime in December, and west wall surface temperature all day in August, is respectively higher than nearby air temperature. The heat fluxes into and out of external wall surfaces show the differences that exist in the various orientations, heights and seasons. In December, south wall surface at the lower sites emits heat and north wall surface at the higher sites absorbs heat. In April, all external wall surfaces, emit heat near the ground and absorb heat near the roof. In August, west wall surface all day emits heat, and other wall surfaces just show the commensurate behavior with that in April.展开更多
In this work, four empirical models of statistical thickness, namely the models of Harkins and Jura, Hasley, Carbon Black and Jaroniec, were compared in order to determine the textural properties (external surface and...In this work, four empirical models of statistical thickness, namely the models of Harkins and Jura, Hasley, Carbon Black and Jaroniec, were compared in order to determine the textural properties (external surface and surface of micropores) of a clay concrete without molasses and clay concretes stabilized with 8%, 12% and 16% molasses. The results obtained show that Hasley’s model can be used to obtain the external surfaces. However, it does not allow the surface of the micropores to be obtained, and is not suitable for the case of simple clay concrete (without molasses) and for clay concretes stabilized with molasses. The Carbon Black, Jaroniec and Harkins and Jura models can be used for clay concrete and stabilized clay concrete. However, the Carbon Black model is the most relevant for clay concrete and the Harkins and Jura model is for molasses-stabilized clay concrete. These last two models augur well for future research.展开更多
Internal and external wall surface temperatures (Tws) in April, August and December in Kunming, a city in low latitude plateau, were investigated. Results showed that the Tws in April were of the highest among the thr...Internal and external wall surface temperatures (Tws) in April, August and December in Kunming, a city in low latitude plateau, were investigated. Results showed that the Tws in April were of the highest among the three, followed by August and December. The Tws differences among walls with different orientation were higher in April and December when the weather tends to be sunny, and lower in August with more cloudy days in the time. In April and August, Tws of E-wall was the highest, followed by S- and N-wall. But in December Tws of S-wall might be sometimes higher than E one. Diurnal range of internal Tws was usually smaller than that of the external, with also a time lag for the occurrence of its maximum and minimum. The results can serve as a basis for further research on building microclimate and urban architecture designs. It also gives suggestions for similar studies in other areas.展开更多
Silicoaluminophosphate-34(SAPO-34) molecular sieves have important applications in the petrochemical industry as a result of their shape selectivity and suitable acidity. In this work, nanoaggregate SAPO-34 with a lar...Silicoaluminophosphate-34(SAPO-34) molecular sieves have important applications in the petrochemical industry as a result of their shape selectivity and suitable acidity. In this work, nanoaggregate SAPO-34 with a large external surface area was obtained by dissolving pseudoboehmite and tetraethylorthosilicate in an aqueous solution of tetraethylammonium hydroxide and subsequently adding phosphoric acid. After hydrolysis in an alkaline solution, the aluminum and silicon precursors exist as Al(OH)4-and SiO2(OH)-, respectively;this is beneficial for rapid nucleation and the formation of nanoaggregates in the following crystallization process. Additionally, to study the effect of the external surface area and pore size on the catalytic performance of different SAPO-34 structures, the alcoholysis of furfuryl alcohol to ethyl levulinate(EL) was chosen as a model reaction. In a comparison with the traditional cube-like SAPO-34, nanoaggregate SAPO-34 generated a higher yield of 74.1% of EL, whereas that with cube-like SAPO-34 was only 19.9%. Moreover, the stability was remarkably enhanced for nanoaggregate SAPO-34. The greater external surface area and larger number of external surface acid sites are helpful in improving the catalytic performance and avoiding coke deposition.展开更多
To enhance the gasoline octane number,low-octane linear n-alkanes should be converted into their high-octane di-branched isomers via n-alkane hydroisomerization.Therefore,hierarchical SAPO-11-based catalysts are prepa...To enhance the gasoline octane number,low-octane linear n-alkanes should be converted into their high-octane di-branched isomers via n-alkane hydroisomerization.Therefore,hierarchical SAPO-11-based catalysts are prepared by adding different contents of sodium dodecylbenzene sulfonate(SDBS),and they are applied in n-nonane hydroisomerization.When n(SDBS)/n(SiO2)is less than or equal to 0.125,the synthesized hierarchical molecular sieves are all pure SAPO-11,and as the SDBS content increases,the submicron particle size decreases,and the external surface area(ESA)increases.Additionally,these hierarchical SAPO-11 have smaller submicron particles and higher ESA values than conventional SAPO-11.When n(SDBS)/n(SiO2)is greater than 0.125,with increasing SDBS content(n(SDBS)/n(SiO2)=0.25),the synthesized SAPO-11 contains amorphous materials,which leads to a decline in the ESA;with the further increase in SDBS content(n(SDBS)/n(SiO2)=0.5),the products are all amorphous materials.These results indicate that in the case of n(SDBS)/n(SiO2)=0.125,the synthesized SAPO-11 molecular sieve(S–S3)has the most external Brønsted acid centers and the highest ESA of these SAPO-11,and these advantages favor generation of the di-branched isomers in hydrocarbon hydroisomerization.Among these Pt/SAPO-11 catalysts,Pt/S–S3 displays the highest selectivity to entire isomers(83.4%),the highest selectivity to di-branched isomers(28.1%)and the minimum hydrocracking selectivity(15.7%)in n-nonane hydroisomerization.展开更多
The last half-century was transformed by the electronic revolution that essentially reproduced the human brain and its computing capacity on a chip. But over time, scientists have realized that something was missing t...The last half-century was transformed by the electronic revolution that essentially reproduced the human brain and its computing capacity on a chip. But over time, scientists have realized that something was missing to give life, so to speak, to the small chip with a brain: One needed to awaken its senses and develop its muscles! This challenge was solved through MEMS (micro electro mechanical systems). Indeed, MEMS today are equipped with the sense of sight, smell, hearing, taste and touch through microsensors. They are also capable of physical exertion through small muscles called microactuators. These new capabilities open wide fields of imagination and important specific applications.展开更多
The physicochemical properties of surfaces have a great effect on the micro-morphologies of the crystal structures which are in contact with them.Understanding the interaction mechanism between the internal driving fo...The physicochemical properties of surfaces have a great effect on the micro-morphologies of the crystal structures which are in contact with them.Understanding the interaction mechanism between the internal driving forces of the crystal and external inducing forces of the surfaces is the prerequisite of controlling and obtaining the desirable morphologies.In this work,the dynamic density functional theory was applied to construct the free energy functional expression of polyethylene(PE)lattice,and the micro-dynamic evolution processes of PE lattice morphology near the surfaces with different properties were observed to reveal the interaction mechanism at atomic scale.The results showed that the physical and chemical properties of the external surfaces synergistically affect the morphologies in both the defect shapes and the distribution of the defect regions.In the absence of the contact surfaces,driven by the oriented interactions among different CH2 groups,PE lattices gradually grow and form a defect-free structure.Conversely,the presence of contact surfaces leads to lattice defects in the interfacial regions,and PE lattice shows different self-healing abilities around different surfaces.展开更多
Gauss maps of oriented timelike 2-surfaces in are characterized, and it is shown that Gallss maps can determine surfaces locally as they do in case. Moreover, some essential differences are discovered between the prop...Gauss maps of oriented timelike 2-surfaces in are characterized, and it is shown that Gallss maps can determine surfaces locally as they do in case. Moreover, some essential differences are discovered between the properties of the Gauss maps of surfaces in Rn and those of the Gauss maps of timelike surfaces in. In particular, a counterexample shows that a nonminimal timelike surface in cannot be essentially determined by its Gauss map.展开更多
The nonlinear sorption of hydrophobic organic contaminants(HOCs)could be changed to linear sorption by the suppression of coexisting solutes in natural system,resulting in the enhancement of mobility,bioavailability a...The nonlinear sorption of hydrophobic organic contaminants(HOCs)could be changed to linear sorption by the suppression of coexisting solutes in natural system,resulting in the enhancement of mobility,bioavailability and risks of HOCs in the environment.In previous study,inspired from the competitive adsorption on activated carbon(AC),the displaceable fraction of HOCs sorption to soot by competitor was attributed to the adsorption on elemental carbon fraction of soot(EC-Soot),while the linear and nondisplaceable fraction was attributed to the partition in authigenic organic matter of soot(OM-Soot).In this study,however,we observed that the linear and nondisplaceable fraction of HOC(naphthalene)to a diesel soot(D-Soot)by competitor(phenanthrene or p-nitrophenol)should be attributed to not only the linear partition in OM-Soot,but also the residual linear adsorption on EC-Soot.We also observed that the competition on the surface of soot dominated by external surface was different from that of AC dominated by micropore surface,i.e.,complete displacement of HOCs by p-nitrophenol could occur for the micropore surface of AC,but not for the external surface of soot.These observations were obtained through the separation of EC-Soot and OM-Soot from D-Soot with organic-solvent extraction and the sorption comparisons of D-Soot with an AC(ACF300)and a multiwalled carbon nanotube(MWCNT30).The obtained results would give new insights to the sorption mechanisms of HOCs by soot and help to assess their environmental risks.展开更多
基金supported by Shanghai Key Basic Research(Grant No.11JC1412500)the National Natural Science Foundation of China(Grant No.51174277)
文摘The external surface of HZSM-5 zeolite was passivated by liquid siliceous deposition and by acidic sites poisoning with lepidine, respectively. Then methanol-to-hydrocarbons (MTH) reaction was investigated over the above as-prepared catalysts and the dissoluble coke on these used catalysts was analyzed by GC-MS, to study the role of the external surface of HZSM-5 in the catalytic reaction. Comparison with the experi- mental results based on parent ZSM-5 showed that the product distribution of MTH reaction was obviously influenced by the external surface. Evidences were listed as follows: (1) the final product on parent HZSM-5 showed higher aromatic selectivity, lower olefin selectivity, lower ra- tio of C2/C3+ aliphatics and higher ratio of C3/C4+ aliphatics than the reaction mixture produced by the sole catalysis of acidic sites in HZSM-5 channel; (2) a little of pentamethylbenzene and hexamethylbenzene in the product on parent HZSM-5, was produced via multi-methylation of methylbenzene on the external surface. The above conclusion may also be suitable for MTH reaction over other zeolites with 10-ring channel.
文摘This study examined the thermal effects of building′s external wall surfaces, using observational data of spatial-temporal distribution of surface temperature, air temperature, and heat flux into and out of external surface. Results indicate that external wall surface temperature and nearby air temperature vary with the change of orientation, height and season. In general, the external wall surface temperature is lower near the ground, and is higher near the roof, than nearby air temperature. But north wall surface temperature is mostly lower than nearby air temperature at the same height; south wall surface temperature during the daytime in December, and west wall surface temperature all day in August, is respectively higher than nearby air temperature. The heat fluxes into and out of external wall surfaces show the differences that exist in the various orientations, heights and seasons. In December, south wall surface at the lower sites emits heat and north wall surface at the higher sites absorbs heat. In April, all external wall surfaces, emit heat near the ground and absorb heat near the roof. In August, west wall surface all day emits heat, and other wall surfaces just show the commensurate behavior with that in April.
文摘In this work, four empirical models of statistical thickness, namely the models of Harkins and Jura, Hasley, Carbon Black and Jaroniec, were compared in order to determine the textural properties (external surface and surface of micropores) of a clay concrete without molasses and clay concretes stabilized with 8%, 12% and 16% molasses. The results obtained show that Hasley’s model can be used to obtain the external surfaces. However, it does not allow the surface of the micropores to be obtained, and is not suitable for the case of simple clay concrete (without molasses) and for clay concretes stabilized with molasses. The Carbon Black, Jaroniec and Harkins and Jura models can be used for clay concrete and stabilized clay concrete. However, the Carbon Black model is the most relevant for clay concrete and the Harkins and Jura model is for molasses-stabilized clay concrete. These last two models augur well for future research.
基金Key project from the Natural Science Foundation of China (59836250)
文摘Internal and external wall surface temperatures (Tws) in April, August and December in Kunming, a city in low latitude plateau, were investigated. Results showed that the Tws in April were of the highest among the three, followed by August and December. The Tws differences among walls with different orientation were higher in April and December when the weather tends to be sunny, and lower in August with more cloudy days in the time. In April and August, Tws of E-wall was the highest, followed by S- and N-wall. But in December Tws of S-wall might be sometimes higher than E one. Diurnal range of internal Tws was usually smaller than that of the external, with also a time lag for the occurrence of its maximum and minimum. The results can serve as a basis for further research on building microclimate and urban architecture designs. It also gives suggestions for similar studies in other areas.
文摘Silicoaluminophosphate-34(SAPO-34) molecular sieves have important applications in the petrochemical industry as a result of their shape selectivity and suitable acidity. In this work, nanoaggregate SAPO-34 with a large external surface area was obtained by dissolving pseudoboehmite and tetraethylorthosilicate in an aqueous solution of tetraethylammonium hydroxide and subsequently adding phosphoric acid. After hydrolysis in an alkaline solution, the aluminum and silicon precursors exist as Al(OH)4-and SiO2(OH)-, respectively;this is beneficial for rapid nucleation and the formation of nanoaggregates in the following crystallization process. Additionally, to study the effect of the external surface area and pore size on the catalytic performance of different SAPO-34 structures, the alcoholysis of furfuryl alcohol to ethyl levulinate(EL) was chosen as a model reaction. In a comparison with the traditional cube-like SAPO-34, nanoaggregate SAPO-34 generated a higher yield of 74.1% of EL, whereas that with cube-like SAPO-34 was only 19.9%. Moreover, the stability was remarkably enhanced for nanoaggregate SAPO-34. The greater external surface area and larger number of external surface acid sites are helpful in improving the catalytic performance and avoiding coke deposition.
基金The authors gratefully acknowledge the financial support of the National Natural Science Foundation of China(Grant No.21978323)。
文摘To enhance the gasoline octane number,low-octane linear n-alkanes should be converted into their high-octane di-branched isomers via n-alkane hydroisomerization.Therefore,hierarchical SAPO-11-based catalysts are prepared by adding different contents of sodium dodecylbenzene sulfonate(SDBS),and they are applied in n-nonane hydroisomerization.When n(SDBS)/n(SiO2)is less than or equal to 0.125,the synthesized hierarchical molecular sieves are all pure SAPO-11,and as the SDBS content increases,the submicron particle size decreases,and the external surface area(ESA)increases.Additionally,these hierarchical SAPO-11 have smaller submicron particles and higher ESA values than conventional SAPO-11.When n(SDBS)/n(SiO2)is greater than 0.125,with increasing SDBS content(n(SDBS)/n(SiO2)=0.25),the synthesized SAPO-11 contains amorphous materials,which leads to a decline in the ESA;with the further increase in SDBS content(n(SDBS)/n(SiO2)=0.5),the products are all amorphous materials.These results indicate that in the case of n(SDBS)/n(SiO2)=0.125,the synthesized SAPO-11 molecular sieve(S–S3)has the most external Brønsted acid centers and the highest ESA of these SAPO-11,and these advantages favor generation of the di-branched isomers in hydrocarbon hydroisomerization.Among these Pt/SAPO-11 catalysts,Pt/S–S3 displays the highest selectivity to entire isomers(83.4%),the highest selectivity to di-branched isomers(28.1%)and the minimum hydrocracking selectivity(15.7%)in n-nonane hydroisomerization.
文摘The last half-century was transformed by the electronic revolution that essentially reproduced the human brain and its computing capacity on a chip. But over time, scientists have realized that something was missing to give life, so to speak, to the small chip with a brain: One needed to awaken its senses and develop its muscles! This challenge was solved through MEMS (micro electro mechanical systems). Indeed, MEMS today are equipped with the sense of sight, smell, hearing, taste and touch through microsensors. They are also capable of physical exertion through small muscles called microactuators. These new capabilities open wide fields of imagination and important specific applications.
基金supported by the National Natural Science Foundation of China(Nos.21476007,21673197,21621091)the National Key R&D Program of China(No.2018YFA0209500)+4 种基金the 111 Project(No.B16029)the Fundamental Research Funds for the Central Universities of China(No.20720190037)the Natural Science Foundation of Fujian Province of China(No.2018J06003)the Special Project of Strategic Emerging Industries from Fujian Development and Reform CommissionChemcloudcomputing of Beijing University of Chemical Technology。
文摘The physicochemical properties of surfaces have a great effect on the micro-morphologies of the crystal structures which are in contact with them.Understanding the interaction mechanism between the internal driving forces of the crystal and external inducing forces of the surfaces is the prerequisite of controlling and obtaining the desirable morphologies.In this work,the dynamic density functional theory was applied to construct the free energy functional expression of polyethylene(PE)lattice,and the micro-dynamic evolution processes of PE lattice morphology near the surfaces with different properties were observed to reveal the interaction mechanism at atomic scale.The results showed that the physical and chemical properties of the external surfaces synergistically affect the morphologies in both the defect shapes and the distribution of the defect regions.In the absence of the contact surfaces,driven by the oriented interactions among different CH2 groups,PE lattices gradually grow and form a defect-free structure.Conversely,the presence of contact surfaces leads to lattice defects in the interfacial regions,and PE lattice shows different self-healing abilities around different surfaces.
文摘Gauss maps of oriented timelike 2-surfaces in are characterized, and it is shown that Gallss maps can determine surfaces locally as they do in case. Moreover, some essential differences are discovered between the properties of the Gauss maps of surfaces in Rn and those of the Gauss maps of timelike surfaces in. In particular, a counterexample shows that a nonminimal timelike surface in cannot be essentially determined by its Gauss map.
基金supported partly by the National Natural Science Foundation of China(Nos.21777138 and 21621005)the National Key Research and Development Program of China(No.2017YFA0207001)+1 种基金the Key Research and Development Program of Zhejiang Province(No.2019C03105)。
文摘The nonlinear sorption of hydrophobic organic contaminants(HOCs)could be changed to linear sorption by the suppression of coexisting solutes in natural system,resulting in the enhancement of mobility,bioavailability and risks of HOCs in the environment.In previous study,inspired from the competitive adsorption on activated carbon(AC),the displaceable fraction of HOCs sorption to soot by competitor was attributed to the adsorption on elemental carbon fraction of soot(EC-Soot),while the linear and nondisplaceable fraction was attributed to the partition in authigenic organic matter of soot(OM-Soot).In this study,however,we observed that the linear and nondisplaceable fraction of HOC(naphthalene)to a diesel soot(D-Soot)by competitor(phenanthrene or p-nitrophenol)should be attributed to not only the linear partition in OM-Soot,but also the residual linear adsorption on EC-Soot.We also observed that the competition on the surface of soot dominated by external surface was different from that of AC dominated by micropore surface,i.e.,complete displacement of HOCs by p-nitrophenol could occur for the micropore surface of AC,but not for the external surface of soot.These observations were obtained through the separation of EC-Soot and OM-Soot from D-Soot with organic-solvent extraction and the sorption comparisons of D-Soot with an AC(ACF300)and a multiwalled carbon nanotube(MWCNT30).The obtained results would give new insights to the sorption mechanisms of HOCs by soot and help to assess their environmental risks.