Due to the advantages of high surface areas, large pore volumes and pore sizes, abundant nitrogen content that favored the metal-support interactions, N-doped ordered mesoporous carbons are regarded as a kind ...Due to the advantages of high surface areas, large pore volumes and pore sizes, abundant nitrogen content that favored the metal-support interactions, N-doped ordered mesoporous carbons are regarded as a kind of fascinating and potential support for the synthesis of effective supported cat-alysts. Here, a N-doped ordered mesoporous carbon with a high N content (9.58 wt%), high surface area (417 m^2/g), and three-dimensional cubic structure was synthesized successfully and used as an effective support for immobilizing Pt nanoparticles (NPs). The positive effects of nitrogen on the metal particle size enabled ultrasmall Pt NPs (about 1.0 ± 0.5 nm) to be obtained. Moreover, most of the Pt NPs are homogeneously dispersed in the mesoporous channels. However, using the ordered mesoporous carbon without nitrogen as support, the particles were larger (4.4 ± 1.7 nm) and many Pt NPs were distributed on the external surface, demonstrating the important role of the nitrogen species. The obtained N-doped ordered mesoporous material supported catalyst showed excellent catalytic activity (conversion 100%) and selectivity (〉99%) in the hydrogenation of halogenated nitrobenzenes under mild conditions. These values are much higher than those achieved using a commercial Pt/C catalyst (conversion 89% and selectivity 90%). This outstanding catalytic perfor-mance can be attributed to the synergetic effects of the mesoporous structure, N-functionalized support, and stabilized ultrasmall Pt NPs. Moreover, such supported catalyst also showed excellent catalytic performance in the hydrogenation of other halogenated nitrobenzenes and nitroarenes. In addition, the stability of the multifunctional catalyst was excellent and it could be reused more than 10 times without significant losses of activity and selectivity. Our results conclusively show that a N-doped carbon support enable the formation of ultrafine metal NPs and improve the reaction ac-tivity and selectivity.展开更多
The phase composition, phase transition and phase structure transformation of the wire-cut section of functionally graded WC-Co cemented carbide with dual phase structure were investigated by XRD phase analysis. It is...The phase composition, phase transition and phase structure transformation of the wire-cut section of functionally graded WC-Co cemented carbide with dual phase structure were investigated by XRD phase analysis. It is shown that the composition of η phase in the core zone is Co_3W_3C (M_6 C type). The structure of cobalt based solid solution binder phase is fcc type. At the cooling stage of the sintering process, the phase transition of η phase, i.e. M_6C→M_12C and the martensitic phase transition of the cobalt based solid solution binder phase, i.e. fcc→hcp are suppressed, which facilitates the strengthening of the alloy. Because the instantaneous temperature of the discharge channel is as high as 10 000 ℃ during the wire cutting process, the processed surface is oxidized. Nevertheless, the oxide layer thickness is in micro grade. In the oxide film, η phase is decomposed into W_2C and CoO, and cobalt based solid solution binder is selectively oxidized, while WC remains stable due to the existence of carbon containing liquid organic cutting medium.展开更多
Al/SiC functionally graded material(FGM) was developed through a novel multi-step friction stir processing(FSP) method. Si C particles with a mean size of 27.5 μm were embedded in the groove on the 6082-Al plate. To ...Al/SiC functionally graded material(FGM) was developed through a novel multi-step friction stir processing(FSP) method. Si C particles with a mean size of 27.5 μm were embedded in the groove on the 6082-Al plate. To create a graded structure over a predefined value, FSP was carried out with three tools with different pin lengths and with varying volume fractions of SiC particles. The structure was formed by passing tools with 1-3 passes with a constant rotational and traveling speeds of 900 r/min and 20 mm/min, respectively. The experiments were conducted at room temperature. Microstructural features of functionally graded(FG) samples were examined by using scanning electron microscopy(SEM) and 3D light microscopy. Mechanical properties in terms of wear resistance and microhardness were thoroughly assessed. The results indicate that the increase in FSP pass number causes more uniform SiC particle dispersion. The microhardness values were impacted by the number of passes and improved by 51.54% for Pass 3 when compared to as-received 6082-Al. Wear resistance of Al/SiC FG samples was found to increase as a result of the addition of SiC particles.展开更多
The energy-efficient purification of methane from C2-hydrocarbons is of great significance for the upgrading of natural gas. So does the capture of carbon dioxide for remission of greenhouse effect. It is well establi...The energy-efficient purification of methane from C2-hydrocarbons is of great significance for the upgrading of natural gas. So does the capture of carbon dioxide for remission of greenhouse effect. It is well established that some functional sites, such as open metals sites, Lewis basic nitrogen sites and fluorine groups, have shown significantly enhanced affinity toward more polarizable molecules. Thus, a water-stable Eu3+-based fcu-metal-organic framework(MOF)(compound 1) with amino functional groups has been successfully constructed through a reticular chemistry approach.As a result, the activated compound 1 exhibits moderately high uptakes of C2-hydrocarbons, but a less obvious adsorption of CH4 at the same conditions. Among them, the adsorption capacity of C2 H2 is up to 143.6 cm3 cm-3 and a relatively high selectivity of C2 H2/CH4(107.7) is obtained at near room temperature. Moreover, compound 1 is also validated as an exceptional adsorbent for CO2 capture, with the fairly high capacity of CO2(92.6 cm3 cm-3) and CO2/N2 selectivity(151.7) at ambient conditions. The excellent performance of compound 1 is mainly driven by the exposed amino functional groups within the contracted pores. Such effect thus leads to the achievement of dual-functional platform for methane purification and carbon dioxide capture. Furthermore, compound 1 features a satisfactory water stability,which is confirmed by the powder X-ray diffraction(PXRD)analysis and the retest of porosity after being soaked in water.展开更多
Ultrasmall FeCo-graphitic carbon shell nanocrystals (FeCo/GC) are promising multifunctional materials capable of highly efficient drug delivery in vitro and magnetic resonance imaging in vivo. In this work, we demon...Ultrasmall FeCo-graphitic carbon shell nanocrystals (FeCo/GC) are promising multifunctional materials capable of highly efficient drug delivery in vitro and magnetic resonance imaging in vivo. In this work, we demonstrate the use of FeCo/GC for highly effective cancer therapy through combined drug delivery, tumor-selective near-infrared photothermal therapy, and cancer imaging of a 4T1 syngeneic breast cancer model. The graphitic carbon shell of the ~4 nm FeCo/GC readily loads doxorubicin (DOX) via π-π stacking and absorbs near-infrared light giving photothermal heating. When used for cancer treatment, intravenously administrated FeCo/GC-DOX led to complete tumor regression in 45% of mice when combined with 20 min of near-infrared laser irradiation selectively heating the tumor to 43-45 ℃. In addition, the use of FeCo/GC-DOX results in reduced systemic toxicity compared with free DOX and appears to be safe in mice monitored for over 1 yr. FeCo/GC-DOX is shown to be a highly integrated nanoparticle system for synergistic cancer therapy leading to tumor regression of a highly aggressive tumor model.展开更多
Poly(3-hexylthiophene) (P3HT) has received much attention as a good candidate to replace inorganic semiconductors for flexible electronics due to its solution-processability. However, the low charge mobility of P3...Poly(3-hexylthiophene) (P3HT) has received much attention as a good candidate to replace inorganic semiconductors for flexible electronics due to its solution-processability. However, the low charge mobility of P3HT is an obstacle to its commercialization. To overcome this problem, we propose a new non-covalent functionalization method for carbon nanotubes (CNTs) for use in CNT/P3HT nanocomposites. By using modified pyrene molecules with hydrophobic long alkyl chains, the non-covalently functionalized CNTs can become well dispersed in hydrophobic solutions and organic semiconductor matrices. Fabrication of organic thin-film transistors (OTFTs) from the non-covalently functionalized CNT/organic semiconductor nanocomposites shows that our non-covalent functionalization method significantly reduces damage to CNTs during functionalization when compared with covalent functionalization by treatment with acids. The OTFTs show 15 times enhancement of field effect mobility (1.5 × 10^-2 cm^2/(V.s)) compared to the mobility of OTFTs made from pure P3HT. This enhancement is achieved by addition of only 0.25 wt% of CNTs to P3HT.展开更多
Rare earth doping has been widely applied in many functional nanomaterials with desirable properties and functions,which would have a significant effect on the growth process of the materials.However,the controlling s...Rare earth doping has been widely applied in many functional nanomaterials with desirable properties and functions,which would have a significant effect on the growth process of the materials.However,the controlling strategy is limited into high concentration of lanthanide doping,which produces concentration quenching of the lanthanide ion luminescence with an increase in the Ln^(3+)concentration,resulting in lowering the fluorescence quantum yield of lanthanide ion.Herein,for the first time,we demonstrate simultaneous control of the structures and luminescence properties of BaCO_3nanocrystals via a small amount of Tb^(3+)doping strategy.In fact,Tb^(3+)would partially occupy Ba^(2+)sites,resulting in the changes to the structures of the BaCO_3nanocrystals,which is primarily determined by charge modulation,including the contributions from the surfaces of crystal nuclei and building blocks.These structurally modified nanocrystals exhibit tunable luminescence properties,thus emerging as potential candidates for photonic devices such as light-emitting diodes and color displays.展开更多
基金supported by the National Natural Science Foundation of China(201573136,U1510105)the Scientific Research Start-up Funds of Shanxi University(RSC723)~~
文摘Due to the advantages of high surface areas, large pore volumes and pore sizes, abundant nitrogen content that favored the metal-support interactions, N-doped ordered mesoporous carbons are regarded as a kind of fascinating and potential support for the synthesis of effective supported cat-alysts. Here, a N-doped ordered mesoporous carbon with a high N content (9.58 wt%), high surface area (417 m^2/g), and three-dimensional cubic structure was synthesized successfully and used as an effective support for immobilizing Pt nanoparticles (NPs). The positive effects of nitrogen on the metal particle size enabled ultrasmall Pt NPs (about 1.0 ± 0.5 nm) to be obtained. Moreover, most of the Pt NPs are homogeneously dispersed in the mesoporous channels. However, using the ordered mesoporous carbon without nitrogen as support, the particles were larger (4.4 ± 1.7 nm) and many Pt NPs were distributed on the external surface, demonstrating the important role of the nitrogen species. The obtained N-doped ordered mesoporous material supported catalyst showed excellent catalytic activity (conversion 100%) and selectivity (〉99%) in the hydrogenation of halogenated nitrobenzenes under mild conditions. These values are much higher than those achieved using a commercial Pt/C catalyst (conversion 89% and selectivity 90%). This outstanding catalytic perfor-mance can be attributed to the synergetic effects of the mesoporous structure, N-functionalized support, and stabilized ultrasmall Pt NPs. Moreover, such supported catalyst also showed excellent catalytic performance in the hydrogenation of other halogenated nitrobenzenes and nitroarenes. In addition, the stability of the multifunctional catalyst was excellent and it could be reused more than 10 times without significant losses of activity and selectivity. Our results conclusively show that a N-doped carbon support enable the formation of ultrafine metal NPs and improve the reaction ac-tivity and selectivity.
基金Projects(50323008, 50574104) supported by the National Natural Science Foundation of ChinaProject (04JJ3084) supported by the Natural Science Foundation of Hunan Province, China
文摘The phase composition, phase transition and phase structure transformation of the wire-cut section of functionally graded WC-Co cemented carbide with dual phase structure were investigated by XRD phase analysis. It is shown that the composition of η phase in the core zone is Co_3W_3C (M_6 C type). The structure of cobalt based solid solution binder phase is fcc type. At the cooling stage of the sintering process, the phase transition of η phase, i.e. M_6C→M_12C and the martensitic phase transition of the cobalt based solid solution binder phase, i.e. fcc→hcp are suppressed, which facilitates the strengthening of the alloy. Because the instantaneous temperature of the discharge channel is as high as 10 000 ℃ during the wire cutting process, the processed surface is oxidized. Nevertheless, the oxide layer thickness is in micro grade. In the oxide film, η phase is decomposed into W_2C and CoO, and cobalt based solid solution binder is selectively oxidized, while WC remains stable due to the existence of carbon containing liquid organic cutting medium.
文摘Al/SiC functionally graded material(FGM) was developed through a novel multi-step friction stir processing(FSP) method. Si C particles with a mean size of 27.5 μm were embedded in the groove on the 6082-Al plate. To create a graded structure over a predefined value, FSP was carried out with three tools with different pin lengths and with varying volume fractions of SiC particles. The structure was formed by passing tools with 1-3 passes with a constant rotational and traveling speeds of 900 r/min and 20 mm/min, respectively. The experiments were conducted at room temperature. Microstructural features of functionally graded(FG) samples were examined by using scanning electron microscopy(SEM) and 3D light microscopy. Mechanical properties in terms of wear resistance and microhardness were thoroughly assessed. The results indicate that the increase in FSP pass number causes more uniform SiC particle dispersion. The microhardness values were impacted by the number of passes and improved by 51.54% for Pass 3 when compared to as-received 6082-Al. Wear resistance of Al/SiC FG samples was found to increase as a result of the addition of SiC particles.
基金supported by the National Natural Science Foundation of China(U1609219,51632008,61721005,51432001and 51772268)Zhejiang Provincial Natural Science Foundation(LD18E020001)
文摘The energy-efficient purification of methane from C2-hydrocarbons is of great significance for the upgrading of natural gas. So does the capture of carbon dioxide for remission of greenhouse effect. It is well established that some functional sites, such as open metals sites, Lewis basic nitrogen sites and fluorine groups, have shown significantly enhanced affinity toward more polarizable molecules. Thus, a water-stable Eu3+-based fcu-metal-organic framework(MOF)(compound 1) with amino functional groups has been successfully constructed through a reticular chemistry approach.As a result, the activated compound 1 exhibits moderately high uptakes of C2-hydrocarbons, but a less obvious adsorption of CH4 at the same conditions. Among them, the adsorption capacity of C2 H2 is up to 143.6 cm3 cm-3 and a relatively high selectivity of C2 H2/CH4(107.7) is obtained at near room temperature. Moreover, compound 1 is also validated as an exceptional adsorbent for CO2 capture, with the fairly high capacity of CO2(92.6 cm3 cm-3) and CO2/N2 selectivity(151.7) at ambient conditions. The excellent performance of compound 1 is mainly driven by the exposed amino functional groups within the contracted pores. Such effect thus leads to the achievement of dual-functional platform for methane purification and carbon dioxide capture. Furthermore, compound 1 features a satisfactory water stability,which is confirmed by the powder X-ray diffraction(PXRD)analysis and the retest of porosity after being soaked in water.
文摘Ultrasmall FeCo-graphitic carbon shell nanocrystals (FeCo/GC) are promising multifunctional materials capable of highly efficient drug delivery in vitro and magnetic resonance imaging in vivo. In this work, we demonstrate the use of FeCo/GC for highly effective cancer therapy through combined drug delivery, tumor-selective near-infrared photothermal therapy, and cancer imaging of a 4T1 syngeneic breast cancer model. The graphitic carbon shell of the ~4 nm FeCo/GC readily loads doxorubicin (DOX) via π-π stacking and absorbs near-infrared light giving photothermal heating. When used for cancer treatment, intravenously administrated FeCo/GC-DOX led to complete tumor regression in 45% of mice when combined with 20 min of near-infrared laser irradiation selectively heating the tumor to 43-45 ℃. In addition, the use of FeCo/GC-DOX results in reduced systemic toxicity compared with free DOX and appears to be safe in mice monitored for over 1 yr. FeCo/GC-DOX is shown to be a highly integrated nanoparticle system for synergistic cancer therapy leading to tumor regression of a highly aggressive tumor model.
文摘Poly(3-hexylthiophene) (P3HT) has received much attention as a good candidate to replace inorganic semiconductors for flexible electronics due to its solution-processability. However, the low charge mobility of P3HT is an obstacle to its commercialization. To overcome this problem, we propose a new non-covalent functionalization method for carbon nanotubes (CNTs) for use in CNT/P3HT nanocomposites. By using modified pyrene molecules with hydrophobic long alkyl chains, the non-covalently functionalized CNTs can become well dispersed in hydrophobic solutions and organic semiconductor matrices. Fabrication of organic thin-film transistors (OTFTs) from the non-covalently functionalized CNT/organic semiconductor nanocomposites shows that our non-covalent functionalization method significantly reduces damage to CNTs during functionalization when compared with covalent functionalization by treatment with acids. The OTFTs show 15 times enhancement of field effect mobility (1.5 × 10^-2 cm^2/(V.s)) compared to the mobility of OTFTs made from pure P3HT. This enhancement is achieved by addition of only 0.25 wt% of CNTs to P3HT.
基金supported by the National Natural Science Foundation of China (21403189, 21371149) Natural Science Foundation of Hebei Province (B2017203198)+1 种基金China Postdoctoral Science Foundation (2014M551047)Yanshan University Doctoral Foundation (B790)
文摘Rare earth doping has been widely applied in many functional nanomaterials with desirable properties and functions,which would have a significant effect on the growth process of the materials.However,the controlling strategy is limited into high concentration of lanthanide doping,which produces concentration quenching of the lanthanide ion luminescence with an increase in the Ln^(3+)concentration,resulting in lowering the fluorescence quantum yield of lanthanide ion.Herein,for the first time,we demonstrate simultaneous control of the structures and luminescence properties of BaCO_3nanocrystals via a small amount of Tb^(3+)doping strategy.In fact,Tb^(3+)would partially occupy Ba^(2+)sites,resulting in the changes to the structures of the BaCO_3nanocrystals,which is primarily determined by charge modulation,including the contributions from the surfaces of crystal nuclei and building blocks.These structurally modified nanocrystals exhibit tunable luminescence properties,thus emerging as potential candidates for photonic devices such as light-emitting diodes and color displays.