Low‐temperature CO oxidation is important for both fundamental studies and practical applica‐tions. Supported gold catalysts are generally regarded as the most active catalysts for low‐temperature CO oxidation. The...Low‐temperature CO oxidation is important for both fundamental studies and practical applica‐tions. Supported gold catalysts are generally regarded as the most active catalysts for low‐temperature CO oxidation. The active sites are traditionally believed to be Au nanoclusters or nanoparticles in the size range of 0.5–5 nm. Only in the last few years have single‐atom Au catalysts been proved to be active for CO oxidation. Recent advances in both experimental and theoretical studies on single‐atom Au catalysts unambiguously demonstrated that when dispersed on suitable oxide supports the Au single atoms can be extremely active for CO oxidation. In this mini‐review, recent advances in the development of Au single‐atom catalysts are discussed, with the aim of illus‐trating their unique catalytic features during CO oxidation.展开更多
Resurrection plants which are able to quickly reactivate after falling into a period of anabiosis caused by dehydration have been very rare among angiosperms, especially among dicotyledons whose chlorophyll content an...Resurrection plants which are able to quickly reactivate after falling into a period of anabiosis caused by dehydration have been very rare among angiosperms, especially among dicotyledons whose chlorophyll content and chloroplast structure little changed in the course of desiccation, therefore has been called homoiochlorophyllous desiccation-tolerant plants (HDTs). Another type of resurrection angiosperms that lost its chlorophyll dining desiccation is called poikilochlorophyllous desiccation-tolerant plants (PDTs). HDTs have been received more attention because of simplicity of protection mechanism which is much easy to the study and utilization of the desiccation tolerance of resurrection angiosperms. Recent advances in studies of photosynthesis of resurrection angiosperms indicate that photochemical activities are sensitive indicators for the study of physiological state of resurrection angiosperms during desiccation and rehydration. Photochemical activities of resurrection angiosperms are inhibited with loss of water similar to those of general plants, however, the magic thing is that they could reactivate rapidly during rehydration even losing more than 95% water. Up-regulations in xanthophyll cycle and antioxidative systems as well as preservation in integrity and stability of photosynthetic membranes during desiccation may be very important to desiccation tolerance of resurrection angiosperms. The fact that phosphate treatment in rehydration stage also strongly influences resurrection indicated importance of studies on rehydration stages of resurrection angiosperms.展开更多
Flower-like 3D CuO microspheres were synthesized and used to photo-catalyze water oxidation under visible light.The structure of the CuO microspheres was characterized by scanning electron microscopy,transmission elec...Flower-like 3D CuO microspheres were synthesized and used to photo-catalyze water oxidation under visible light.The structure of the CuO microspheres was characterized by scanning electron microscopy,transmission electron microscopy,infrared,powder X-ray diffraction,electron dispersive spectroscopy,Raman and X-ray photoelectron spectroscopy(XPS).This is the first time that a copper oxide was demonstrated as a photocatalytic water oxidation catalyst under near neutral conditions.The catalytic activity of CuO microspheres in borate buffer shows the best performance with O2 yield of 11.5%.No change in the surface properties of CuO before and after the photocatalytic reaction was seen by XPS,which showed good catalyst stability.A photocatalytic water oxidation reaction mechanism catalyzed by the CuO microspheres was proposed.展开更多
Colored layered double hydroxides (LDHs) can be synthesized by introducing colored cations such as Fe^3+ and Cr^3 +, which call be used as thermal stabilizers for polyvinyl chloride (PVC). The yellowish Mg/Fe an...Colored layered double hydroxides (LDHs) can be synthesized by introducing colored cations such as Fe^3+ and Cr^3 +, which call be used as thermal stabilizers for polyvinyl chloride (PVC). The yellowish Mg/Fe and bluish Mg/Cr LDHs are prepared by the co-precipitation method. The results show that the MgsCr_ CO3 and Mg3Fe_ CO3 colored layered double hydroxides can stabilize PVC for more than 30 min under the thermal aging temperature of 180 ℃. The preparation can use cheap Mg(OH) 2 instead of MgCl2, which produces a much smaller amount of the by-product NH4Cl. It is known that NH4Cl is a cheap fertilizer that is difficult to sell; therefore, the preparation is much greener and more economic than the one using magnesium salt.展开更多
A new type of thermal stabilizer, antimony pent(isooctyl thioglycollate)(Sb(SCH2COOC8H17)5), was synthesized by using antimony trioxide, isooctanol and thioglycolic acid in 2 steps. Firstly, antimony trioxide was ox...A new type of thermal stabilizer, antimony pent(isooctyl thioglycollate)(Sb(SCH2COOC8H17)5), was synthesized by using antimony trioxide, isooctanol and thioglycolic acid in 2 steps. Firstly, antimony trioxide was oxidized into colloidal antimony peroxide. Then antimony peroxide and isooctyl thioglycollate reacted stoichiometrically for 2 h with the yield of 87%. This compound was used as thermal stabilizer for polyvinyl chloride(PVC). The results show that the thermal stability time is 52min at 200℃ by heat-ageing oven test when adding 2.5% thermal stabilizer to PVC resin. Compared with antimony tris(isooctyl thiolycollate), the initial thermal stability of antimony pent(isooctyl thioglycollate) is better than that of antimony tris(isooctyl thioglycollate), while the long-term thermal stability time is shorter than that of antimony tris(isooctyl thioglycollate). Meanwhile, the synergism of antimony pent(isooctyl thioglycollate) with calcium stearate was studied, indicating that when the mass ratio of antimony pent(isooctyl thioglycollate) to calcium stearate is (2∶1,) the thermal stability time of PVC is 58min.展开更多
Beef tallow is a byproduct of the slaughter industry. As a consequence, meat producer countries obtain a high amount of this low value-added fatty material. In Uruguay, it is generally used for food purposes or for bi...Beef tallow is a byproduct of the slaughter industry. As a consequence, meat producer countries obtain a high amount of this low value-added fatty material. In Uruguay, it is generally used for food purposes or for biodiesel production. Globally, around half of the beef tallow produced worldwide is used for the manufacturing of food. To the best of our knowledge there are no published studies concerning the stability of beef tallow when exposed to high temperatures. The aim of this work was to study some Uruguayan beef tallow brands and compare its stability with that of the most frequently used frying oils in Uruguay (sunflower high oleic, rice bran and sunflower oil) to assess its suitability for frying. Stability was assessed by the oxidative stability index and thermoxidation in absence of food. Even though beef tallow's inherent stability indicated that it should be highly stable to oxidation, the majority of the analyzed samples exhibited a similar or lower stability than sunflower high oleic. This might be explained by a different composition in pro-oxidants and/or antioxidants between the beef tallows and the oils. According to the thermoxidation assays, which are carried out in similar conditions to those of a frying process, three of the beef tallow samples, sunflower high oleic and rice bran oil would be similarly suitable for frying, while sunflower oil and the other two samples of beef tallow evidenced a lower thermoxidative stability, thus not being recommended for this use.展开更多
Magneli phase titanium sub-oxide conductive ceramic Tin O2n-1 was used as the support for Pt due to its excellent resistance to electrochemical oxidation, and Pt/Tin O2n-1 composites were prepared by the impregnation-...Magneli phase titanium sub-oxide conductive ceramic Tin O2n-1 was used as the support for Pt due to its excellent resistance to electrochemical oxidation, and Pt/Tin O2n-1 composites were prepared by the impregnation-reduction method. The electrochemical stability of Tin O2n-1 was investigated and the results show almost no change in the redox region after oxidation for 20 h at 1.2 V(vs NHE) in 0.5 mol/L H2SO4 aqueous solution. The catalytic activity and stability of the Pt/Tin O2n-1 toward the oxygen reduction reaction(ORR) in 0.5 mol/L H2SO4 solution were investigated through the accelerated aging tests(AAT), and the morphology of the catalysts before and after the AAT was observed by transmission electron microscopy. At the potential of 0.55 V(vs SCE), the specific kinetic current density of the ORR on the Pt/Tin O2n-1 is about 1.5 times that of the Pt/C. The LSV curves for the Pt/C shift negatively obviously with the half-wave potential shifting about 0.02 V after 8000 cycles AAT, while no obvious change takes place for the LSV curves for the Pt/Tin O2n-1. The Pt particles supported on the carbon aggregate obviously, while the morphology of the Pt supported on Tin O2n-1 remains almost unchanged, which contributes to the electrochemical surface area loss of Pt/C being about 2times that of the Pt/Tin O2n-1. The superior catalytic stability of Pt/Tin O2n-1 toward the ORR could be attributed to the excellent stability of the Tin O2n-1 and the electronic interaction between the metals and the support.展开更多
Conventional Pd/γ-A12O3 methane sensors are easily poisoned in a sulfur-containing atmosphere, with a subsequent decrease in sensitivity and the working life of methane sensors. We mainly investigated the effect of n...Conventional Pd/γ-A12O3 methane sensors are easily poisoned in a sulfur-containing atmosphere, with a subsequent decrease in sensitivity and the working life of methane sensors. We mainly investigated the effect of nanotechnology and a cerium co-catalyst on the stability and anti-sulfur performance of methane sensors. In our experiment, an anti-sulfur methane sensor was prepared by immersing cerium-containing γ-alumina nanometer elements into a Pt-Pd bimetallic nanometer catalyst. The experi- ment about the sensitivity and stability performance of different catalytic methane sensors indicate that sensitivity, decreased by catalyst sulfur poisoning, is improved significantly by adding cerium to the vector. As well, the long-term operational stability of methane sensors increased significantly.展开更多
Separation of trivalent minor actinides(MA(ⅡI): Am(ⅡI), Cm(ⅡI)) from fission products(FP) in high-level liquid waste(HLLW) is an important task in advanced nuclear-fuel reprocessing systems. For this purpose, an ad...Separation of trivalent minor actinides(MA(ⅡI): Am(ⅡI), Cm(ⅡI)) from fission products(FP) in high-level liquid waste(HLLW) is an important task in advanced nuclear-fuel reprocessing systems. For this purpose, an advanced aqueous partitioning process based on extraction chromatography method was studied. Because R-BTP extractants(R-BTP: 2,6-bis(5,6-dialkyl-1,2,4-triazin-3-yl)pyridine, R = alkyl group) exhibit high selectivity for MA(ⅡI) over trivalent rare-earth elements(RE(ⅡI)), a novel adsorbent isoHex-BTP/SiO2-P was prepared by impregnating isoHex-BTP extractant into the macroporous SiO2-P support with a mean diameter of 60 μm. The stability of isoHex-BTP/SiO2-P against nitric acid and γ-irradiation was investigated. It was found that isoHex-BTP/SiO2-P adsorbent shows good adsorption affinity to Dy(ⅡI). The hydrolytic and radiolytic stability of isoHex-BTP/SiO2-P adsorbent in 0.01 mol/L HNO3 was fairly promising. However, the adsorption amount Q of Dy(ⅡI) decreased dramatically in 3 mol/L HNO3 with the increase of the absorbed dose and became nearly zero at the absorbed dose over 46 kGy. These results suggest that with the synergetic effect of radiation and acidic hydrolysis, the adsorbent instantly loses its efficacy.展开更多
Using density functional theory (DFT) calculations, we rationally designed metallic nanocatalysts with ternary transition metals for oxygen reduction reactions (ORRs) in fuel cell applications. We surrounded binar...Using density functional theory (DFT) calculations, we rationally designed metallic nanocatalysts with ternary transition metals for oxygen reduction reactions (ORRs) in fuel cell applications. We surrounded binary core-shell nanoparticles with a Pt skin layer. To overcome surface segregation of the core 3-d transition metal, we identified the binary alloy Cu0.76Ni0.24 as having strongly attractive atomic interactions by computationally screening 158 different alloy configurations using energy convex hull theory. The PtskinCu0.76Ni0.24 nanoparticle showed better electrochemical stability than pure Pt nanoparticles -3 nm in size. We propose that the underlying mechanism originates from favorable compressive strain on Pt for ORR catalysis and atomic interactions among the nanoparticle shells for electrochemical stability. Our results will contribute to accurate identification and innovative design of promising nanomaterials for renewable energy systems.展开更多
文摘Low‐temperature CO oxidation is important for both fundamental studies and practical applica‐tions. Supported gold catalysts are generally regarded as the most active catalysts for low‐temperature CO oxidation. The active sites are traditionally believed to be Au nanoclusters or nanoparticles in the size range of 0.5–5 nm. Only in the last few years have single‐atom Au catalysts been proved to be active for CO oxidation. Recent advances in both experimental and theoretical studies on single‐atom Au catalysts unambiguously demonstrated that when dispersed on suitable oxide supports the Au single atoms can be extremely active for CO oxidation. In this mini‐review, recent advances in the development of Au single‐atom catalysts are discussed, with the aim of illus‐trating their unique catalytic features during CO oxidation.
文摘Resurrection plants which are able to quickly reactivate after falling into a period of anabiosis caused by dehydration have been very rare among angiosperms, especially among dicotyledons whose chlorophyll content and chloroplast structure little changed in the course of desiccation, therefore has been called homoiochlorophyllous desiccation-tolerant plants (HDTs). Another type of resurrection angiosperms that lost its chlorophyll dining desiccation is called poikilochlorophyllous desiccation-tolerant plants (PDTs). HDTs have been received more attention because of simplicity of protection mechanism which is much easy to the study and utilization of the desiccation tolerance of resurrection angiosperms. Recent advances in studies of photosynthesis of resurrection angiosperms indicate that photochemical activities are sensitive indicators for the study of physiological state of resurrection angiosperms during desiccation and rehydration. Photochemical activities of resurrection angiosperms are inhibited with loss of water similar to those of general plants, however, the magic thing is that they could reactivate rapidly during rehydration even losing more than 95% water. Up-regulations in xanthophyll cycle and antioxidative systems as well as preservation in integrity and stability of photosynthetic membranes during desiccation may be very important to desiccation tolerance of resurrection angiosperms. The fact that phosphate treatment in rehydration stage also strongly influences resurrection indicated importance of studies on rehydration stages of resurrection angiosperms.
基金supported by the National Natural Science Foundation of China(21173105,21172098)~~
文摘Flower-like 3D CuO microspheres were synthesized and used to photo-catalyze water oxidation under visible light.The structure of the CuO microspheres was characterized by scanning electron microscopy,transmission electron microscopy,infrared,powder X-ray diffraction,electron dispersive spectroscopy,Raman and X-ray photoelectron spectroscopy(XPS).This is the first time that a copper oxide was demonstrated as a photocatalytic water oxidation catalyst under near neutral conditions.The catalytic activity of CuO microspheres in borate buffer shows the best performance with O2 yield of 11.5%.No change in the surface properties of CuO before and after the photocatalytic reaction was seen by XPS,which showed good catalyst stability.A photocatalytic water oxidation reaction mechanism catalyzed by the CuO microspheres was proposed.
基金The Fundamental Research Funds for the Central Universities,the Scientific Innovation Research of College Graduates in Jiangsu Province(No.CXLX12-0105)the Analysis and Test Fund of Southeast University(No.201226)
文摘Colored layered double hydroxides (LDHs) can be synthesized by introducing colored cations such as Fe^3+ and Cr^3 +, which call be used as thermal stabilizers for polyvinyl chloride (PVC). The yellowish Mg/Fe and bluish Mg/Cr LDHs are prepared by the co-precipitation method. The results show that the MgsCr_ CO3 and Mg3Fe_ CO3 colored layered double hydroxides can stabilize PVC for more than 30 min under the thermal aging temperature of 180 ℃. The preparation can use cheap Mg(OH) 2 instead of MgCl2, which produces a much smaller amount of the by-product NH4Cl. It is known that NH4Cl is a cheap fertilizer that is difficult to sell; therefore, the preparation is much greener and more economic than the one using magnesium salt.
基金Project supported by the Postdoctoral Foundation of Central South University
文摘A new type of thermal stabilizer, antimony pent(isooctyl thioglycollate)(Sb(SCH2COOC8H17)5), was synthesized by using antimony trioxide, isooctanol and thioglycolic acid in 2 steps. Firstly, antimony trioxide was oxidized into colloidal antimony peroxide. Then antimony peroxide and isooctyl thioglycollate reacted stoichiometrically for 2 h with the yield of 87%. This compound was used as thermal stabilizer for polyvinyl chloride(PVC). The results show that the thermal stability time is 52min at 200℃ by heat-ageing oven test when adding 2.5% thermal stabilizer to PVC resin. Compared with antimony tris(isooctyl thiolycollate), the initial thermal stability of antimony pent(isooctyl thioglycollate) is better than that of antimony tris(isooctyl thioglycollate), while the long-term thermal stability time is shorter than that of antimony tris(isooctyl thioglycollate). Meanwhile, the synergism of antimony pent(isooctyl thioglycollate) with calcium stearate was studied, indicating that when the mass ratio of antimony pent(isooctyl thioglycollate) to calcium stearate is (2∶1,) the thermal stability time of PVC is 58min.
文摘Beef tallow is a byproduct of the slaughter industry. As a consequence, meat producer countries obtain a high amount of this low value-added fatty material. In Uruguay, it is generally used for food purposes or for biodiesel production. Globally, around half of the beef tallow produced worldwide is used for the manufacturing of food. To the best of our knowledge there are no published studies concerning the stability of beef tallow when exposed to high temperatures. The aim of this work was to study some Uruguayan beef tallow brands and compare its stability with that of the most frequently used frying oils in Uruguay (sunflower high oleic, rice bran and sunflower oil) to assess its suitability for frying. Stability was assessed by the oxidative stability index and thermoxidation in absence of food. Even though beef tallow's inherent stability indicated that it should be highly stable to oxidation, the majority of the analyzed samples exhibited a similar or lower stability than sunflower high oleic. This might be explained by a different composition in pro-oxidants and/or antioxidants between the beef tallows and the oils. According to the thermoxidation assays, which are carried out in similar conditions to those of a frying process, three of the beef tallow samples, sunflower high oleic and rice bran oil would be similarly suitable for frying, while sunflower oil and the other two samples of beef tallow evidenced a lower thermoxidative stability, thus not being recommended for this use.
基金Project(21406273)supported by the National Natural Science Foundation of China
文摘Magneli phase titanium sub-oxide conductive ceramic Tin O2n-1 was used as the support for Pt due to its excellent resistance to electrochemical oxidation, and Pt/Tin O2n-1 composites were prepared by the impregnation-reduction method. The electrochemical stability of Tin O2n-1 was investigated and the results show almost no change in the redox region after oxidation for 20 h at 1.2 V(vs NHE) in 0.5 mol/L H2SO4 aqueous solution. The catalytic activity and stability of the Pt/Tin O2n-1 toward the oxygen reduction reaction(ORR) in 0.5 mol/L H2SO4 solution were investigated through the accelerated aging tests(AAT), and the morphology of the catalysts before and after the AAT was observed by transmission electron microscopy. At the potential of 0.55 V(vs SCE), the specific kinetic current density of the ORR on the Pt/Tin O2n-1 is about 1.5 times that of the Pt/C. The LSV curves for the Pt/C shift negatively obviously with the half-wave potential shifting about 0.02 V after 8000 cycles AAT, while no obvious change takes place for the LSV curves for the Pt/Tin O2n-1. The Pt particles supported on the carbon aggregate obviously, while the morphology of the Pt supported on Tin O2n-1 remains almost unchanged, which contributes to the electrochemical surface area loss of Pt/C being about 2times that of the Pt/Tin O2n-1. The superior catalytic stability of Pt/Tin O2n-1 toward the ORR could be attributed to the excellent stability of the Tin O2n-1 and the electronic interaction between the metals and the support.
基金support for this work, provided by the National Natural Science Foundation of China (No60910005)
文摘Conventional Pd/γ-A12O3 methane sensors are easily poisoned in a sulfur-containing atmosphere, with a subsequent decrease in sensitivity and the working life of methane sensors. We mainly investigated the effect of nanotechnology and a cerium co-catalyst on the stability and anti-sulfur performance of methane sensors. In our experiment, an anti-sulfur methane sensor was prepared by immersing cerium-containing γ-alumina nanometer elements into a Pt-Pd bimetallic nanometer catalyst. The experi- ment about the sensitivity and stability performance of different catalytic methane sensors indicate that sensitivity, decreased by catalyst sulfur poisoning, is improved significantly by adding cerium to the vector. As well, the long-term operational stability of methane sensors increased significantly.
基金supported by the National Natural Science Foundation of China(91126006,11305102)the Research Fund for the Doctoral Program of Higher Education of China(20130073110046)
文摘Separation of trivalent minor actinides(MA(ⅡI): Am(ⅡI), Cm(ⅡI)) from fission products(FP) in high-level liquid waste(HLLW) is an important task in advanced nuclear-fuel reprocessing systems. For this purpose, an advanced aqueous partitioning process based on extraction chromatography method was studied. Because R-BTP extractants(R-BTP: 2,6-bis(5,6-dialkyl-1,2,4-triazin-3-yl)pyridine, R = alkyl group) exhibit high selectivity for MA(ⅡI) over trivalent rare-earth elements(RE(ⅡI)), a novel adsorbent isoHex-BTP/SiO2-P was prepared by impregnating isoHex-BTP extractant into the macroporous SiO2-P support with a mean diameter of 60 μm. The stability of isoHex-BTP/SiO2-P against nitric acid and γ-irradiation was investigated. It was found that isoHex-BTP/SiO2-P adsorbent shows good adsorption affinity to Dy(ⅡI). The hydrolytic and radiolytic stability of isoHex-BTP/SiO2-P adsorbent in 0.01 mol/L HNO3 was fairly promising. However, the adsorption amount Q of Dy(ⅡI) decreased dramatically in 3 mol/L HNO3 with the increase of the absorbed dose and became nearly zero at the absorbed dose over 46 kGy. These results suggest that with the synergetic effect of radiation and acidic hydrolysis, the adsorbent instantly loses its efficacy.
文摘Using density functional theory (DFT) calculations, we rationally designed metallic nanocatalysts with ternary transition metals for oxygen reduction reactions (ORRs) in fuel cell applications. We surrounded binary core-shell nanoparticles with a Pt skin layer. To overcome surface segregation of the core 3-d transition metal, we identified the binary alloy Cu0.76Ni0.24 as having strongly attractive atomic interactions by computationally screening 158 different alloy configurations using energy convex hull theory. The PtskinCu0.76Ni0.24 nanoparticle showed better electrochemical stability than pure Pt nanoparticles -3 nm in size. We propose that the underlying mechanism originates from favorable compressive strain on Pt for ORR catalysis and atomic interactions among the nanoparticle shells for electrochemical stability. Our results will contribute to accurate identification and innovative design of promising nanomaterials for renewable energy systems.