A systematic investigation of oxidation on a superconductive Fe Te_(0.5)Se_(0.5)thin film,which was grown on Nb-doped SrTiO_3(001) by pulsed laser deposition,has been carried out.The sample was exposed to ambien...A systematic investigation of oxidation on a superconductive Fe Te_(0.5)Se_(0.5)thin film,which was grown on Nb-doped SrTiO_3(001) by pulsed laser deposition,has been carried out.The sample was exposed to ambient air for one month for oxidation.Macroscopically,the exposed specimen lost its superconductivity due to oxidation.The specimen was subjected to in situ synchrotron radiation photoelectron spectroscopy(PES) and x-ray absorption spectroscopy(XAS) measurements following cycles of annealing and argon ion etching treatments to unravel what happened in the electronic structure and composition after exposure to air.By the spectroscopic measurements,we found that the as-grown FeTe_(0.5)Se_(0.5)superconductive thin film experienced an element selective substitution reaction.The oxidation preferentially proceeds through pumping out the Te and forming Fe–O bonds by O substitution of Te.In addition,our results certify that in situ vacuum annealing and low-energy argon ion etching methods combined with spectroscopy are suitable for depth element and valence analysis of layered structure superconductor materials.展开更多
Rare earth elements(REEs) are critical materials and provide significant values to national security,energy production, environmental protection and economic growth. The supply of REEs in U.S. solely relies on impor...Rare earth elements(REEs) are critical materials and provide significant values to national security,energy production, environmental protection and economic growth. The supply of REEs in U.S. solely relies on import as domestic production of REEs was ceased because of the environmental concerns during mining and lack of competitiveness. Nonetheless, unconventional REEs-containing resources,including produced water. acid mine drainage, and coal and coal byproducts(C&CBs) contain significant amounts of REEs. However, the concentrations of REEs in these resources are several orders of magnitude lower than that of REEs ores. Thus, extraction of REEs from these materials is challenging. Here we report REEs extraction with environmentally friendly method that successfully concentrated REEs from312 ppm in fly ash to 99.4% in the final product. Especially, the five critically important REEs(Dy, Eu, Nd.Tb. and Y) account for up to ~63% of the total weight of all REEs in the final 99.4%-purity product. Coal fly ash is one of the major solid coal utilization byproducts, representing great potential resources for REEs extraction. Extraction of REEs from these unconventional resources could be the way to secure domestic supply of these critical materials.展开更多
Inductively coupled plasma mass spectrometry (ICP-MS) is the most commonly used technique to deter- mine the abundances of trace elements in a wide range of geological materials. However, incomplete sample digestion...Inductively coupled plasma mass spectrometry (ICP-MS) is the most commonly used technique to deter- mine the abundances of trace elements in a wide range of geological materials. However, incomplete sample digestion, isobaric interferences and instrumental drift remain obvious problems that must be overcome in order to obtain precise and accurate results, For this reason, we have done many experi- ments and developed a set of simple, cost-effective and practical methods widely applicable for precise and rapid determination of trace element abundances in geological materials using ICP-MS. Commonly used high-pressure digestion technique is indeed effective in decomposing refractory phases, but this inevitably produces fluoride complexes that create new problems. We demonstrate that the fluoride complexes formed during high-pressure digestion can be readily re-dissolved using high-pressure vessel at 190 ℃ for only 2 h for 50 mg sample. In the case of isobaric interferences, although oxide (e.g., MO^+/M^+) and hydroxide (e.g., MO^+/M^+) productivity is variable between runs, the (MO^+/M^+)/(CeO^+/Ce^+) and (MOH^+/M^+)/(CeO^+/Ce^+) ratios remain constant, making isobaric interference correction for all other elements of interest straightforward, for which we provide an easy-to-use off-line procedure. We also show that mass-time-intensity drift curve is smooth as recognized previously, for which the correction can be readily done by analyzing a quality-control (QC) solution and using off-line Excel VBA procedure without internal standards. With these methods, we can produce data in reasonable agreement with rec- ommended values of international rock reference standards with a relative error of 〈8% and precision generally better than 5%. Importantly, compared to the widely used analytical practice, we can effectively save 〉60% of time (e.g., 〈24 h vs. 〉60 h).展开更多
The Cr-/Si-modified Ni Al Hf coatings were produced on single-crystal(SC) superalloy N5 by electron beam physical vapor deposition(EB-PVD). The cyclic oxidation behavior of the coatings at 1100 °C was investi...The Cr-/Si-modified Ni Al Hf coatings were produced on single-crystal(SC) superalloy N5 by electron beam physical vapor deposition(EB-PVD). The cyclic oxidation behavior of the coatings at 1100 °C was investigated. The microstructures of the oxide scales grown on the coatings were characterized by scanning electron microscope(SEM) with energy-dispersive X-ray spectrum(EDX),electron probe micro-analyzer(EPMA) and X-ray diffraction(XRD). The effects of Cr and Si on the cyclic oxidation behavior of the Ni Al Hf coatings were discussed. The addition of Si to the Ni Al Hf Cr coating not only reduces the oxidation rate but also enhances the oxide scale adherence.Owing to the addition of Si in the coating, the segregation of Cr and Mo beneath the oxide scale is effectively avoided,which contributes to enhancing oxide scale adherence.展开更多
A series of MgAl-layered double oxides(LDO) doped with different rare-earth elements(Y, La, and Ce)were synthesized by the calcination of Mg-Al layered double hydroxides, and Ru, which were used to prepare ammonia...A series of MgAl-layered double oxides(LDO) doped with different rare-earth elements(Y, La, and Ce)were synthesized by the calcination of Mg-Al layered double hydroxides, and Ru, which were used to prepare ammonia synthesis catalysts. The as-obtained oxides and catalysts were characterized by XRD,TEM, TPD, TPR and XPS to understand their catalytic performances in ammonia synthesis. The H_2-TPR and HRTEM studies reveal that Ru/Y-LDO catalyst possesses more active Ru metal and small particle size.The XPS demonstrates that the electronic interaction between Y and Ru metals is stronger, which can be tentatively explained by most of Y inserted into the hydrotalcites structure. CO_2-TPD demonstrates that Ru/Y-LDO catalyst shows stronger basic site densities than catalysts doped with Ce and La. Higher activity of the Ru/Y-LDO catalyst can be attributed to smaller particle size, more active metal(Ru) and strong Ru-support interaction.展开更多
基金Project supported by the Chinese Academy of Sciences(Grant No.1G2009312311750101)the National Natural Science Foundation of China(Grant Nos.11375228,11204303,and U1332105)
文摘A systematic investigation of oxidation on a superconductive Fe Te_(0.5)Se_(0.5)thin film,which was grown on Nb-doped SrTiO_3(001) by pulsed laser deposition,has been carried out.The sample was exposed to ambient air for one month for oxidation.Macroscopically,the exposed specimen lost its superconductivity due to oxidation.The specimen was subjected to in situ synchrotron radiation photoelectron spectroscopy(PES) and x-ray absorption spectroscopy(XAS) measurements following cycles of annealing and argon ion etching treatments to unravel what happened in the electronic structure and composition after exposure to air.By the spectroscopic measurements,we found that the as-grown FeTe_(0.5)Se_(0.5)superconductive thin film experienced an element selective substitution reaction.The oxidation preferentially proceeds through pumping out the Te and forming Fe–O bonds by O substitution of Te.In addition,our results certify that in situ vacuum annealing and low-energy argon ion etching methods combined with spectroscopy are suitable for depth element and valence analysis of layered structure superconductor materials.
基金Project supported by the Department of Energy through"Rare Earth Elements From Coal and Coal By-Products"program(DE-FE00027069)
文摘Rare earth elements(REEs) are critical materials and provide significant values to national security,energy production, environmental protection and economic growth. The supply of REEs in U.S. solely relies on import as domestic production of REEs was ceased because of the environmental concerns during mining and lack of competitiveness. Nonetheless, unconventional REEs-containing resources,including produced water. acid mine drainage, and coal and coal byproducts(C&CBs) contain significant amounts of REEs. However, the concentrations of REEs in these resources are several orders of magnitude lower than that of REEs ores. Thus, extraction of REEs from these materials is challenging. Here we report REEs extraction with environmentally friendly method that successfully concentrated REEs from312 ppm in fly ash to 99.4% in the final product. Especially, the five critically important REEs(Dy, Eu, Nd.Tb. and Y) account for up to ~63% of the total weight of all REEs in the final 99.4%-purity product. Coal fly ash is one of the major solid coal utilization byproducts, representing great potential resources for REEs extraction. Extraction of REEs from these unconventional resources could be the way to secure domestic supply of these critical materials.
基金supported by National Natural Science Foundation of China(41130314 and 41630968)Chinese Academy of Sciences Innovation Grant(Y42217101L)+1 种基金Qingdao National Laboratory for Marine Science and Technology(2015ASKJ03)Marine Geological Process and Environment(U1606401)
文摘Inductively coupled plasma mass spectrometry (ICP-MS) is the most commonly used technique to deter- mine the abundances of trace elements in a wide range of geological materials. However, incomplete sample digestion, isobaric interferences and instrumental drift remain obvious problems that must be overcome in order to obtain precise and accurate results, For this reason, we have done many experi- ments and developed a set of simple, cost-effective and practical methods widely applicable for precise and rapid determination of trace element abundances in geological materials using ICP-MS. Commonly used high-pressure digestion technique is indeed effective in decomposing refractory phases, but this inevitably produces fluoride complexes that create new problems. We demonstrate that the fluoride complexes formed during high-pressure digestion can be readily re-dissolved using high-pressure vessel at 190 ℃ for only 2 h for 50 mg sample. In the case of isobaric interferences, although oxide (e.g., MO^+/M^+) and hydroxide (e.g., MO^+/M^+) productivity is variable between runs, the (MO^+/M^+)/(CeO^+/Ce^+) and (MOH^+/M^+)/(CeO^+/Ce^+) ratios remain constant, making isobaric interference correction for all other elements of interest straightforward, for which we provide an easy-to-use off-line procedure. We also show that mass-time-intensity drift curve is smooth as recognized previously, for which the correction can be readily done by analyzing a quality-control (QC) solution and using off-line Excel VBA procedure without internal standards. With these methods, we can produce data in reasonable agreement with rec- ommended values of international rock reference standards with a relative error of 〈8% and precision generally better than 5%. Importantly, compared to the widely used analytical practice, we can effectively save 〉60% of time (e.g., 〈24 h vs. 〉60 h).
基金financially supported by the National Basic Research Program of China (Nos. 2012CB625100 and 2010CB631200)the National Natural Science Foundation of China (No. 51231001)
文摘The Cr-/Si-modified Ni Al Hf coatings were produced on single-crystal(SC) superalloy N5 by electron beam physical vapor deposition(EB-PVD). The cyclic oxidation behavior of the coatings at 1100 °C was investigated. The microstructures of the oxide scales grown on the coatings were characterized by scanning electron microscope(SEM) with energy-dispersive X-ray spectrum(EDX),electron probe micro-analyzer(EPMA) and X-ray diffraction(XRD). The effects of Cr and Si on the cyclic oxidation behavior of the Ni Al Hf coatings were discussed. The addition of Si to the Ni Al Hf Cr coating not only reduces the oxidation rate but also enhances the oxide scale adherence.Owing to the addition of Si in the coating, the segregation of Cr and Mo beneath the oxide scale is effectively avoided,which contributes to enhancing oxide scale adherence.
基金Project supported by the Natural Science Foundation of Fujian Province(2014J01043)the National Natural Science Foundation of China(21203028)PetroChina Innovation Foundation(2016D-5007-0504)
文摘A series of MgAl-layered double oxides(LDO) doped with different rare-earth elements(Y, La, and Ce)were synthesized by the calcination of Mg-Al layered double hydroxides, and Ru, which were used to prepare ammonia synthesis catalysts. The as-obtained oxides and catalysts were characterized by XRD,TEM, TPD, TPR and XPS to understand their catalytic performances in ammonia synthesis. The H_2-TPR and HRTEM studies reveal that Ru/Y-LDO catalyst possesses more active Ru metal and small particle size.The XPS demonstrates that the electronic interaction between Y and Ru metals is stronger, which can be tentatively explained by most of Y inserted into the hydrotalcites structure. CO_2-TPD demonstrates that Ru/Y-LDO catalyst shows stronger basic site densities than catalysts doped with Ce and La. Higher activity of the Ru/Y-LDO catalyst can be attributed to smaller particle size, more active metal(Ru) and strong Ru-support interaction.