A high pressure energy dispersive X-ray diffraction apparatus on 3W1A bearmline,at BSRF,is described.A ten-Poles permanent magnetic wiggler provided white X-ray beam.The extreme high pressure up to 115GPa has been obt...A high pressure energy dispersive X-ray diffraction apparatus on 3W1A bearmline,at BSRF,is described.A ten-Poles permanent magnetic wiggler provided white X-ray beam.The extreme high pressure up to 115GPa has been obtained by a modified Mao-Bell diamond anvil cell.A motorized loading system with strain sensor can finely control the pressure change.The in situ experimental procedures are described.Some applications are also presented.2001 Elsevier Science B.V.All rights reserved.展开更多
It is the first report of study on the vacuum--evaporated electrochromic WO3 filmusing EXAFS (Extended X-ray Absorption of Fine Structure) .During evaporation, the longrange of WO3 powder-the precursor was vigorously ...It is the first report of study on the vacuum--evaporated electrochromic WO3 filmusing EXAFS (Extended X-ray Absorption of Fine Structure) .During evaporation, the longrange of WO3 powder-the precursor was vigorously d estroyed and decomposed into manyhighly-dispersed dusters. The formed WO3 film, compared to WO3 powder, shortened in W-Odistance and its lattice contracted. When it was cathodically colored in LiClO4/propylenecarbonate solution its lattice Cell further decrea sed. This condusion was also strongly supportedby Raman spectra.展开更多
The compression behaviour of Ni77P23 amorphous alloy is investigated at room temperature in a diamond-anvil cell instrument using in-situ high pressure energy dispersive x-ray diffraction with a synchrotron radiation ...The compression behaviour of Ni77P23 amorphous alloy is investigated at room temperature in a diamond-anvil cell instrument using in-situ high pressure energy dispersive x-ray diffraction with a synchrotron radiation source. The equation of state is determined by fitting the experimental data according to the Birch-Murnaghan equation. It is found that the structure of Ni77P23 amorphous alloy is stable under pressures up to 30.5 GPa. Within the pressure range from zero to the experimental one, the pressure-induced structural relaxation is reversible.展开更多
A new stripping agent N,N-dimethyl-3-oxa-glutaramic Acid (DOGA) was used in TRPO process to simplify the TRPO process. The structures of the complexes of the DOGA with Eu(Ⅲ), Nd(Ⅲ), La(Ⅲ) were characterized with ex...A new stripping agent N,N-dimethyl-3-oxa-glutaramic Acid (DOGA) was used in TRPO process to simplify the TRPO process. The structures of the complexes of the DOGA with Eu(Ⅲ), Nd(Ⅲ), La(Ⅲ) were characterized with extended X-ray absorption fine structure spectroscopy (EXAFS), infrared spectra (IR) and mass spectra (MS). The molecular formula of the complexes of Eu(Ⅲ) and Nd(Ⅲ) is deduced to be M(DOGA)_3, and only La(Ⅲ) can form the complex HM(DOGA)_4 under condition of high consistency of the DOGA. The coordination number of Ln(Ⅲ) in the complexes is 8, and all of coordinated donor atoms are O atoms. For Eu(Ⅲ), Nd(Ⅲ), the coordination numbers of O atom in the first coordination shell is 6 and the average coordination bond lengths of Ln-O are 0 240 nm, 0 244 nm respectively, while the numbers of the second O shell are 2.4, and the average coordination bond lengths of Ln-O are 0 260 nm, 0 262 nm. For La(Ⅲ), the coordination numbers of O atom in the first coordination shell is 6 and the average coordination bond lengths of La-O are 0 258 nm, while the number of O atom in the second coordination shell is 4.4, and the average coordination bond length of La-O is 0 28 nm. The results of IR and MS show that there is no water coordinating with Ln(Ⅲ) in the complexes.展开更多
Environmental photocatalysis is a promising technology for treating antibiotics in wastewater.In this study,a supercritical carbonization method was developed to synthesize a single-atom photocatalyst with a high load...Environmental photocatalysis is a promising technology for treating antibiotics in wastewater.In this study,a supercritical carbonization method was developed to synthesize a single-atom photocatalyst with a high loading of Ni(above 5 wt.%)anchored on a carbonnitrogen-silicate substrate for the efficient photodegradation of a ubiquitous environmental contaminant of tetracycline(TC).The photocatalyst was prepared from an easily obtained metal-biopolymer-inorganic supramolecular hydrogel,followed by supercritical drying and carbonization treatment.The low-temperature(300℃)supercritical ethanol treatment prevents the excessive structural degradation of hydrogel and greatly reduces the metal clustering and aggregation,which contributed to the high Ni loading.Atomic characterizations confirmed that Ni was present at isolated sites and stabilized by Ni-N and Ni-O bonds in a Ni-(N/O)_(6)-C/SiC configuration.A 5%Ni-C-Si catalyst,which performed the best among the studied catalysts,exhibited a wide visible light response with a narrow bandgap of 1.45 eV that could efficiently and repeatedly catalyze the oxidation of TC with a conversion rate of almost 100% within 40 min.The reactive species trapping experiments and electron spin resonance(ESR)tests demonstrated that the h+,and·O_(2)-were mainly responsible for TC degradation.The TC degradation mechanism and possible reaction pathways were provided also.Overall,this study proposed a novel strategy to synthesize a high metal loading singleatom photocatalyst that can efficiently remove TC with high concentrations,and this strategy might be extended for synthesis of other carbon-based single-atom catalysts with valuable properties.展开更多
Al-S batteries are promising next generation energy storage devices due to their high theoretical energy density(1340 Wh kg^(-1)),low cost,and safe operation.However,the electrochemical performance of Al-S batteries s...Al-S batteries are promising next generation energy storage devices due to their high theoretical energy density(1340 Wh kg^(-1)),low cost,and safe operation.However,the electrochemical performance of Al-S batteries suffers poor reversibility owing to slow kinetic processes determined by the difficulty of reversible conversion between Al and S.Here,we proposed a single-atom catalysts comprising Co atoms embedded in a nitrogen-doped graphene(Co NG)as an electrochemical catalyst in the sulfur cathode that renders a reduced discharge-charge voltage hysteresis and improved sulfur utilization in the cathode.The structural and electrochemical analyses suggest that the Co NG facilitated both the formation and oxidation of Al S;during the electrochemical reactions of the sulfur species.Consequently,the Co NG-S composite can deliver a considerably reduced voltage hysteresis of 0.76 V and a reversible specific capacity of 1631 m Ah g^(-1) at 0.2 A g^(-1) with a sulfur utilization of more than 97%.展开更多
UiO-66-NH_(2),an important metal-organic framework,is usually synthesized by solvothermal method and the particle size is generally larger than 200 nm,which limits its catalytic applications in chemical reactions.It i...UiO-66-NH_(2),an important metal-organic framework,is usually synthesized by solvothermal method and the particle size is generally larger than 200 nm,which limits its catalytic applications in chemical reactions.It is very meaningful to produce UiO-66-NH_(2) nanoparticles with ultrasmall size,but remains challenging.Herein,we synthesized UiO-66-NH_(2) nanoparticles in size of 8-15 nm that are immobilized on g-C_(3)N_(4)nanosheets.Compared with the UiO-66-NH_(2) synthesized by the traditional solvothermal method(>200 nm),the ultra-small UiO-66-NH_(2) nanoparticles immobilized on g-C_(3)N_(4)have more unsaturated coordination positions and increased Lewis acidity.Owing to these combined advantages,the ultra-small UiO-66-NH_(2)nanoparticles exhibit greatly improved catalytic activity for Meerwein-Ponndorf-Verley reaction than larger UiO-66-NH_(2)particles.展开更多
Cerium oxide nanoparticles coated by sodium bis(2-ethylexyl) sulphosuccinate(AOT) were prepared by using a microemulsion method.Transmission electron microscopy revealed an average particle siae of 2-3nm.X-ray diffrac...Cerium oxide nanoparticles coated by sodium bis(2-ethylexyl) sulphosuccinate(AOT) were prepared by using a microemulsion method.Transmission electron microscopy revealed an average particle siae of 2-3nm.X-ray diffraction showed that the cerium oxide nanoparticles retain the CeF2-type cubic structures like the bulk crystal.The intermediate valence offormally tetravalent compounds had been detected by x-ray-absorption near-edge structetravalent compounds had been detected by x-ray-absorption near-dege structure(XANES) spectra of Ce LIII absorption in bulk CeO2 and the cerium oxide nanoparticles.Two well resoved white lines can be assigned to the electron configurations of 4f^0L and 4f^1L,respectively,where L denotes a ligand hole.At the same time,the cerium oxide nanoparticles also showed the structural featres of trivalent compounds,in comparison to the trivalent Ce(NO3)3·6H2O.Fuor Lorentzian functions and two arctan functions were used to fit the normalized XANES spectra.The extended x-ray-absorption fine-structure(EXAFS) technique was used to probe the local atomic structures around the absorber Ce.The multielectrorn excitation effect on the EXAFS spectra was eliminated.A cor-shell model was used to deduce the near-neighbour structural parameters around cerium.Bulk CeO2 with eight oxygen atoms located at 2.343A was used as the reference sample to extract the backscattering amplitude and phase shift of the Ce-O bond.One half of the atome locate at the core part with the CeF2-type cubic structures(eight oxyens at 2.343A around Ce),the other half of the atoms are amorphous phase located in the shell part (surface of the nanoparticles) with approximately Ce2O3 structural features (averageed seven oxygens at 2.50A around Ce).展开更多
Rational heterostructure-design in electrocatalysts represents a promising approach toward high performance in the electrocatalytic hydrogen evolution reaction(HER).In specific,optimizing the H adsorption behavior at ...Rational heterostructure-design in electrocatalysts represents a promising approach toward high performance in the electrocatalytic hydrogen evolution reaction(HER).In specific,optimizing the H adsorption behavior at the surface/interface of heterostructure is of key importance to improve the catalytic performance.Herein,we demonstrate the construction of a heterostructure from a well-defined oxygenbridged Co/Mo heterometallic zeolitic imidazolate framework(MOZ) as an efficient electrocatalyst for HER.The optimized hybrid exhibits high catalytic activity and stability in electrolytes with a wide pH range.Detailed XPS,XAS and theoretical studies reveal that the regulation of metal species can tailor the lattice of Mo_(2)C within the hybrid and induce the formation of defect sites,which could not only induce surface charge transfer between the atoms and provide an additional active site,but also affect the H adsorption behavior at the interface of a heterostructure.This work provides an effective strategy to design a heterostructure with tailored active sites for energy conversion.展开更多
Ductal carcinoma in-situ (DCIS) has been visualized by 2D XDFI (X-ray dark-field imaging) and further by a 3D X-ray CT, and the data was acquired by the X-ray optics DEI (diffraction-enhanced imaging). A newly made al...Ductal carcinoma in-situ (DCIS) has been visualized by 2D XDFI (X-ray dark-field imaging) and further by a 3D X-ray CT, and the data was acquired by the X-ray optics DEI (diffraction-enhanced imaging). A newly made algorithm was used for CT. Data of 900 projections with interval of 0.2 degrees were used. Ductus lactiferi, microcalci-fication in a 3D form have been clearly visible. The spatial resolution available was approximately 30μm.展开更多
The compression properties of Zr41Ti14Cu12.aNi10Be22.5, Zr44.4Nb7Cu13.5Ni10.8Be24.3 bulk metallic glasses and Ni77P23 binary amorphous alloy are investigated at room temperature up to 24 GPa, 39 GPa and 30.5 GPa, resp...The compression properties of Zr41Ti14Cu12.aNi10Be22.5, Zr44.4Nb7Cu13.5Ni10.8Be24.3 bulk metallic glasses and Ni77P23 binary amorphous alloy are investigated at room temperature up to 24 GPa, 39 GPa and 30.5 GPa, respectively, using in-situ high pressure energy dispersive x-ray diffraction with a synchrotron radiation source. The pressure-volume relationship of Ni77P23 amorphous alloy is consistent well with the second order BirchMurnaghan （B-M） equation within the experimental pressure range. However, under higher pressure, the experimental data of Zr-based specimens deviate from the B-M equation. Compare to the binary amorphous alloy less excess free volume existing in the bulk metallic glass and multi-component atomic configuration results in a two-stage relationship between compressibility and pressure.展开更多
文摘A high pressure energy dispersive X-ray diffraction apparatus on 3W1A bearmline,at BSRF,is described.A ten-Poles permanent magnetic wiggler provided white X-ray beam.The extreme high pressure up to 115GPa has been obtained by a modified Mao-Bell diamond anvil cell.A motorized loading system with strain sensor can finely control the pressure change.The in situ experimental procedures are described.Some applications are also presented.2001 Elsevier Science B.V.All rights reserved.
文摘It is the first report of study on the vacuum--evaporated electrochromic WO3 filmusing EXAFS (Extended X-ray Absorption of Fine Structure) .During evaporation, the longrange of WO3 powder-the precursor was vigorously d estroyed and decomposed into manyhighly-dispersed dusters. The formed WO3 film, compared to WO3 powder, shortened in W-Odistance and its lattice contracted. When it was cathodically colored in LiClO4/propylenecarbonate solution its lattice Cell further decrea sed. This condusion was also strongly supportedby Raman spectra.
基金Supported by the National Natural Science Foundation of China under Grant No 50325103,Hebei Natural Science Foundation under Grant No 503278and the Scientific Research Foundation for the Returned 0verseas Chinese Scholars, State Education Ministry of China.
文摘The compression behaviour of Ni77P23 amorphous alloy is investigated at room temperature in a diamond-anvil cell instrument using in-situ high pressure energy dispersive x-ray diffraction with a synchrotron radiation source. The equation of state is determined by fitting the experimental data according to the Birch-Murnaghan equation. It is found that the structure of Ni77P23 amorphous alloy is stable under pressures up to 30.5 GPa. Within the pressure range from zero to the experimental one, the pressure-induced structural relaxation is reversible.
基金Project supported by the China National"863"Program
文摘A new stripping agent N,N-dimethyl-3-oxa-glutaramic Acid (DOGA) was used in TRPO process to simplify the TRPO process. The structures of the complexes of the DOGA with Eu(Ⅲ), Nd(Ⅲ), La(Ⅲ) were characterized with extended X-ray absorption fine structure spectroscopy (EXAFS), infrared spectra (IR) and mass spectra (MS). The molecular formula of the complexes of Eu(Ⅲ) and Nd(Ⅲ) is deduced to be M(DOGA)_3, and only La(Ⅲ) can form the complex HM(DOGA)_4 under condition of high consistency of the DOGA. The coordination number of Ln(Ⅲ) in the complexes is 8, and all of coordinated donor atoms are O atoms. For Eu(Ⅲ), Nd(Ⅲ), the coordination numbers of O atom in the first coordination shell is 6 and the average coordination bond lengths of Ln-O are 0 240 nm, 0 244 nm respectively, while the numbers of the second O shell are 2.4, and the average coordination bond lengths of Ln-O are 0 260 nm, 0 262 nm. For La(Ⅲ), the coordination numbers of O atom in the first coordination shell is 6 and the average coordination bond lengths of La-O are 0 258 nm, while the number of O atom in the second coordination shell is 4.4, and the average coordination bond length of La-O is 0 28 nm. The results of IR and MS show that there is no water coordinating with Ln(Ⅲ) in the complexes.
基金supported by the National Key Research and Development Program(No.2019YFC1803903)the Program for Guangdong Introducing Innovative and Entrepreneurial Teams(No.2017ZT07Z479)+1 种基金China Postdoctoral Science Foundation(No.2021M701561)the National Natural Science Foundation of China(No.42007318)。
文摘Environmental photocatalysis is a promising technology for treating antibiotics in wastewater.In this study,a supercritical carbonization method was developed to synthesize a single-atom photocatalyst with a high loading of Ni(above 5 wt.%)anchored on a carbonnitrogen-silicate substrate for the efficient photodegradation of a ubiquitous environmental contaminant of tetracycline(TC).The photocatalyst was prepared from an easily obtained metal-biopolymer-inorganic supramolecular hydrogel,followed by supercritical drying and carbonization treatment.The low-temperature(300℃)supercritical ethanol treatment prevents the excessive structural degradation of hydrogel and greatly reduces the metal clustering and aggregation,which contributed to the high Ni loading.Atomic characterizations confirmed that Ni was present at isolated sites and stabilized by Ni-N and Ni-O bonds in a Ni-(N/O)_(6)-C/SiC configuration.A 5%Ni-C-Si catalyst,which performed the best among the studied catalysts,exhibited a wide visible light response with a narrow bandgap of 1.45 eV that could efficiently and repeatedly catalyze the oxidation of TC with a conversion rate of almost 100% within 40 min.The reactive species trapping experiments and electron spin resonance(ESR)tests demonstrated that the h+,and·O_(2)-were mainly responsible for TC degradation.The TC degradation mechanism and possible reaction pathways were provided also.Overall,this study proposed a novel strategy to synthesize a high metal loading singleatom photocatalyst that can efficiently remove TC with high concentrations,and this strategy might be extended for synthesis of other carbon-based single-atom catalysts with valuable properties.
基金funding support from the Natural Science Foundation of China(U2032202,21975243 and 51672262)the National Program for Support of Topnotch Young Professional and the Fundamental Research Funds for the Central Universities(WK2060000026)。
文摘Al-S batteries are promising next generation energy storage devices due to their high theoretical energy density(1340 Wh kg^(-1)),low cost,and safe operation.However,the electrochemical performance of Al-S batteries suffers poor reversibility owing to slow kinetic processes determined by the difficulty of reversible conversion between Al and S.Here,we proposed a single-atom catalysts comprising Co atoms embedded in a nitrogen-doped graphene(Co NG)as an electrochemical catalyst in the sulfur cathode that renders a reduced discharge-charge voltage hysteresis and improved sulfur utilization in the cathode.The structural and electrochemical analyses suggest that the Co NG facilitated both the formation and oxidation of Al S;during the electrochemical reactions of the sulfur species.Consequently,the Co NG-S composite can deliver a considerably reduced voltage hysteresis of 0.76 V and a reversible specific capacity of 1631 m Ah g^(-1) at 0.2 A g^(-1) with a sulfur utilization of more than 97%.
基金financial supports from National Natural Science Foundation of China(21525316,21673254)Ministry of Science and Technology of China(2017YFA0403003)+1 种基金Chinese Academy of Sciences(QYZDYSSW-SLH013)Beijing Municipal Science&Technology Commission(Z191100007219009)。
文摘UiO-66-NH_(2),an important metal-organic framework,is usually synthesized by solvothermal method and the particle size is generally larger than 200 nm,which limits its catalytic applications in chemical reactions.It is very meaningful to produce UiO-66-NH_(2) nanoparticles with ultrasmall size,but remains challenging.Herein,we synthesized UiO-66-NH_(2) nanoparticles in size of 8-15 nm that are immobilized on g-C_(3)N_(4)nanosheets.Compared with the UiO-66-NH_(2) synthesized by the traditional solvothermal method(>200 nm),the ultra-small UiO-66-NH_(2) nanoparticles immobilized on g-C_(3)N_(4)have more unsaturated coordination positions and increased Lewis acidity.Owing to these combined advantages,the ultra-small UiO-66-NH_(2)nanoparticles exhibit greatly improved catalytic activity for Meerwein-Ponndorf-Verley reaction than larger UiO-66-NH_(2)particles.
文摘Cerium oxide nanoparticles coated by sodium bis(2-ethylexyl) sulphosuccinate(AOT) were prepared by using a microemulsion method.Transmission electron microscopy revealed an average particle siae of 2-3nm.X-ray diffraction showed that the cerium oxide nanoparticles retain the CeF2-type cubic structures like the bulk crystal.The intermediate valence offormally tetravalent compounds had been detected by x-ray-absorption near-edge structetravalent compounds had been detected by x-ray-absorption near-dege structure(XANES) spectra of Ce LIII absorption in bulk CeO2 and the cerium oxide nanoparticles.Two well resoved white lines can be assigned to the electron configurations of 4f^0L and 4f^1L,respectively,where L denotes a ligand hole.At the same time,the cerium oxide nanoparticles also showed the structural featres of trivalent compounds,in comparison to the trivalent Ce(NO3)3·6H2O.Fuor Lorentzian functions and two arctan functions were used to fit the normalized XANES spectra.The extended x-ray-absorption fine-structure(EXAFS) technique was used to probe the local atomic structures around the absorber Ce.The multielectrorn excitation effect on the EXAFS spectra was eliminated.A cor-shell model was used to deduce the near-neighbour structural parameters around cerium.Bulk CeO2 with eight oxygen atoms located at 2.343A was used as the reference sample to extract the backscattering amplitude and phase shift of the Ce-O bond.One half of the atome locate at the core part with the CeF2-type cubic structures(eight oxyens at 2.343A around Ce),the other half of the atoms are amorphous phase located in the shell part (surface of the nanoparticles) with approximately Ce2O3 structural features (averageed seven oxygens at 2.50A around Ce).
基金the financial support from the National Natural Science Foundation of China(Nos.51772291,21673238 and 21773242)Fundamental Research Funds for the Central Universities(No.19lgpy117)+1 种基金China Postdoctoral Science Foundation(No.2019M653176)the Strategic Priority Research Program of the Chinese Academy of Sciences(No.XDB20000000)。
文摘Rational heterostructure-design in electrocatalysts represents a promising approach toward high performance in the electrocatalytic hydrogen evolution reaction(HER).In specific,optimizing the H adsorption behavior at the surface/interface of heterostructure is of key importance to improve the catalytic performance.Herein,we demonstrate the construction of a heterostructure from a well-defined oxygenbridged Co/Mo heterometallic zeolitic imidazolate framework(MOZ) as an efficient electrocatalyst for HER.The optimized hybrid exhibits high catalytic activity and stability in electrolytes with a wide pH range.Detailed XPS,XAS and theoretical studies reveal that the regulation of metal species can tailor the lattice of Mo_(2)C within the hybrid and induce the formation of defect sites,which could not only induce surface charge transfer between the atoms and provide an additional active site,but also affect the H adsorption behavior at the interface of a heterostructure.This work provides an effective strategy to design a heterostructure with tailored active sites for energy conversion.
文摘Ductal carcinoma in-situ (DCIS) has been visualized by 2D XDFI (X-ray dark-field imaging) and further by a 3D X-ray CT, and the data was acquired by the X-ray optics DEI (diffraction-enhanced imaging). A newly made algorithm was used for CT. Data of 900 projections with interval of 0.2 degrees were used. Ductus lactiferi, microcalci-fication in a 3D form have been clearly visible. The spatial resolution available was approximately 30μm.
基金Supported by the National Natural Science Foundation of China under Grant No 50325103, the Natural Science Foundation of Hebei Province under Grant No A2007000296, and the National Key Basic Research Special Foundation （NKBRSF） of China under Grant No 2006CB605201.
文摘The compression properties of Zr41Ti14Cu12.aNi10Be22.5, Zr44.4Nb7Cu13.5Ni10.8Be24.3 bulk metallic glasses and Ni77P23 binary amorphous alloy are investigated at room temperature up to 24 GPa, 39 GPa and 30.5 GPa, respectively, using in-situ high pressure energy dispersive x-ray diffraction with a synchrotron radiation source. The pressure-volume relationship of Ni77P23 amorphous alloy is consistent well with the second order BirchMurnaghan （B-M） equation within the experimental pressure range. However, under higher pressure, the experimental data of Zr-based specimens deviate from the B-M equation. Compare to the binary amorphous alloy less excess free volume existing in the bulk metallic glass and multi-component atomic configuration results in a two-stage relationship between compressibility and pressure.
