Supported gold nanoparticle catalysts show extraordinarily high activity in many reactions. While the relative poor thermal stability of Au nanoparticles against sintering at elevated temperatures severely limits thei...Supported gold nanoparticle catalysts show extraordinarily high activity in many reactions. While the relative poor thermal stability of Au nanoparticles against sintering at elevated temperatures severely limits their practical applications. Here atomic layer deposition (ALD) of TiO2 and Al2O3 was performed to deposit an Au/TiO2 catalyst with precise thickness con-trol, and the thermal stability was investigated. We surprisingly found that sub-nanometer-thick Al2O3 overcoat can su ciently inhibit the aggregation of Au particles up to 600 C in oxygen. On the other hand, the enhancement of Au nanoparticle stability by TiO2 overcoat is very limited. Di use reffectance infrared Fourier transform spectroscopy (DRIFTS) of CO chemisorption and X-ray photoelectron spectroscopy measurements both con rmed the ALD overcoat on Au particles surface and suggested that the presence of TiO2 and Al2O3 ALD overcoat on Au nanoparticles does not considerably change the electronic properties of Au nanoparticles. The catalytic activities of the Al2O3 overcoated Au/TiO2 catalysts in CO oxidation increased as increasing calcination temperature, which suggests that the embed-ded Au nanoparticles become more accessible for catalytic function after high temperature treatment, consistent with our DRIFTS CO chemisorption results.展开更多
We study behavior of an atomic wave packet in a circularly polarized electromagnetic wave, and particularly calculate the atomic inversion of the wave packet. A general method of calculation is presented. The results ...We study behavior of an atomic wave packet in a circularly polarized electromagnetic wave, and particularly calculate the atomic inversion of the wave packet. A general method of calculation is presented. The results are interesting. For example, if the wave packet is very narrow or/and the interaction is very strong, no matter the atom is initially in its ground state or excited state, the atomic inversion approaches zero as time approaches infinity. If the atom is initially in its ground state and excited state with the probability 1/2 respectively, and if the momentum density is an even function, then the atomic inversion equals zero at any time.展开更多
Hydrogen generation from formic acid (FA) has received significant attention. The challenge is to obtain a highly active catalyst under mild conditions for practical applications. Here atomic layer deposition (ALD...Hydrogen generation from formic acid (FA) has received significant attention. The challenge is to obtain a highly active catalyst under mild conditions for practical applications. Here atomic layer deposition (ALD) of FeOx was performed to deposit an ultrathin oxide coating layer to a Pd/C catalyst, therein the FeOx coverage was precisely controlled by ALD cycles. Transmission electron microscopy and powder X-ray diffraction measurements suggest that the FeOx coating layer improved the thermal stability of Pd nanoparticles (NPs). X-ray photoelectron spectroscopy measurement showed that deposition of FeOx on the Pd NPs caused a positive shift of Pd3d binding energy. In the FA dehydrogenation reaction, the ultrathin FeOx layer on the Pd/C could considerably improve the catalytic activity, and Pd/C coated with 8 cycles of FeOx showed an optimized activity with turnover frequency being about 2 times higher than the uncoated one. shape as a function of the number of FeOx ALD The improved activities were in a volcanocycles, indicating the coverage of FeOx is critical for the optimized activity. In summary, simultaneous improvements of activity and thermal stability of Pd/C catalyst by ultra-thin FeOx overlayer suggest to be an effective way to design active catalysts for the FA dehydrogenation reaction.展开更多
Two dimensional Fourier transforrn electronic spectroscopy (2DES) in the visible region enables direct observation of complex dynamics of molecules including quantum coherence in the condensed phase. This review aim...Two dimensional Fourier transforrn electronic spectroscopy (2DES) in the visible region enables direct observation of complex dynamics of molecules including quantum coherence in the condensed phase. This review aims to provide a bridge between the principles and intuitive physical description of 2DES for tutorial purpose. Special emphasis is laid upon how 2DES circumvents the restrictions from both uncertainty principle and the wave-packet collapse during the coherent detection, leading to the successful detection of the coherence in terms of energy difference between the eigenstates showing as the quantum beats; then upon the possible mixing among the pure electronic transition, single-rnode and multi-mode coupled vibronic transition leading to the observed beating phenomena. Finally, recent ad- vances in experimentally distinguishing between the electronic coherence and the vibrational coherence are briefly discussed.展开更多
Photo dissociation dynamics of diatomic molecular ion HBr+ interacting with ultra fast laser pulses of different envelop function has been presented both in zero and non zero temperature environment. The calculations...Photo dissociation dynamics of diatomic molecular ion HBr+ interacting with ultra fast laser pulses of different envelop function has been presented both in zero and non zero temperature environment. The calculations pertain primarily to the ground electronic state of the molecular ion HBr+. The used potential of HBr+ is calibrated with the help of the ab initio theoretical calculation at the CCSD/6-311++G(3df, 2pd) level and then fitted with appropriate Morse parameters. The numerical bound states vibrational eigenvalues obtained by the time independent Fourier Grid Hamiltonian method have been compared with analytical values of the fitted Morse potential. The effect of temperature, pulse envelops function, and light intensity on the dissociation process has been explored.展开更多
In contrast to the toxic inorganic forms of selenium to life at very low concentrations, the organic-selenium compounds are of considerable interest and several of them play essential roles in cell biochemistry and nu...In contrast to the toxic inorganic forms of selenium to life at very low concentrations, the organic-selenium compounds are of considerable interest and several of them play essential roles in cell biochemistry and nutritional science. Se-yeast (Selenium-enriched yeast) is a common form of selenium used to supplement dietary intake of this important trace mineral. In the present study, we tried to prepare an organic selenocystine using locally isolated bread yeast (Saccharomyces cerevisiae). A novel locally prepared date extract media enriched by addition of 0.2% KH2PO4 (potassium phosphate), 0.6% ammonium sulfate was adopted as alternative culture media. Differences concentrations of selenium salt (30, 60, 120 and 240 lag/mL) were added to the yeast culture media. While the best concentration of selenium added was 30Bg/mL, it achieved optimal conditions for the growth of yeast and the production of red yeast growth identical to the standard. The products (organic selenocystine) were analyzed by HPLC (High Performance Liquid Chromatography) and AAS (Atomic Absorption Spectrophotometer) comparing with authentic standard obtained from Sigma. Results confirmed the formation of similar selenocystine products.展开更多
文摘Supported gold nanoparticle catalysts show extraordinarily high activity in many reactions. While the relative poor thermal stability of Au nanoparticles against sintering at elevated temperatures severely limits their practical applications. Here atomic layer deposition (ALD) of TiO2 and Al2O3 was performed to deposit an Au/TiO2 catalyst with precise thickness con-trol, and the thermal stability was investigated. We surprisingly found that sub-nanometer-thick Al2O3 overcoat can su ciently inhibit the aggregation of Au particles up to 600 C in oxygen. On the other hand, the enhancement of Au nanoparticle stability by TiO2 overcoat is very limited. Di use reffectance infrared Fourier transform spectroscopy (DRIFTS) of CO chemisorption and X-ray photoelectron spectroscopy measurements both con rmed the ALD overcoat on Au particles surface and suggested that the presence of TiO2 and Al2O3 ALD overcoat on Au nanoparticles does not considerably change the electronic properties of Au nanoparticles. The catalytic activities of the Al2O3 overcoated Au/TiO2 catalysts in CO oxidation increased as increasing calcination temperature, which suggests that the embed-ded Au nanoparticles become more accessible for catalytic function after high temperature treatment, consistent with our DRIFTS CO chemisorption results.
文摘We study behavior of an atomic wave packet in a circularly polarized electromagnetic wave, and particularly calculate the atomic inversion of the wave packet. A general method of calculation is presented. The results are interesting. For example, if the wave packet is very narrow or/and the interaction is very strong, no matter the atom is initially in its ground state or excited state, the atomic inversion approaches zero as time approaches infinity. If the atom is initially in its ground state and excited state with the probability 1/2 respectively, and if the momentum density is an even function, then the atomic inversion equals zero at any time.
基金This work was supported by the National Natural Science Foundation of China (No.51402283 and No.21473169), One Thousand Young Talents Program under the Recruitment Program of Global Experts, the Fundamental Research Funds for the Central Universi- ties (No.WK2060030017), and the Startup Funds from University of Science and Technology of China.
文摘Hydrogen generation from formic acid (FA) has received significant attention. The challenge is to obtain a highly active catalyst under mild conditions for practical applications. Here atomic layer deposition (ALD) of FeOx was performed to deposit an ultrathin oxide coating layer to a Pd/C catalyst, therein the FeOx coverage was precisely controlled by ALD cycles. Transmission electron microscopy and powder X-ray diffraction measurements suggest that the FeOx coating layer improved the thermal stability of Pd nanoparticles (NPs). X-ray photoelectron spectroscopy measurement showed that deposition of FeOx on the Pd NPs caused a positive shift of Pd3d binding energy. In the FA dehydrogenation reaction, the ultrathin FeOx layer on the Pd/C could considerably improve the catalytic activity, and Pd/C coated with 8 cycles of FeOx showed an optimized activity with turnover frequency being about 2 times higher than the uncoated one. shape as a function of the number of FeOx ALD The improved activities were in a volcanocycles, indicating the coverage of FeOx is critical for the optimized activity. In summary, simultaneous improvements of activity and thermal stability of Pd/C catalyst by ultra-thin FeOx overlayer suggest to be an effective way to design active catalysts for the FA dehydrogenation reaction.
基金supported by the National Natural Science Foundation of China (No.21227003, No.21433014, No.11721404)
文摘Two dimensional Fourier transforrn electronic spectroscopy (2DES) in the visible region enables direct observation of complex dynamics of molecules including quantum coherence in the condensed phase. This review aims to provide a bridge between the principles and intuitive physical description of 2DES for tutorial purpose. Special emphasis is laid upon how 2DES circumvents the restrictions from both uncertainty principle and the wave-packet collapse during the coherent detection, leading to the successful detection of the coherence in terms of energy difference between the eigenstates showing as the quantum beats; then upon the possible mixing among the pure electronic transition, single-rnode and multi-mode coupled vibronic transition leading to the observed beating phenomena. Finally, recent ad- vances in experimentally distinguishing between the electronic coherence and the vibrational coherence are briefly discussed.
文摘Photo dissociation dynamics of diatomic molecular ion HBr+ interacting with ultra fast laser pulses of different envelop function has been presented both in zero and non zero temperature environment. The calculations pertain primarily to the ground electronic state of the molecular ion HBr+. The used potential of HBr+ is calibrated with the help of the ab initio theoretical calculation at the CCSD/6-311++G(3df, 2pd) level and then fitted with appropriate Morse parameters. The numerical bound states vibrational eigenvalues obtained by the time independent Fourier Grid Hamiltonian method have been compared with analytical values of the fitted Morse potential. The effect of temperature, pulse envelops function, and light intensity on the dissociation process has been explored.
文摘In contrast to the toxic inorganic forms of selenium to life at very low concentrations, the organic-selenium compounds are of considerable interest and several of them play essential roles in cell biochemistry and nutritional science. Se-yeast (Selenium-enriched yeast) is a common form of selenium used to supplement dietary intake of this important trace mineral. In the present study, we tried to prepare an organic selenocystine using locally isolated bread yeast (Saccharomyces cerevisiae). A novel locally prepared date extract media enriched by addition of 0.2% KH2PO4 (potassium phosphate), 0.6% ammonium sulfate was adopted as alternative culture media. Differences concentrations of selenium salt (30, 60, 120 and 240 lag/mL) were added to the yeast culture media. While the best concentration of selenium added was 30Bg/mL, it achieved optimal conditions for the growth of yeast and the production of red yeast growth identical to the standard. The products (organic selenocystine) were analyzed by HPLC (High Performance Liquid Chromatography) and AAS (Atomic Absorption Spectrophotometer) comparing with authentic standard obtained from Sigma. Results confirmed the formation of similar selenocystine products.