In this study,a trifunctional strategy was developed to prepare a confined Ni-based catalyst(Ni-CeO_(2)@SiO_(2))for dry reforming of methane(DRM)of two main greenhouse gases-CO_(2)and CH_(4).The Ni-CeO_(2)@SiO_(2)cata...In this study,a trifunctional strategy was developed to prepare a confined Ni-based catalyst(Ni-CeO_(2)@SiO_(2))for dry reforming of methane(DRM)of two main greenhouse gases-CO_(2)and CH_(4).The Ni-CeO_(2)@SiO_(2)catalyst was fabricated by utilizing the confinement effect of the SiO_(2)shell and the synergistic interaction between Ni-Ce and the decoking effect of CeO_(2).The catalysts were systematically characterized via X-ray diffraction,N_(2 )adsorption/desorption,transmission electron microscopy,energy dispersive X-ray spectroscopy,hydrogen temperature reduction and desorption set by program,oxygen temperature program desorption,Raman spectroscopy,thermogravimetric analysis,and in situ diffuse reflectance infrared Fourier transform spectroscopy measurements to reveal their physicochemical properties and reaction mechanism.The Ni-CeO_(2)@SiO_(2)catalyst exhibited higher activity and stability than the catalyst synthesized via the traditional impregnation method.In addition,no carbon deposition was detected over Ni-CeO_(2)@SiO_(2)after a 100 h durability test at 800℃,and the average particle size of Ni nanoparticles(NPs)in the catalyst increased from 5.01 to 5.77 nm.Remarkably,Ni-CeO_(2)@SiO_(2)also exhibited superior low-temperature stability;no coke deposition was observed when the catalyst was reacted at 600℃ for 20 h.The high coking and sintering resistance of this confined Ni-based DRM catalyst can be attributed to its trifunctional effect.The trifunctional strategy developed in this study could be used as a guideline to design other high-performance catalysts for CO_(2)and CH4 dry forming and accelerate their industrialization.展开更多
Recently, many attempts have been made to use carbon nanotubes in analytical chemistry, especially in adsorption of heavy metal ions from water. In this study, multiwalled carbon nanotubes (MWCNTs) were functionalized...Recently, many attempts have been made to use carbon nanotubes in analytical chemistry, especially in adsorption of heavy metal ions from water. In this study, multiwalled carbon nanotubes (MWCNTs) were functionalized with tris(2-aminoethyl) amine. The functionalized nanoparticles were characterized using Fourier transform infrared (FTIR), thermal gravimetric analyzer (TGA), elemental analysis, and Raman spectroscopy. The results revealed that the functionalization reaction was successfully accomplished. Lead adsorption from water was carried out using functionalized MWCNTs and measured by flame atomic absorption spectrometry (FAAS). The effects of pH, shaking time, initial metal ion concentration, and adsorbent dosage on the adsorption process were studied via batch method. The results obtained showed that removal of lead ions strongly depended on the pH. Desorption study revealed that lead ions adsorbed on the functionalized MWCNTs could be desorbed at pH 3 due to breakage of complexes formed on the sorbent surface. Maximum adsorption capacity of the sorbent under the optimal conditions was 43 mg/g. This favorable adsorption capacity suggests that functionalized carbon nanotubes can be applied for removal of lead from water solutions. The data obtained were fitted with the Langmuir and Freundlich isotherm adsorption models and Langmuir model showed better agreement with the experimental data.展开更多
Background: Isolated tricuspid valve disease remains a controversial indication for surgical intervention. Many patients referred for surgery already have a poor clinical condition and an advanced New York Heart Assoc...Background: Isolated tricuspid valve disease remains a controversial indication for surgical intervention. Many patients referred for surgery already have a poor clinical condition and an advanced New York Heart Association functional class. There is no consensus on the optimal surgical technique for this condition, including on whether to perform the procedure on a beating or an arrested heart and whether to perform valve repair or replacement. Methods: We analyzed four case series between 2015 and 2022 in which patients with secondary tricuspid regurgitation (TR) underwent valve repair on a beating heart and right atrial plication for a dilated right atrium. The TRI-SCORE was calculated for each patient. Results: All patients experienced a favorable postoperative course with significant improvements in heart failure symptoms. TR was markedly reduced;however, in one patient with concomitant mitral regurgitation (MR) and a high TRI-SCORE, MR worsened postoperatively. This patient later died from unknown causes due to multiple comorbidities in the late phase. Conclusions: Tricuspid valve repair on a beating heart was effective for improving the cardiac function, and the TRI-SCORE proved useful as a preoperative risk assessment tool. The underlying mechanism by which TR exacerbates MR requires further investigation.展开更多
In this study, the first raw transition metals from V to Co complexes with benzene-1,2-dithiolate (L2-) ligand have been studied theoretically to elucidate the geometry, electronic structure and spectroscopic properti...In this study, the first raw transition metals from V to Co complexes with benzene-1,2-dithiolate (L2-) ligand have been studied theoretically to elucidate the geometry, electronic structure and spectroscopic properties of the complexes. Density Functional Theory (DFT) and Time-Dependent Density Functional Theory (TD-DFT) methods have been used. The ground state geometries, binding energies, spectral properties (UV-vis), frontier molecular orbitals (FMOs) analysis, charge analysis and natural bond orbital (NBO) have been investigated. The geometrical parameters are in good agreement with the available experimental data. The metal-ligand binding energies are 1 order of magnitude larger than the physisorption energy of a benzene-1, 2-dthiolate molecule on a metallic surface. The electronic structures of the first raw transition metal series from V to Co have been elucidated by UV-vis spectroscopic using DFT calculations. In accordance with experiment the calculated electronic spectra of these tris complexes show bands at 522, 565, 559, 546 and 863 nm for V3+, Cr3+, Mn3+, Fe3+ and Co3+ respectively which are mainly attributed to ligand to metal charge transfer (LMCT) transitions. The electronic properties analysis shows that the highest occupied molecular orbital (HOMO) is mainly centered on metal coordinated sulfur atoms whereas the lowest unoccupied molecular orbital (LUMO) is mainly located on the metal surface. From calculation of intramolecular interactions and electron delocalization by natural bond orbital (NBO) analysis, the stability of the complexes was estimated. The NBO results showed significant charge transfer from sulfur to central metal ions in the complexes, as well as to the benzene. The calculated charges on metal ions are also reported at various charge schemes. The calculations show encouraging agreement with the available experimental data.展开更多
In this paper, a tri-dimensional filter method for nonlinear programming was proposed. We add a parameter into the traditional filter for relaxing the criterion of iterates. The global convergent properties of the pro...In this paper, a tri-dimensional filter method for nonlinear programming was proposed. We add a parameter into the traditional filter for relaxing the criterion of iterates. The global convergent properties of the proposed algorithm are proved under some appropriate conditions.展开更多
We present a theoretical investigation of plasma generation in sodium vapor induced by laser radiation tuned to the first resonance line (3S-3P) at λ = 589 ns. A set of rate equations that describe the rate of change...We present a theoretical investigation of plasma generation in sodium vapor induced by laser radiation tuned to the first resonance line (3S-3P) at λ = 589 ns. A set of rate equations that describe the rate of change of the ground and excited states population as well as the temporal variation of the electron energy distribution function (EEDF), beside the formed atomic ion Na+, molecular ion ?and tri-atomic ions are solved numerically. The calculations are carried out at different laser energy and different sodium atomic vapor densities under the experimental conditions of Tapalian and Smith (1993) to test the existence of the formed tri-atomic ions. The numerical calculations of the electron energy distribution function (EEDF) show that a deviation from the Maxwellian distribution due to the super elastic collisions effect. In addition to the competition between associative ionization (3P-3P), associative ionization (3P-3D) and Molnar-Horn- beck ionization processes for producing , the calculations have also shown that the atomic ions Na+ are formed through the Penning ionization and photoionization processes. These results are found to be consistent with the experimental observations.展开更多
Tri-butyl citrate(TBC) is synthesized by using several kinds of ionic liquids as catalyst.The results show that the functionalized Brnsted acid ionic liquid([TEA-PS]) is the best catalytic among them;and use it as c...Tri-butyl citrate(TBC) is synthesized by using several kinds of ionic liquids as catalyst.The results show that the functionalized Brnsted acid ionic liquid([TEA-PS]) is the best catalytic among them;and use it as catalyst to optimize the reaction conditions:the proportion of reaction materiel is 1∶3.8(citric acid∶1-butanol);reaction temperature is 130℃;reaction time is 3.5h;cat./citric acid=15∶100(wt);the conversion of citric acid up to 99%.After simply separated from the products and treated with diethyl ether,the ionic liquid could be reused 8 times without noticeably decreasing in the catalytic activity.Therefore,an environmental friendly approach for synthesis of TBC could be provided with the ionic liquid as catalysts.展开更多
文摘In this study,a trifunctional strategy was developed to prepare a confined Ni-based catalyst(Ni-CeO_(2)@SiO_(2))for dry reforming of methane(DRM)of two main greenhouse gases-CO_(2)and CH_(4).The Ni-CeO_(2)@SiO_(2)catalyst was fabricated by utilizing the confinement effect of the SiO_(2)shell and the synergistic interaction between Ni-Ce and the decoking effect of CeO_(2).The catalysts were systematically characterized via X-ray diffraction,N_(2 )adsorption/desorption,transmission electron microscopy,energy dispersive X-ray spectroscopy,hydrogen temperature reduction and desorption set by program,oxygen temperature program desorption,Raman spectroscopy,thermogravimetric analysis,and in situ diffuse reflectance infrared Fourier transform spectroscopy measurements to reveal their physicochemical properties and reaction mechanism.The Ni-CeO_(2)@SiO_(2)catalyst exhibited higher activity and stability than the catalyst synthesized via the traditional impregnation method.In addition,no carbon deposition was detected over Ni-CeO_(2)@SiO_(2)after a 100 h durability test at 800℃,and the average particle size of Ni nanoparticles(NPs)in the catalyst increased from 5.01 to 5.77 nm.Remarkably,Ni-CeO_(2)@SiO_(2)also exhibited superior low-temperature stability;no coke deposition was observed when the catalyst was reacted at 600℃ for 20 h.The high coking and sintering resistance of this confined Ni-based DRM catalyst can be attributed to its trifunctional effect.The trifunctional strategy developed in this study could be used as a guideline to design other high-performance catalysts for CO_(2)and CH4 dry forming and accelerate their industrialization.
文摘Recently, many attempts have been made to use carbon nanotubes in analytical chemistry, especially in adsorption of heavy metal ions from water. In this study, multiwalled carbon nanotubes (MWCNTs) were functionalized with tris(2-aminoethyl) amine. The functionalized nanoparticles were characterized using Fourier transform infrared (FTIR), thermal gravimetric analyzer (TGA), elemental analysis, and Raman spectroscopy. The results revealed that the functionalization reaction was successfully accomplished. Lead adsorption from water was carried out using functionalized MWCNTs and measured by flame atomic absorption spectrometry (FAAS). The effects of pH, shaking time, initial metal ion concentration, and adsorbent dosage on the adsorption process were studied via batch method. The results obtained showed that removal of lead ions strongly depended on the pH. Desorption study revealed that lead ions adsorbed on the functionalized MWCNTs could be desorbed at pH 3 due to breakage of complexes formed on the sorbent surface. Maximum adsorption capacity of the sorbent under the optimal conditions was 43 mg/g. This favorable adsorption capacity suggests that functionalized carbon nanotubes can be applied for removal of lead from water solutions. The data obtained were fitted with the Langmuir and Freundlich isotherm adsorption models and Langmuir model showed better agreement with the experimental data.
文摘Background: Isolated tricuspid valve disease remains a controversial indication for surgical intervention. Many patients referred for surgery already have a poor clinical condition and an advanced New York Heart Association functional class. There is no consensus on the optimal surgical technique for this condition, including on whether to perform the procedure on a beating or an arrested heart and whether to perform valve repair or replacement. Methods: We analyzed four case series between 2015 and 2022 in which patients with secondary tricuspid regurgitation (TR) underwent valve repair on a beating heart and right atrial plication for a dilated right atrium. The TRI-SCORE was calculated for each patient. Results: All patients experienced a favorable postoperative course with significant improvements in heart failure symptoms. TR was markedly reduced;however, in one patient with concomitant mitral regurgitation (MR) and a high TRI-SCORE, MR worsened postoperatively. This patient later died from unknown causes due to multiple comorbidities in the late phase. Conclusions: Tricuspid valve repair on a beating heart was effective for improving the cardiac function, and the TRI-SCORE proved useful as a preoperative risk assessment tool. The underlying mechanism by which TR exacerbates MR requires further investigation.
文摘In this study, the first raw transition metals from V to Co complexes with benzene-1,2-dithiolate (L2-) ligand have been studied theoretically to elucidate the geometry, electronic structure and spectroscopic properties of the complexes. Density Functional Theory (DFT) and Time-Dependent Density Functional Theory (TD-DFT) methods have been used. The ground state geometries, binding energies, spectral properties (UV-vis), frontier molecular orbitals (FMOs) analysis, charge analysis and natural bond orbital (NBO) have been investigated. The geometrical parameters are in good agreement with the available experimental data. The metal-ligand binding energies are 1 order of magnitude larger than the physisorption energy of a benzene-1, 2-dthiolate molecule on a metallic surface. The electronic structures of the first raw transition metal series from V to Co have been elucidated by UV-vis spectroscopic using DFT calculations. In accordance with experiment the calculated electronic spectra of these tris complexes show bands at 522, 565, 559, 546 and 863 nm for V3+, Cr3+, Mn3+, Fe3+ and Co3+ respectively which are mainly attributed to ligand to metal charge transfer (LMCT) transitions. The electronic properties analysis shows that the highest occupied molecular orbital (HOMO) is mainly centered on metal coordinated sulfur atoms whereas the lowest unoccupied molecular orbital (LUMO) is mainly located on the metal surface. From calculation of intramolecular interactions and electron delocalization by natural bond orbital (NBO) analysis, the stability of the complexes was estimated. The NBO results showed significant charge transfer from sulfur to central metal ions in the complexes, as well as to the benzene. The calculated charges on metal ions are also reported at various charge schemes. The calculations show encouraging agreement with the available experimental data.
文摘In this paper, a tri-dimensional filter method for nonlinear programming was proposed. We add a parameter into the traditional filter for relaxing the criterion of iterates. The global convergent properties of the proposed algorithm are proved under some appropriate conditions.
文摘We present a theoretical investigation of plasma generation in sodium vapor induced by laser radiation tuned to the first resonance line (3S-3P) at λ = 589 ns. A set of rate equations that describe the rate of change of the ground and excited states population as well as the temporal variation of the electron energy distribution function (EEDF), beside the formed atomic ion Na+, molecular ion ?and tri-atomic ions are solved numerically. The calculations are carried out at different laser energy and different sodium atomic vapor densities under the experimental conditions of Tapalian and Smith (1993) to test the existence of the formed tri-atomic ions. The numerical calculations of the electron energy distribution function (EEDF) show that a deviation from the Maxwellian distribution due to the super elastic collisions effect. In addition to the competition between associative ionization (3P-3P), associative ionization (3P-3D) and Molnar-Horn- beck ionization processes for producing , the calculations have also shown that the atomic ions Na+ are formed through the Penning ionization and photoionization processes. These results are found to be consistent with the experimental observations.
文摘Tri-butyl citrate(TBC) is synthesized by using several kinds of ionic liquids as catalyst.The results show that the functionalized Brnsted acid ionic liquid([TEA-PS]) is the best catalytic among them;and use it as catalyst to optimize the reaction conditions:the proportion of reaction materiel is 1∶3.8(citric acid∶1-butanol);reaction temperature is 130℃;reaction time is 3.5h;cat./citric acid=15∶100(wt);the conversion of citric acid up to 99%.After simply separated from the products and treated with diethyl ether,the ionic liquid could be reused 8 times without noticeably decreasing in the catalytic activity.Therefore,an environmental friendly approach for synthesis of TBC could be provided with the ionic liquid as catalysts.
