Homogeneous and heterogeneous types of catalysis are frequently considered as separate disciplines or even opposed to each other.In the present work,a new type of mixed het-ero-/homogeneous catalysis was demonstrated ...Homogeneous and heterogeneous types of catalysis are frequently considered as separate disciplines or even opposed to each other.In the present work,a new type of mixed het-ero-/homogeneous catalysis was demonstrated for the case of selective alkylarene oxidation by molecular oxygen.The proposed catalytic system consists of two widely available components:N-hydroxyphthalimide(NHPI,a homogeneous organocatalyst for free-radical chain reactions)and nanosized TiO_(2)(heterogeneous UV-active photoredox catalyst).The interaction of NHPI with TiO_(2) allows for a shift from UV to visible light photoredox activity and generation of phthalimide-N-oxyl(PINO)radicals that diffuse into the solution where NHPI/PINO-catalyzed free-radical chain reaction can proceed without the additional light input providing a fundamental increase in energy efficiency.The NHPI/TiO_(2) ratio controls the selectivity of oxidation affording preferential formation of hydroperoxide or ketone from alkylarene.展开更多
Pt based materials are the most efficient electrocatalysts for the oxygen reduction reaction(ORR)and methanol oxidation reaction(MOR)in fuel cells.Maximizing the utilization of Pt based materials by modulating their m...Pt based materials are the most efficient electrocatalysts for the oxygen reduction reaction(ORR)and methanol oxidation reaction(MOR)in fuel cells.Maximizing the utilization of Pt based materials by modulating their morphologies to expose more active sites is a fundamental objective for the practical application of fuel cells.Herein,we report a new class of hierarchically skeletal Pt-Ni nanocrystals(HSNs)with a multi-layered structure,prepared by an inorganic acid-induced solvothermal method.The addition of H_(2)SO_(4)to the synthetic protocol provides a critical trigger for the successful growth of Pt-Ni nanocrystals with the desired structure.The Pt-Ni HSNs synthesized by this method exhibit enhanced mass activity of 1.25 A mgpt−1 at 0.9 V(versus the reversible hydrogen electrode)towards ORR in 0.1-M HClO_(4),which is superior to that of Pt-Ni multi-branched nanocrystals obtained by the same method in the absence of inorganic acid;it is additionally 8.9-fold higher than that of the commercial Pt/C catalyst.Meanwhile,it displays enhanced stability,with only 21.6%mass activity loss after 10,000 cycles(0.6–1.0 V)for ORR.Furthermore,the Pt-Ni HSNs show enhanced activity and anti-toxic ability in CO for MOR.The superb activity of the Pt-Ni HSNs for ORR and MOR is fully attributed to an extensively exposed electrochemical surface area and high intrinsic activity,induced by strain effects,provided by the unique hierarchically skeletal alloy structure.The novel open and hierarchical structure of Pt-Ni alloy provides a promising approach for significant improvements of the activity of Pt based alloy electrocatalysts.展开更多
A robust control strategy using the second-order integral sliding mode control(SOISMC)based on the variable speed grey wolf optimization(VGWO)is proposed.The aim is to maximize the wind power extraction of wind turbin...A robust control strategy using the second-order integral sliding mode control(SOISMC)based on the variable speed grey wolf optimization(VGWO)is proposed.The aim is to maximize the wind power extraction of wind turbine.Firstly,according to the uncertainty model of wind turbine,a SOISMC torque controller with fast convergence speed,strong robustness and effective chattering reduction is designed,which ensures that the torque controller can effectively track the reference speed.Secondly,given the strong local search ability of the grey wolf optimization(GWO)and the fast convergence speed and strong global search ability of the particle swarm optimization(PSO),the speed component of PSO is introduced into GWO,and VGWO with fast convergence speed,high solution accuracy and strong global search ability is used to optimize the parameters of wind turbine torque controller.Finally,the simulation is implemented based on Simulink/SimPowerSystem.The results demonstrate the effectiveness of the proposed strategy under both external disturbance and model uncertainty.展开更多
NOx can cause severe environmental problems such as acid rain and photochemical smog,endangering human health and the living environment.Among them,NO pollution accounts for about 95%.NO can exist stably in the air fo...NOx can cause severe environmental problems such as acid rain and photochemical smog,endangering human health and the living environment.Among them,NO pollution accounts for about 95%.NO can exist stably in the air for a long time when the concentration is lower than the ppm level.Therefore,the conversion of low concentration of NO has attracted more and more attention.However,traditional physical or chemical methods are difficult to deal with low concentration of NO,having high requirements on equipment and being not cost‐effective.Semiconductor photocatalytic technology can convert low concentration of NO into non‐toxic products and reduce its harm.This work briefly surveys the commonly used materials,modification methods,and mechanisms for semiconductor photocatalytic conversion of low concentration of NO.In addition,the challenges and prospects of ppb level of NO treatment are also discussed,aiming to promote the development of semiconductor photocatalytic conversion of NO.展开更多
Resonance enhancement has been increasingly employed in the emergent felntosecond stimu- lated Raman spectroscopy (FSRS) to selectively monitor molecular structure and dynamics with improved spectral and temporal re...Resonance enhancement has been increasingly employed in the emergent felntosecond stimu- lated Raman spectroscopy (FSRS) to selectively monitor molecular structure and dynamics with improved spectral and temporal resolutions and signal-to-noise ratios. Such joint eflforts by the technique- and application-oriented scientists and engineers have laid the foundation for exploiting the tunable FSRS methodology to investigate a great variety of photosensitive systems and elucidate the underlying functional mechanisms on molecular time scales. Dur- ing spectral analysis, peak line shapes remain a major concern with an intricate dependence on resonance conditions. Here, we present a comprehensive study of line shapes by tuning the Rarnan pump wavelength from red to blue side of the ground-state absorption band of the fluorescent dye rhodarnine 6G in solution. Distinct line shape patterns in Stokes and anti-Stokes FSRS as well as from the low to high-frequency modes highlight the competition between multiple third-order and higher-order nonlinear pathways, governed by difl^rent res- onance conditions achieved by Raman pump and probe pulses. In particular, the resonance condition of probe wavelength is revealed to play an important role in generating circular line shape changes through oppositely phased dispersion via hot luminescence (HL) pathways. Meanwhile, on-resonance conditions of the Rarnan pump could promote excited-state vibrational modes which are broadened and red-shifted from the coincident ground-state vibrational modes, posing challenges for spectral analysis. Certain strategies in tuning the Raman pump and probe to characteristic regions across an electronic transition band are discussed to improve the FSRS usability and versatility as a powerful structural dynamics toolset to advance chemical, physical, materials, and biological sciences.展开更多
The influence of the textural and acidic properties ofγ‐Al2O3,(γ+χ)‐Al2O3,and?‐Al2O3on the catalytic activity,selectivity,and stability of direct H2S oxidation has been studied.A comparison of the H2S‐to‐S con...The influence of the textural and acidic properties ofγ‐Al2O3,(γ+χ)‐Al2O3,and?‐Al2O3on the catalytic activity,selectivity,and stability of direct H2S oxidation has been studied.A comparison of the H2S‐to‐S conversion effectiveness of aluminas with their acidic properties(identified by Fourier transform infrared spectroscopy and temperature programmed desorption of NH3)shows that H2S adsorption occurs predominantly on weak Lewis acid sites(LAS).γ‐Alumina samples containing aχ‐phase and/or modified Mg2+ions have a greater concentration of weak LAS and exhibit greater catalytic activity.When alumina is treated with a sulfuric acid solution,strong LAS appear and the number of LAS decreases significantly.Modification of alumina with hydrochloric acid has a limited effect on LAS strength.Weak LAS are retained and double in number compared to that present in the unmodified alumina,but the treated sample has Al?Cl bonds.Alumina samples modified by sulfate and chloride anions exhibit poor catalytic activity in H2S oxidation.展开更多
A fully automated atomic force microscope(AFM)is presented.The mechanical motion of the AFM stage was controlled by three steppers.The fine motion of the AFM was controlled by an MCL one-axis piezo plate.A32.768kHz cr...A fully automated atomic force microscope(AFM)is presented.The mechanical motion of the AFM stage was controlled by three steppers.The fine motion of the AFM was controlled by an MCL one-axis piezo plate.A32.768kHz crystal tuning fork(TF)was used as the transducer with a probe attached.An acoustic sensor was used to measure the interactions between the probe and the sample.An SR850lock-in amplifier was used to monitor the TF signals.An additional lock-in amplifier was used to monitor the acoustic signal.A field programmable gate array(FPGA)board was used to collect the data in automatic mode.The main controller was coded with LabVIEW,which was in charge of Z-axis scan,signal processing and data visualization.A manual mode and an automatic mode were implemented in the controller.Users can switch the two modes at any time during the operation.This AFM system showed several advantages during the test operations.It is simple,flexible and easy to use.展开更多
The purpose of this article is to reduce the barrier of developing a house made scanning probe microscope (SPM). Here in this paper, we cover all the details of programming an SPM controller with LabVIEW. The main c...The purpose of this article is to reduce the barrier of developing a house made scanning probe microscope (SPM). Here in this paper, we cover all the details of programming an SPM controller with LabVIEW. The main controller has three major sequential portions. They are system initialization portion, scan control and image display portion and system shutdown portion. The most complicated and essential part of the main controller is the scan control and image display portion, which is achieved with various parallel tasks. These tasks are scan area and image size adjusting module, Y axis scan control module, X axis scan and image transferring module, parameters readjusting module, emergency shutdown module, etc. A NI7831R FPGA board is used to output the control signals and utilize the Z-axis real time feedback controls. The system emergency shutdown is also carried out by the FPGA module. Receiving the shutdown command from the main controller, the FPGA board will move the probe to its XYZ zero position, turn off all the high voltage control signals and also eliminate the possible oscillations in the system. Finally, how to operate the controller is also briefly introduced. That messy wires fly back and forth is the main drawback of LabVIEW programming. Especially when the program is complicated, this problem becomes more serious. We use a real example to show how to achieve complex functionalities with structural programming and parallel multi task programming. The actual code showed in this paper is clear, intuitive and simple. Following the examples showed in this paper, readers are able to develop simple LabVIEW programs to achieve complex functionalities.展开更多
We have investigated the adsorption of nine different adatoms on the(111)and(100)surfaces of Iridium(Ir)using first principles density functional theory.The study explores surface functionalization of Ir which would p...We have investigated the adsorption of nine different adatoms on the(111)and(100)surfaces of Iridium(Ir)using first principles density functional theory.The study explores surface functionalization of Ir which would provide important information for further study of its functionality in catalysis and other surface applications.The adsorption energy,stable geometry,density of states and magnetic moment are some of the physical quantities of our interest.The study reveals that the three-/four-fold hollow site is energetically the most favorable adsorption site on the(111)/(100)surface of Ir.The investigation on a wide range of coverages(from 0.04 to 1 monolayer)reveals the strong coverage dependence of adsorption energy of the adsorbate atoms.The adsorption energy is found to increase as the coverage increases,implying a repulsive interaction between the adsorbates.Strong hybridization between the adsorbates and the substrate electronic states is revealed to impact the adsorption,while the magnetic moment of the adsorbates is found to be suppressed.The Bader analysis reveals significant amount of charge transfers between the adsorbate atoms and the substrate.The binding of adsorbate atoms on the(100)surface is observed to be moderately stronger as compared to that on the(111)surface.展开更多
A simple,stable and reliable virtual logic analyzer is presented. The logic analyzer had two modules:one was the test pattern generation module,the other was the logic monitoring module. Combining the two modules,one ...A simple,stable and reliable virtual logic analyzer is presented. The logic analyzer had two modules:one was the test pattern generation module,the other was the logic monitoring module. Combining the two modules,one is able to test a digital circuit automatically. The user interface of the logic analyzer was programmed with LabVIEW. Two Arduino UNO boards were used as the hardware targets to input and output the logic signals. The maximum pattern update rate was set to be 20 Hz. The maximum logic sampling rate was set to be 200 Hz. After twelve thousand cycles of exhaustive tests,the logic analyzer had a 100% accuracy. As a tutorial showing how to build virtual instruments with Arduino,the software detail is also explained in this article.展开更多
In the face of deteriorating environmental conditions in the world,water quality control is an urgent task.It can be solved by creating sensors with high accuracy and low cost,which requires the development of fundame...In the face of deteriorating environmental conditions in the world,water quality control is an urgent task.It can be solved by creating sensors with high accuracy and low cost,which requires the development of fundamentally new radiophysical methods that take advantage of the optical,microwave and millimeter wavelengths that have a significantly greater sensitivity to low concentrations of pollutants and a lower inertia.The article presents prototypes of measuring cells of the microwave and optical ranges as well as the results of an experimental study of water of various degrees of pollution with their help.The results show that the use of the highly sensitive method of capillary-waveguide resonance makes it possible to detect the presence of micro impurities in water with concentrations up to0.1%and to identify water even from sources of various natural origins.In addition,the use of measurements at several frequencies in the optical range will make it possible to solve the problem of creating water control sensors with high sensitivity to pollution and low cost.It can be concluded that the possibility of complex use of multiwave sensors(optical,infrared and microwave ranges)allows to increase the sensitivity and reliability of water quality assessment.展开更多
The cleavage of the alkoxy(Ar-O-R) ether bond present in anisole is an interesting hydrodeoxygenation(HDO) reaction, since this asymmetric group contains two different C–O bonds, Caryl–O or Calkyl–O, which could po...The cleavage of the alkoxy(Ar-O-R) ether bond present in anisole is an interesting hydrodeoxygenation(HDO) reaction, since this asymmetric group contains two different C–O bonds, Caryl–O or Calkyl–O, which could potentially cleave. Recent work on the HDO of anisole over Pt, Ru, and Fe catalysts has shown that a common phenoxy surface intermediate is formed on all three metals. The subsequent reaction path of this intermediate varies from metal to metal, depending on the metal oxophilicity. Over the less oxophilic Pt, phenol is the only primary product. By contrast, on the more oxophilic Fe catalyst, the sole primary product is benzene instead of phenol. On Ru, with intermediate oxophilicity, both benzene and phenol are primary products. In this contribution, we have investigated Rh catalysts of varying surface nanostructures. A combination of experimental measurements and computational calculations was used to explore the effects of varying metal coordination number, an additional parameter that can be used to control the oxophilicity of a metal. The results confirm that metal oxophilicity is a good descriptor for HDO performance of metal catalysts and it can be controlled via selection of metal type and/or metal extent of coordination. Small Rh metal clusters with low coordination metal sites are more active for the deoxygenation pathway but also quickly deactivated while large clusters with high coordination sites are more active toward hydrogenation and more stable.展开更多
The possibility of using finite atomic functions of Kravchenko-Rvachev for description of the laws of distribution of the refractive index of the troposphere,the intensity of the scattering from the sea,seasonal behav...The possibility of using finite atomic functions of Kravchenko-Rvachev for description of the laws of distribution of the refractive index of the troposphere,the intensity of the scattering from the sea,seasonal behavior unit radar cross section(RCS)of land areas with vegetation covering,as well as the spectrum of electromagnetic spikes of lithospheric origin is considered.展开更多
Objective:This study aimed to lay the foundation for the research on Panax notoginseng saponins(PNS)in pH-sensitive in situ gel and the development and improvement of related preparations.Methods:We used Carbopol■940...Objective:This study aimed to lay the foundation for the research on Panax notoginseng saponins(PNS)in pH-sensitive in situ gel and the development and improvement of related preparations.Methods:We used Carbopol■940,a commonly used pH-sensitive polymer,and the thickener hydroxypropyl methylcellulose(HPMC E4M)as an ophthalmic gel matrix to prepare an ophthalmic in situ gel of PNS.In addition,formula optimization was performed by assessing gelling capability with the results of in vitro release studies.In vitro(corneal permeation,rheological,and stability)and in vivo(ocular irritation and preliminary pharmacokinetics in the vitreous)studies were also performed.Results:The results demonstrated that the in situ gelling systems containing PNS showed a sustained release of the drug,making it an ideal ocular delivery system for improving posterior ocular bioavailability.Conclusions:This study lays the foundation for the research of PNS contained in an in situ pH-triggered gel as well as the development and improvement of related preparations.It concurrently traditional Chinese medicine with a contemporary in situ gelling approach to provide new directions for the treatment of posterior ocular diseases such as diabetic retinopathy.展开更多
Non-equidistant sparse antenna arrays constructed on the basis of Latin squares are considered. A method for their construction and a synthesis algorithm are proposed,and the properties of two-dimensional antennas bas...Non-equidistant sparse antenna arrays constructed on the basis of Latin squares are considered. A method for their construction and a synthesis algorithm are proposed,and the properties of two-dimensional antennas based on them,which ensure,at a high degree of rarefaction,a sufficiently small lateral radiation are studied. The features and main characteristics of such antennas are studied.展开更多
A technique for testing space object receivers using global navigation satellite system (GNSS) signal simulator of the navigation field is proposed. Its structure consists of two blocks which allow synthesizing the ...A technique for testing space object receivers using global navigation satellite system (GNSS) signal simulator of the navigation field is proposed. Its structure consists of two blocks which allow synthesizing the scenario of reciprocal displacement of the receiver relative to navigation satellites and their signals. In the first block, according to the known coordinates of the receiver which are specified in tabular form or analytically, the distances between the receiver and the navigation satellites are calculated as well as their relative velocities. According to these data, the second block synthesizes the signals of navigational travelers with the specified characteristics which are transmitted via the air or cable with a given attenuation to the receiver. This allows testing on the earth receivers for airplanes and space objects under different scenarios of their movement, which not only reduces the risk of problems during the flight, but also avoids significant economic costs. Based on real data obtained by approaching two spacecraft using a simulator, the receiver was tested, which shows the promise of the proposed technology.展开更多
To understand the effect of the doping amount of Cu^2+ on the structure and reactivity of SnO2 in NOx-SCR with NH3, a series of Sn-Cu-O binary oxide catalysts with different Sn/Cu ratios have been prepared and thoroug...To understand the effect of the doping amount of Cu^2+ on the structure and reactivity of SnO2 in NOx-SCR with NH3, a series of Sn-Cu-O binary oxide catalysts with different Sn/Cu ratios have been prepared and thoroughly characterized. Using the XRD extrapolation method, the SnO2 lattice capacity for Cu^2+ cations is determined at 0.10 g Cu O per g of SnO2, equaling a Sn/Cu molar ratio of 84/16. Therefore, in a tetragonal rutile SnO2 lattice, only a maximum of 16% of the Sn4+ cations can be replaced by Cu^2+ to form a stable solid solution structure. If the Cu content is higher, Cu O will form on the catalyst surface, which has a negative effect on the reaction performance. For samples in a pure solid solution phase, the number of surface defects increase with increasing Cu content until it reaches the lattice capacity, as confirmed by Raman spectroscopy. As a result, the amounts of both active oxygen species and acidic sites on the surface, which critically determine the reaction performance, also increase and reach the maximum level for the catalyst with a Cu content close to the lattice capacity. A distinct lattice capacity threshold effect on the structure and reactivity of Sn-Cu binary oxide catalysts has been observed. A Sn-Cu catalyst with the best reaction performance can be obtained by doping the SnO2 matrix with the lattice capacity amount of Cu^2+.展开更多
New methods of synthetizing nonequidistant sparse antenna arrays based on the properties of magic squares are studied.The methods of construction and algorithms of synthesis of two-dimensional antennas based on them p...New methods of synthetizing nonequidistant sparse antenna arrays based on the properties of magic squares are studied.The methods of construction and algorithms of synthesis of two-dimensional antennas based on them providing a high degreeof dilution and sufficiently small side radiation are proposed.The methods for construction of such antennas and their maincharacteristics are considered.展开更多
文摘Homogeneous and heterogeneous types of catalysis are frequently considered as separate disciplines or even opposed to each other.In the present work,a new type of mixed het-ero-/homogeneous catalysis was demonstrated for the case of selective alkylarene oxidation by molecular oxygen.The proposed catalytic system consists of two widely available components:N-hydroxyphthalimide(NHPI,a homogeneous organocatalyst for free-radical chain reactions)and nanosized TiO_(2)(heterogeneous UV-active photoredox catalyst).The interaction of NHPI with TiO_(2) allows for a shift from UV to visible light photoredox activity and generation of phthalimide-N-oxyl(PINO)radicals that diffuse into the solution where NHPI/PINO-catalyzed free-radical chain reaction can proceed without the additional light input providing a fundamental increase in energy efficiency.The NHPI/TiO_(2) ratio controls the selectivity of oxidation affording preferential formation of hydroperoxide or ketone from alkylarene.
文摘Pt based materials are the most efficient electrocatalysts for the oxygen reduction reaction(ORR)and methanol oxidation reaction(MOR)in fuel cells.Maximizing the utilization of Pt based materials by modulating their morphologies to expose more active sites is a fundamental objective for the practical application of fuel cells.Herein,we report a new class of hierarchically skeletal Pt-Ni nanocrystals(HSNs)with a multi-layered structure,prepared by an inorganic acid-induced solvothermal method.The addition of H_(2)SO_(4)to the synthetic protocol provides a critical trigger for the successful growth of Pt-Ni nanocrystals with the desired structure.The Pt-Ni HSNs synthesized by this method exhibit enhanced mass activity of 1.25 A mgpt−1 at 0.9 V(versus the reversible hydrogen electrode)towards ORR in 0.1-M HClO_(4),which is superior to that of Pt-Ni multi-branched nanocrystals obtained by the same method in the absence of inorganic acid;it is additionally 8.9-fold higher than that of the commercial Pt/C catalyst.Meanwhile,it displays enhanced stability,with only 21.6%mass activity loss after 10,000 cycles(0.6–1.0 V)for ORR.Furthermore,the Pt-Ni HSNs show enhanced activity and anti-toxic ability in CO for MOR.The superb activity of the Pt-Ni HSNs for ORR and MOR is fully attributed to an extensively exposed electrochemical surface area and high intrinsic activity,induced by strain effects,provided by the unique hierarchically skeletal alloy structure.The novel open and hierarchical structure of Pt-Ni alloy provides a promising approach for significant improvements of the activity of Pt based alloy electrocatalysts.
基金This work was supported by the National Natural Science Foundation of China(No.51876089)the Fundamental Research Funds for the Central Universities(No.kfjj20190205).
文摘A robust control strategy using the second-order integral sliding mode control(SOISMC)based on the variable speed grey wolf optimization(VGWO)is proposed.The aim is to maximize the wind power extraction of wind turbine.Firstly,according to the uncertainty model of wind turbine,a SOISMC torque controller with fast convergence speed,strong robustness and effective chattering reduction is designed,which ensures that the torque controller can effectively track the reference speed.Secondly,given the strong local search ability of the grey wolf optimization(GWO)and the fast convergence speed and strong global search ability of the particle swarm optimization(PSO),the speed component of PSO is introduced into GWO,and VGWO with fast convergence speed,high solution accuracy and strong global search ability is used to optimize the parameters of wind turbine torque controller.Finally,the simulation is implemented based on Simulink/SimPowerSystem.The results demonstrate the effectiveness of the proposed strategy under both external disturbance and model uncertainty.
文摘NOx can cause severe environmental problems such as acid rain and photochemical smog,endangering human health and the living environment.Among them,NO pollution accounts for about 95%.NO can exist stably in the air for a long time when the concentration is lower than the ppm level.Therefore,the conversion of low concentration of NO has attracted more and more attention.However,traditional physical or chemical methods are difficult to deal with low concentration of NO,having high requirements on equipment and being not cost‐effective.Semiconductor photocatalytic technology can convert low concentration of NO into non‐toxic products and reduce its harm.This work briefly surveys the commonly used materials,modification methods,and mechanisms for semiconductor photocatalytic conversion of low concentration of NO.In addition,the challenges and prospects of ppb level of NO treatment are also discussed,aiming to promote the development of semiconductor photocatalytic conversion of NO.
基金supported by the U.S.National Science Foundation CAREER grant(CHE-1455353)the Oregon State University(OSU) Research Equipment Reserve Fund(Spring 2014)to C.Fang(USTC9603)the Wei Family Private Foundation in supporting C.Chen(USTC 0903) during his graduate studies at OSU Chemistry
文摘Resonance enhancement has been increasingly employed in the emergent felntosecond stimu- lated Raman spectroscopy (FSRS) to selectively monitor molecular structure and dynamics with improved spectral and temporal resolutions and signal-to-noise ratios. Such joint eflforts by the technique- and application-oriented scientists and engineers have laid the foundation for exploiting the tunable FSRS methodology to investigate a great variety of photosensitive systems and elucidate the underlying functional mechanisms on molecular time scales. Dur- ing spectral analysis, peak line shapes remain a major concern with an intricate dependence on resonance conditions. Here, we present a comprehensive study of line shapes by tuning the Rarnan pump wavelength from red to blue side of the ground-state absorption band of the fluorescent dye rhodarnine 6G in solution. Distinct line shape patterns in Stokes and anti-Stokes FSRS as well as from the low to high-frequency modes highlight the competition between multiple third-order and higher-order nonlinear pathways, governed by difl^rent res- onance conditions achieved by Raman pump and probe pulses. In particular, the resonance condition of probe wavelength is revealed to play an important role in generating circular line shape changes through oppositely phased dispersion via hot luminescence (HL) pathways. Meanwhile, on-resonance conditions of the Rarnan pump could promote excited-state vibrational modes which are broadened and red-shifted from the coincident ground-state vibrational modes, posing challenges for spectral analysis. Certain strategies in tuning the Raman pump and probe to characteristic regions across an electronic transition band are discussed to improve the FSRS usability and versatility as a powerful structural dynamics toolset to advance chemical, physical, materials, and biological sciences.
基金This work was conducted within the framework of Program of the Russian Academy of Sciences and the Federal Agency for Scientific Organizations (state‐guaranteed order for BIC, Project АААА‐А17‐117041710086‐6).
文摘The influence of the textural and acidic properties ofγ‐Al2O3,(γ+χ)‐Al2O3,and?‐Al2O3on the catalytic activity,selectivity,and stability of direct H2S oxidation has been studied.A comparison of the H2S‐to‐S conversion effectiveness of aluminas with their acidic properties(identified by Fourier transform infrared spectroscopy and temperature programmed desorption of NH3)shows that H2S adsorption occurs predominantly on weak Lewis acid sites(LAS).γ‐Alumina samples containing aχ‐phase and/or modified Mg2+ions have a greater concentration of weak LAS and exhibit greater catalytic activity.When alumina is treated with a sulfuric acid solution,strong LAS appear and the number of LAS decreases significantly.Modification of alumina with hydrochloric acid has a limited effect on LAS strength.Weak LAS are retained and double in number compared to that present in the unmodified alumina,but the treated sample has Al?Cl bonds.Alumina samples modified by sulfate and chloride anions exhibit poor catalytic activity in H2S oxidation.
文摘A fully automated atomic force microscope(AFM)is presented.The mechanical motion of the AFM stage was controlled by three steppers.The fine motion of the AFM was controlled by an MCL one-axis piezo plate.A32.768kHz crystal tuning fork(TF)was used as the transducer with a probe attached.An acoustic sensor was used to measure the interactions between the probe and the sample.An SR850lock-in amplifier was used to monitor the TF signals.An additional lock-in amplifier was used to monitor the acoustic signal.A field programmable gate array(FPGA)board was used to collect the data in automatic mode.The main controller was coded with LabVIEW,which was in charge of Z-axis scan,signal processing and data visualization.A manual mode and an automatic mode were implemented in the controller.Users can switch the two modes at any time during the operation.This AFM system showed several advantages during the test operations.It is simple,flexible and easy to use.
文摘The purpose of this article is to reduce the barrier of developing a house made scanning probe microscope (SPM). Here in this paper, we cover all the details of programming an SPM controller with LabVIEW. The main controller has three major sequential portions. They are system initialization portion, scan control and image display portion and system shutdown portion. The most complicated and essential part of the main controller is the scan control and image display portion, which is achieved with various parallel tasks. These tasks are scan area and image size adjusting module, Y axis scan control module, X axis scan and image transferring module, parameters readjusting module, emergency shutdown module, etc. A NI7831R FPGA board is used to output the control signals and utilize the Z-axis real time feedback controls. The system emergency shutdown is also carried out by the FPGA module. Receiving the shutdown command from the main controller, the FPGA board will move the probe to its XYZ zero position, turn off all the high voltage control signals and also eliminate the possible oscillations in the system. Finally, how to operate the controller is also briefly introduced. That messy wires fly back and forth is the main drawback of LabVIEW programming. Especially when the program is complicated, this problem becomes more serious. We use a real example to show how to achieve complex functionalities with structural programming and parallel multi task programming. The actual code showed in this paper is clear, intuitive and simple. Following the examples showed in this paper, readers are able to develop simple LabVIEW programs to achieve complex functionalities.
基金supported by the National Natural Science Foundation of China(No.11750110415,No.11474246,and No.11774178)the Natural Science Foundation of Jiangsu Province(BK20160061)。
文摘We have investigated the adsorption of nine different adatoms on the(111)and(100)surfaces of Iridium(Ir)using first principles density functional theory.The study explores surface functionalization of Ir which would provide important information for further study of its functionality in catalysis and other surface applications.The adsorption energy,stable geometry,density of states and magnetic moment are some of the physical quantities of our interest.The study reveals that the three-/four-fold hollow site is energetically the most favorable adsorption site on the(111)/(100)surface of Ir.The investigation on a wide range of coverages(from 0.04 to 1 monolayer)reveals the strong coverage dependence of adsorption energy of the adsorbate atoms.The adsorption energy is found to increase as the coverage increases,implying a repulsive interaction between the adsorbates.Strong hybridization between the adsorbates and the substrate electronic states is revealed to impact the adsorption,while the magnetic moment of the adsorbates is found to be suppressed.The Bader analysis reveals significant amount of charge transfers between the adsorbate atoms and the substrate.The binding of adsorbate atoms on the(100)surface is observed to be moderately stronger as compared to that on the(111)surface.
文摘A simple,stable and reliable virtual logic analyzer is presented. The logic analyzer had two modules:one was the test pattern generation module,the other was the logic monitoring module. Combining the two modules,one is able to test a digital circuit automatically. The user interface of the logic analyzer was programmed with LabVIEW. Two Arduino UNO boards were used as the hardware targets to input and output the logic signals. The maximum pattern update rate was set to be 20 Hz. The maximum logic sampling rate was set to be 200 Hz. After twelve thousand cycles of exhaustive tests,the logic analyzer had a 100% accuracy. As a tutorial showing how to build virtual instruments with Arduino,the software detail is also explained in this article.
文摘In the face of deteriorating environmental conditions in the world,water quality control is an urgent task.It can be solved by creating sensors with high accuracy and low cost,which requires the development of fundamentally new radiophysical methods that take advantage of the optical,microwave and millimeter wavelengths that have a significantly greater sensitivity to low concentrations of pollutants and a lower inertia.The article presents prototypes of measuring cells of the microwave and optical ranges as well as the results of an experimental study of water of various degrees of pollution with their help.The results show that the use of the highly sensitive method of capillary-waveguide resonance makes it possible to detect the presence of micro impurities in water with concentrations up to0.1%and to identify water even from sources of various natural origins.In addition,the use of measurements at several frequencies in the optical range will make it possible to solve the problem of creating water control sensors with high sensitivity to pollution and low cost.It can be concluded that the possibility of complex use of multiwave sensors(optical,infrared and microwave ranges)allows to increase the sensitivity and reliability of water quality assessment.
基金supported by the U.S.Department of Energy,DOE/EPSCOR(Grant DESC0004600)
文摘The cleavage of the alkoxy(Ar-O-R) ether bond present in anisole is an interesting hydrodeoxygenation(HDO) reaction, since this asymmetric group contains two different C–O bonds, Caryl–O or Calkyl–O, which could potentially cleave. Recent work on the HDO of anisole over Pt, Ru, and Fe catalysts has shown that a common phenoxy surface intermediate is formed on all three metals. The subsequent reaction path of this intermediate varies from metal to metal, depending on the metal oxophilicity. Over the less oxophilic Pt, phenol is the only primary product. By contrast, on the more oxophilic Fe catalyst, the sole primary product is benzene instead of phenol. On Ru, with intermediate oxophilicity, both benzene and phenol are primary products. In this contribution, we have investigated Rh catalysts of varying surface nanostructures. A combination of experimental measurements and computational calculations was used to explore the effects of varying metal coordination number, an additional parameter that can be used to control the oxophilicity of a metal. The results confirm that metal oxophilicity is a good descriptor for HDO performance of metal catalysts and it can be controlled via selection of metal type and/or metal extent of coordination. Small Rh metal clusters with low coordination metal sites are more active for the deoxygenation pathway but also quickly deactivated while large clusters with high coordination sites are more active toward hydrogenation and more stable.
文摘The possibility of using finite atomic functions of Kravchenko-Rvachev for description of the laws of distribution of the refractive index of the troposphere,the intensity of the scattering from the sea,seasonal behavior unit radar cross section(RCS)of land areas with vegetation covering,as well as the spectrum of electromagnetic spikes of lithospheric origin is considered.
文摘Objective:This study aimed to lay the foundation for the research on Panax notoginseng saponins(PNS)in pH-sensitive in situ gel and the development and improvement of related preparations.Methods:We used Carbopol■940,a commonly used pH-sensitive polymer,and the thickener hydroxypropyl methylcellulose(HPMC E4M)as an ophthalmic gel matrix to prepare an ophthalmic in situ gel of PNS.In addition,formula optimization was performed by assessing gelling capability with the results of in vitro release studies.In vitro(corneal permeation,rheological,and stability)and in vivo(ocular irritation and preliminary pharmacokinetics in the vitreous)studies were also performed.Results:The results demonstrated that the in situ gelling systems containing PNS showed a sustained release of the drug,making it an ideal ocular delivery system for improving posterior ocular bioavailability.Conclusions:This study lays the foundation for the research of PNS contained in an in situ pH-triggered gel as well as the development and improvement of related preparations.It concurrently traditional Chinese medicine with a contemporary in situ gelling approach to provide new directions for the treatment of posterior ocular diseases such as diabetic retinopathy.
文摘Non-equidistant sparse antenna arrays constructed on the basis of Latin squares are considered. A method for their construction and a synthesis algorithm are proposed,and the properties of two-dimensional antennas based on them,which ensure,at a high degree of rarefaction,a sufficiently small lateral radiation are studied. The features and main characteristics of such antennas are studied.
文摘A technique for testing space object receivers using global navigation satellite system (GNSS) signal simulator of the navigation field is proposed. Its structure consists of two blocks which allow synthesizing the scenario of reciprocal displacement of the receiver relative to navigation satellites and their signals. In the first block, according to the known coordinates of the receiver which are specified in tabular form or analytically, the distances between the receiver and the navigation satellites are calculated as well as their relative velocities. According to these data, the second block synthesizes the signals of navigational travelers with the specified characteristics which are transmitted via the air or cable with a given attenuation to the receiver. This allows testing on the earth receivers for airplanes and space objects under different scenarios of their movement, which not only reduces the risk of problems during the flight, but also avoids significant economic costs. Based on real data obtained by approaching two spacecraft using a simulator, the receiver was tested, which shows the promise of the proposed technology.
文摘To understand the effect of the doping amount of Cu^2+ on the structure and reactivity of SnO2 in NOx-SCR with NH3, a series of Sn-Cu-O binary oxide catalysts with different Sn/Cu ratios have been prepared and thoroughly characterized. Using the XRD extrapolation method, the SnO2 lattice capacity for Cu^2+ cations is determined at 0.10 g Cu O per g of SnO2, equaling a Sn/Cu molar ratio of 84/16. Therefore, in a tetragonal rutile SnO2 lattice, only a maximum of 16% of the Sn4+ cations can be replaced by Cu^2+ to form a stable solid solution structure. If the Cu content is higher, Cu O will form on the catalyst surface, which has a negative effect on the reaction performance. For samples in a pure solid solution phase, the number of surface defects increase with increasing Cu content until it reaches the lattice capacity, as confirmed by Raman spectroscopy. As a result, the amounts of both active oxygen species and acidic sites on the surface, which critically determine the reaction performance, also increase and reach the maximum level for the catalyst with a Cu content close to the lattice capacity. A distinct lattice capacity threshold effect on the structure and reactivity of Sn-Cu binary oxide catalysts has been observed. A Sn-Cu catalyst with the best reaction performance can be obtained by doping the SnO2 matrix with the lattice capacity amount of Cu^2+.
文摘New methods of synthetizing nonequidistant sparse antenna arrays based on the properties of magic squares are studied.The methods of construction and algorithms of synthesis of two-dimensional antennas based on them providing a high degreeof dilution and sufficiently small side radiation are proposed.The methods for construction of such antennas and their maincharacteristics are considered.