To prepare a highly efficient NiMo/Al_(2)O_(3) hydrodesulfurization catalyst,the combined effects of specific organic functional groups and alumina surface characteristics were investigated.First,the correlation betwe...To prepare a highly efficient NiMo/Al_(2)O_(3) hydrodesulfurization catalyst,the combined effects of specific organic functional groups and alumina surface characteristics were investigated.First,the correlation between the surface characteristics of four different alumina and the existing Mo species states was established.It was found that the Mo equilibrium adsorption capacity can be used as a specific descriptor to quantitatively evaluate the changes in surface characteristics of different alumina.A lower Mo equilibrium adsorption capacity for alumina means weaker metal-support interaction and the loaded Mo species are easier to transform into MoS2.However,the Mo-O-Al bonds still exist at the metal-support interface.The introduction of cationic surfactant hecadecyl trimethyl ammonium bromide(CTAB)can further improve Mo species dispersion through electrostatic attraction with Mo anions and interaction of its alkyl chain with the alumina surface;meanwhile,the introduction of ethylenediamine tetraacetic acid(EDTA)can complex with Ni ions to enhance the Ni-promoting effect on Mo.Therefore,the NiMo catalyst designed using alumina with lower Mo equilibrium adsorption capacity and the simultaneous addition of EDTA and CTAB exhibits the highest hydrodesulfurization activity for 4,6-dimethyl dibenzothiophene because of its proper metal-support interaction and more well-dispersed Ni-Mo-S active phases.展开更多
In the field of dual-pulse laser-induced breakdown spectroscopy(DP-LIBS)research,the pursuit of methods for determining pulse intervals and other parameters quickly and conveniently in order to achieve optimal spectra...In the field of dual-pulse laser-induced breakdown spectroscopy(DP-LIBS)research,the pursuit of methods for determining pulse intervals and other parameters quickly and conveniently in order to achieve optimal spectral signal enhancement is paramount.To aid researchers in identification of optimal signal enhancement conditions and more accurate interpretation of the underlying signal enhancement mechanisms,theoretical simulations of the spatiotemporal processes of coaxial DP-LIBS-induced plasma have been established in this work.Using a model based on laser ablation and two-dimensional axisymmetric fluid dynamics,plasma evolutions during aluminum–magnesium alloy laser ablation under single-pulse and coaxial dualpulse excitations have been simulated.The influences of factors,such as delay time,laser fluence,plasma temperature,and particle number density,on the DP-LIBS spectral signals are investigated.Under pulse intervals ranging from 50 to 1500 ns,the time evolutions of spectral line intensity,dual-pulse emission enhancement relative to the single-pulse results,laser irradiance,spatial distribution of plasma temperature and species number density,as well as laser irradiance shielded by plasma have been obtained.The study indicates that the main reason behind the radiation signal enhancement in coaxial DP-LIBS-induced plasma is attributed to the increased species number density and plasma temperature caused by the second laser,and it is inferred that the shielding effect of the plasma mainly occurs in the boundary layer of the stagnation point flow over the target surface.This research provides a theoretical basis for experimental research,parameter optimization,and signal enhancement tracing in DP-LIBS.展开更多
The self-absorption effect in laser-induced breakdown spectroscopy(LIBS)reduces the accuracy of quantitative measurement results.The self-absorption-free LIBS(SAF-LIBS)has been proved to directly capture the optically...The self-absorption effect in laser-induced breakdown spectroscopy(LIBS)reduces the accuracy of quantitative measurement results.The self-absorption-free LIBS(SAF-LIBS)has been proved to directly capture the optically thin plasma spectra by setting an appropriate exposure time.In this work,a novel SAF-LIBS technique with high repetition rate acousto-optic gating is developed,in which an acousto-optic modulator is used as the shutter to diffract the optically thin fluorescence,and a high repetition rate laser is used to produce quasi-continuous plasmas to enhance the integral spectral intensity,so that the CCD spectrometer can replace an intensified CCD(ICCD)and echelle spectrometer in SAF-LIBS.Experimental results show that the average absolute prediction error of aluminum is reduced to 0.18%,which is equivalent to that of traditional SAF-LIBS.This technique not only effectively shields continuous background radiation and broadened spectral lines in optically thick plasma,but also has advantages of miniaturization,low cost,convenience and reliability.展开更多
We proposed a theoretical spatio-temporal imaging method,which was based on the thermal model of laser ablation and the two-dimensional axisymmetric multi-species hydrodynamics model.By using the intensity formula,the...We proposed a theoretical spatio-temporal imaging method,which was based on the thermal model of laser ablation and the two-dimensional axisymmetric multi-species hydrodynamics model.By using the intensity formula,the integral intensity of spectral lines could be calculated and the corresponding images of intensity distribution could be drawn.Through further image processing such as normalization,determination of minimum intensity,combination and color filtering,a relatively clear species distribution image in the plasma could be obtained.Using the above method,we simulated the plasma ablated from Al-Mg alloy by different laser energies under 1 atm argon,and obtained the theoretical spatio-temporal distributions of Mg I,Mg II,Al I,Al II and Ar I species,which are almost consistent with the experimental results by differential imaging.Compared with the experimental decay time constants,the consistency is higher at low laser energy,indicating that our theoretical model is more suitable for the plasma dominated by laser-supported combustion wave.展开更多
Laser-induced plasma is often produced in the presence of background gas,which causes some new physical processes.In this work,a two-dimensional axisymmetric radiation fluid dynamics model is used to numerically simul...Laser-induced plasma is often produced in the presence of background gas,which causes some new physical processes.In this work,a two-dimensional axisymmetric radiation fluid dynamics model is used to numerically simulate the expansion process of plasma under different pressures and gases,in which the multiple interaction processes of diffusion,viscosity and heat conduction between the laser ablated target vapor and the background gas are further considered,and the spatio-temporal evolutions of plasma parameters(species number density,expansion velocity,size and electron temperature)as well as the emission spectra are obtained.The consistency between the actual and simulated spectra of aluminum plasma in 1 atm argon verifies the correctness of the model and the numerical simulation,thus providing a refinement analysis method for the basic research of plasma expansion in gases and the application of laser-induced breakdown spectroscopy.展开更多
基金funding of the National Key Research and Development Plan(Grant 2017YFB0306600)the Project of SINOPEC(NO.117006).
文摘To prepare a highly efficient NiMo/Al_(2)O_(3) hydrodesulfurization catalyst,the combined effects of specific organic functional groups and alumina surface characteristics were investigated.First,the correlation between the surface characteristics of four different alumina and the existing Mo species states was established.It was found that the Mo equilibrium adsorption capacity can be used as a specific descriptor to quantitatively evaluate the changes in surface characteristics of different alumina.A lower Mo equilibrium adsorption capacity for alumina means weaker metal-support interaction and the loaded Mo species are easier to transform into MoS2.However,the Mo-O-Al bonds still exist at the metal-support interface.The introduction of cationic surfactant hecadecyl trimethyl ammonium bromide(CTAB)can further improve Mo species dispersion through electrostatic attraction with Mo anions and interaction of its alkyl chain with the alumina surface;meanwhile,the introduction of ethylenediamine tetraacetic acid(EDTA)can complex with Ni ions to enhance the Ni-promoting effect on Mo.Therefore,the NiMo catalyst designed using alumina with lower Mo equilibrium adsorption capacity and the simultaneous addition of EDTA and CTAB exhibits the highest hydrodesulfurization activity for 4,6-dimethyl dibenzothiophene because of its proper metal-support interaction and more well-dispersed Ni-Mo-S active phases.
基金supported by the National Key R&D Program of China (No. 2017YFA0304203)the National Energy R&D Center of Petroleum Refining Technology (RIPP, SINOPEC)+3 种基金Changjiang Scholars and Innovative Research Team at the University of the Ministry of Education of China (No. IRT_17R70)National Natural Science Foundation of China (NSFC) (Nos. 61975103, 61875108 and 627010407)111 Project (No. D18001)Fund for Shanxi (No. 1331KSC)
文摘In the field of dual-pulse laser-induced breakdown spectroscopy(DP-LIBS)research,the pursuit of methods for determining pulse intervals and other parameters quickly and conveniently in order to achieve optimal spectral signal enhancement is paramount.To aid researchers in identification of optimal signal enhancement conditions and more accurate interpretation of the underlying signal enhancement mechanisms,theoretical simulations of the spatiotemporal processes of coaxial DP-LIBS-induced plasma have been established in this work.Using a model based on laser ablation and two-dimensional axisymmetric fluid dynamics,plasma evolutions during aluminum–magnesium alloy laser ablation under single-pulse and coaxial dualpulse excitations have been simulated.The influences of factors,such as delay time,laser fluence,plasma temperature,and particle number density,on the DP-LIBS spectral signals are investigated.Under pulse intervals ranging from 50 to 1500 ns,the time evolutions of spectral line intensity,dual-pulse emission enhancement relative to the single-pulse results,laser irradiance,spatial distribution of plasma temperature and species number density,as well as laser irradiance shielded by plasma have been obtained.The study indicates that the main reason behind the radiation signal enhancement in coaxial DP-LIBS-induced plasma is attributed to the increased species number density and plasma temperature caused by the second laser,and it is inferred that the shielding effect of the plasma mainly occurs in the boundary layer of the stagnation point flow over the target surface.This research provides a theoretical basis for experimental research,parameter optimization,and signal enhancement tracing in DP-LIBS.
基金National Key R&D Program of China(No.2017YFA0304203)National Energy R&D Center of Petroleum Refining Technology(RIPP,SINOPEC),Changjiang Scholars and Innovative Research Team in University of Ministry of Education of China(IRT_17R70)+3 种基金National Natural Science Foundation of China(Nos.61975103,61875108,61775125 and 11434007)Major Special Science and Technology Projects in Shanxi(No.201804D131036)111 Project(No.D18001)Fund for Shanxi’1331KSC’。
文摘The self-absorption effect in laser-induced breakdown spectroscopy(LIBS)reduces the accuracy of quantitative measurement results.The self-absorption-free LIBS(SAF-LIBS)has been proved to directly capture the optically thin plasma spectra by setting an appropriate exposure time.In this work,a novel SAF-LIBS technique with high repetition rate acousto-optic gating is developed,in which an acousto-optic modulator is used as the shutter to diffract the optically thin fluorescence,and a high repetition rate laser is used to produce quasi-continuous plasmas to enhance the integral spectral intensity,so that the CCD spectrometer can replace an intensified CCD(ICCD)and echelle spectrometer in SAF-LIBS.Experimental results show that the average absolute prediction error of aluminum is reduced to 0.18%,which is equivalent to that of traditional SAF-LIBS.This technique not only effectively shields continuous background radiation and broadened spectral lines in optically thick plasma,but also has advantages of miniaturization,low cost,convenience and reliability.
基金supported by National Key R&D Program of China(No.2017YFA0304203)National Energy R&D Center of Petroleum Refining Technology(RIPP,SINOPEC)+4 种基金Changjiang Scholars and Innovative Research Team in University of Ministry of Education of China(No.IRT_17R70)National Natural Science Foundation of China(NSFC)(Nos.61975103,61875108,61775125,11434007)Major Special Science and Technology Projects in Shanxi(No.201804D131036)111 Project(No.D18001)Fund for Shanxi‘1331KSC’。
文摘We proposed a theoretical spatio-temporal imaging method,which was based on the thermal model of laser ablation and the two-dimensional axisymmetric multi-species hydrodynamics model.By using the intensity formula,the integral intensity of spectral lines could be calculated and the corresponding images of intensity distribution could be drawn.Through further image processing such as normalization,determination of minimum intensity,combination and color filtering,a relatively clear species distribution image in the plasma could be obtained.Using the above method,we simulated the plasma ablated from Al-Mg alloy by different laser energies under 1 atm argon,and obtained the theoretical spatio-temporal distributions of Mg I,Mg II,Al I,Al II and Ar I species,which are almost consistent with the experimental results by differential imaging.Compared with the experimental decay time constants,the consistency is higher at low laser energy,indicating that our theoretical model is more suitable for the plasma dominated by laser-supported combustion wave.
基金supported by National Key R&D Program of China(No.2017YFA0304203)National Energy R&D Center of Petroleum Refining Technology(RIPP,SINOPEC)+4 种基金Changjiang Scholars and Innovative Research Team in University of Ministry of Education of China(No.IRT_17R70)National Natural Science Foundation of China(NSFC)(Nos.61975103,61875108,61775125,11434007)Major Special Science and Technology Projects in Shanxi(No.201804D131036)111 project(No.D18001)Fund for Shanxi‘1331KSC’。
文摘Laser-induced plasma is often produced in the presence of background gas,which causes some new physical processes.In this work,a two-dimensional axisymmetric radiation fluid dynamics model is used to numerically simulate the expansion process of plasma under different pressures and gases,in which the multiple interaction processes of diffusion,viscosity and heat conduction between the laser ablated target vapor and the background gas are further considered,and the spatio-temporal evolutions of plasma parameters(species number density,expansion velocity,size and electron temperature)as well as the emission spectra are obtained.The consistency between the actual and simulated spectra of aluminum plasma in 1 atm argon verifies the correctness of the model and the numerical simulation,thus providing a refinement analysis method for the basic research of plasma expansion in gases and the application of laser-induced breakdown spectroscopy.