Atomically-dispersed metal-based materials represent an emerging class of photocatalysts attributed to their high catalytic activity,abundant surface active sites,and efficient charge separation.Nevertheless,the roles...Atomically-dispersed metal-based materials represent an emerging class of photocatalysts attributed to their high catalytic activity,abundant surface active sites,and efficient charge separation.Nevertheless,the roles of different forms of atomically-dispersed metals(i.e.,single-atoms and atomic clusters)in photocatalytic reactions remain ambiguous.Herein,we developed an ethylenediamine(EDA)-assisted reduction method to controllably synthesize atomically dispersed Au in the forms of Au single atoms(Au_(SA)),Au clusters(Au_(C)),and a mixed-phase of Au_(SA)and Au_(C)(Au_(SA+C))on CdS.In addition,we elucidate the synergistic effect of Au_(SA)and Au_(C)in enhancing the photocatalytic performance of CdS substrates for simultaneous CO_(2)reduction and aryl alcohol oxidation.Specifically,Au_(SA)can effectively lower the energy barrier for the CO_(2)→*COOH conversion,while Au_(C)can enhance the adsorption of alcohols and reduce the energy barrier for dehydrogenation.As a result,the Au_(SA)and Au_(C)co-loaded CdS show impressive overall photocatalytic CO_(2)conversion performance,achieving remarkable CO and BAD production rates of 4.43 and 4.71 mmol g^(−1)h^(−1),with the selectivities of 93%and 99%,respectively.More importantly,the solar-to-chemical conversion efficiency of Au_(SA+C)/CdS reaches 0.57%,which is over fivefold higher than the typical solar-to-biomass conversion efficiency found in nature(ca.0.1%).This study comprehensively describes the roles of different forms of atomically-dispersed metals and their synergistic effects in photocatalytic reactions,which is anticipated to pave a new avenue in energy and environmental applications.展开更多
The development of InGaAs/InP single-photon avalanche photodiodes(SPADs)necessitates the utiliza-tion of a two-element diffusion technique to achieve accurate manipulation of the multiplication width and the dis-tribu...The development of InGaAs/InP single-photon avalanche photodiodes(SPADs)necessitates the utiliza-tion of a two-element diffusion technique to achieve accurate manipulation of the multiplication width and the dis-tribution of its electric field.Regarding the issue of accurately predicting the depth of diffusion in InGaAs/InP SPAD,simulation analysis and device development were carried out,focusing on the dual diffusion behavior of zinc atoms.A formula of X_(j)=k√t-t_(0)+c to quantitatively predict the diffusion depth is obtained by fitting the simulated twice-diffusion depths based on a two-dimensional(2D)model.The 2D impurity morphologies and the one-dimensional impurity profiles for the dual-diffused region are characterized by using scanning electron micros-copy and secondary ion mass spectrometry as a function of the diffusion depth,respectively.InGaAs/InP SPAD devices with different dual-diffusion conditions are also fabricated,which show breakdown behaviors well consis-tent with the simulated results under the same junction geometries.The dark count rate(DCR)of the device de-creased as the multiplication width increased,as indicated by the results.DCRs of 2×10^(6),1×10^(5),4×10^(4),and 2×10^(4) were achieved at temperatures of 300 K,273 K,263 K,and 253 K,respectively,with a bias voltage of 3 V,when the multiplication width was 1.5µm.These results demonstrate an effective prediction route for accu-rately controlling the dual-diffused zinc junction geometry in InP-based planar device processing.展开更多
Taking simultaneous variations in both particle volume and density into account, the radial mixing and segregation of binary granular bed in a rotating drum half loaded were investigated by a 3D discrete element metho...Taking simultaneous variations in both particle volume and density into account, the radial mixing and segregation of binary granular bed in a rotating drum half loaded were investigated by a 3D discrete element method. Then, based on the competition theory of condensation and percolation, radial segregation due to differences in particle volume and/or density was analyzed. The results show that if either percolation effect induced by volume difference or condensation effect induced by density difference dominates in the active layer of moving bed, separation will occur. Controlling the volume ratio or density ratio of the two types of particles can achieve an equilibrium state between percolation and condensation, and then homogenous mixture can be obtained. When the percolation balances with the condensation, the relationship between volume ratioand density ratiopresents nearly a power function. Scaling up a rotating drum will not affect the mixing degree of the granular bed so long as the volume ratio and density ratio are predefined.展开更多
CuO/γ-Al2O3 catalysts were prepared by impregnation with different CuO loadings. The dispersion of CuO supported on γ-Al2O3 support was studied using X-ray diffraction (XRD), scanning electron microscopy (SEM), ...CuO/γ-Al2O3 catalysts were prepared by impregnation with different CuO loadings. The dispersion of CuO supported on γ-Al2O3 support was studied using X-ray diffraction (XRD), scanning electron microscopy (SEM), and temperature programmed reduction (TPR). The dispersion threshold of CuO in γ-Al2O3 determined by X-ray quantitative analysis was 0.275 g/g, i.e., 0.275CuAl. Highly dispersed CuO or crystalline CuO would appear on the γ-Al2O3 support when CuO loading was below or more than its dispersion threshold. TPR experiments show that reduction peak temperature ranges of 0.1CuAl and pure CuO are 420-690 °C and 290-380 °C, respectively. 0.1CuAl is not easily reduced due to interaction between CuO and γ-Al2O3. 0.5CuAl shows a two-step reduction range during 210-300 °C and 410-730 °C, which confirms the existence of highly dispersed CuO and crystalline CuO. The sulfation experiments show the optimal CuO loading amount is far below its dispersion threshold, and copper oxide supported on γ-Al2O3 is in the form of submonolayer.展开更多
MoS_2 samples with controllable morphologies and structures were synthesized using surfactantassisted hydrothermal processes.The effects of surfactants(PEG,PVP,P123,SDS,AOT,and CTAB)on the morphologies and structure...MoS_2 samples with controllable morphologies and structures were synthesized using surfactantassisted hydrothermal processes.The effects of surfactants(PEG,PVP,P123,SDS,AOT,and CTAB)on the morphologies and structures of MoS_2 samples were investigated.The results revealed that spherical,bulk-like,and flower-like MoS_2 particles assembled by NH4~+-intercalated MoS_2 nano-sheets were synthesized.The morphologies of the MoS_2 samples and their structures(including the slab length and the number of stacked layers) of MoS_2 nano-sheets in these samples could be controlled by adjusting the surfactants.Mono-dispersed spherical MoS_2 particles could be synthesized with PEG via the creation of MoS_2 nano-sheets with slab lengths shorter than 15 nm and fewer than six stacked layers.Possible formation mechanisms of these MoS_2 samples created via surfactant-assisted hydrothermal processes are proposed.Further,the catalytic activities of MoS_2 samples for anthracene hydrogenation were evaluated in a slurry-bed reactor.The catalyst synthesized with the surfactant PEG exhibited the highest catalytic hydrogenation activity.Compared with the other catalysts,it had a smaller particle size,mono-dispersed spherical morphology,shorter slab length,and fewer stacked layers;these were all beneficial to exposing its active edges.This work provides an efficient approach to synthesize transition metal sulfides with controllable morphologies and structures.展开更多
A Markov chain-based stochastic model (MCM) is developed to simulate the movement of particles in a 2D bubbling fluidized bed (BFB). The state spaces are determined by the discretized physical cells of the bed, an...A Markov chain-based stochastic model (MCM) is developed to simulate the movement of particles in a 2D bubbling fluidized bed (BFB). The state spaces are determined by the discretized physical cells of the bed, and the transition probability matrix is directly calculated by the results of a discrete element method (DEM) simulation. The Markov property of the BFB is discussed by the comparison results calculated from both static and dynamic transition probability matrices. The static matrix is calculated based on the Markov chain while the dynamic matrix is calculated based on the memory property of the particle movement. Results show that the difference in the trends of particle movement between the static and dynamic matrix calculation is very small. Besides, the particle mixing curves of the MCM and DEM have the same trend and similar numerical values, and the details show the time averaged characteristic of the MCM and also expose its shortcoming in describing the instantaneous particle dynamics in the BFB.展开更多
To achieve high optical power as well as low vertical divergence angle,a new kind of optim ized large opti- cal cavity (L OC) structure is applied to a ridge waveguide 980 nm In Ga As/ Ga As/ Al Ga As m ulti- quantum...To achieve high optical power as well as low vertical divergence angle,a new kind of optim ized large opti- cal cavity (L OC) structure is applied to a ridge waveguide 980 nm In Ga As/ Ga As/ Al Ga As m ulti- quantum well laser.The optical power density in the waveguide is successfully reduced.The maxim um output power is more than 40 0 m W with a slope efficiency of 0 .89W/ A and the far- field vertical divergence angle is lowered to 2 3°.展开更多
In gas injection refining processes,wide dispersion of small bubbles in the bath is indispensable for high refining efficiency.Eccentric mechanical stirring with unidirectional impeller rotation was tested using a wat...In gas injection refining processes,wide dispersion of small bubbles in the bath is indispensable for high refining efficiency.Eccentric mechanical stirring with unidirectional impeller rotation was tested using a water model for pursuing better bubble disintegration and dispersion.Effects of various factors on bubble disintegration and dispersion were investigated.These factors were stirring mode,eccentricity and rotation speed,nozzle structure,nozzle immersion depth,and gas flow rate.Gas injection from a nozzle at the end of the impeller shaft and from an immersed lance was studied.Under eccentric stirring,a vortex was formed away from the shaft.Small bubbles were produced in the strong turbulence or high shear stress field near the rotating impeller and moved in the direction to the vortex keeping up with the macroscopic flow induced by the mechanical stirring.Thus small bubbles could disperse widely in the bath under eccentric stirring with unidirectional rotation.展开更多
文摘Atomically-dispersed metal-based materials represent an emerging class of photocatalysts attributed to their high catalytic activity,abundant surface active sites,and efficient charge separation.Nevertheless,the roles of different forms of atomically-dispersed metals(i.e.,single-atoms and atomic clusters)in photocatalytic reactions remain ambiguous.Herein,we developed an ethylenediamine(EDA)-assisted reduction method to controllably synthesize atomically dispersed Au in the forms of Au single atoms(Au_(SA)),Au clusters(Au_(C)),and a mixed-phase of Au_(SA)and Au_(C)(Au_(SA+C))on CdS.In addition,we elucidate the synergistic effect of Au_(SA)and Au_(C)in enhancing the photocatalytic performance of CdS substrates for simultaneous CO_(2)reduction and aryl alcohol oxidation.Specifically,Au_(SA)can effectively lower the energy barrier for the CO_(2)→*COOH conversion,while Au_(C)can enhance the adsorption of alcohols and reduce the energy barrier for dehydrogenation.As a result,the Au_(SA)and Au_(C)co-loaded CdS show impressive overall photocatalytic CO_(2)conversion performance,achieving remarkable CO and BAD production rates of 4.43 and 4.71 mmol g^(−1)h^(−1),with the selectivities of 93%and 99%,respectively.More importantly,the solar-to-chemical conversion efficiency of Au_(SA+C)/CdS reaches 0.57%,which is over fivefold higher than the typical solar-to-biomass conversion efficiency found in nature(ca.0.1%).This study comprehensively describes the roles of different forms of atomically-dispersed metals and their synergistic effects in photocatalytic reactions,which is anticipated to pave a new avenue in energy and environmental applications.
基金Supported by Shanghai Natural Science Foundation(22ZR1472600).
文摘The development of InGaAs/InP single-photon avalanche photodiodes(SPADs)necessitates the utiliza-tion of a two-element diffusion technique to achieve accurate manipulation of the multiplication width and the dis-tribution of its electric field.Regarding the issue of accurately predicting the depth of diffusion in InGaAs/InP SPAD,simulation analysis and device development were carried out,focusing on the dual diffusion behavior of zinc atoms.A formula of X_(j)=k√t-t_(0)+c to quantitatively predict the diffusion depth is obtained by fitting the simulated twice-diffusion depths based on a two-dimensional(2D)model.The 2D impurity morphologies and the one-dimensional impurity profiles for the dual-diffused region are characterized by using scanning electron micros-copy and secondary ion mass spectrometry as a function of the diffusion depth,respectively.InGaAs/InP SPAD devices with different dual-diffusion conditions are also fabricated,which show breakdown behaviors well consis-tent with the simulated results under the same junction geometries.The dark count rate(DCR)of the device de-creased as the multiplication width increased,as indicated by the results.DCRs of 2×10^(6),1×10^(5),4×10^(4),and 2×10^(4) were achieved at temperatures of 300 K,273 K,263 K,and 253 K,respectively,with a bias voltage of 3 V,when the multiplication width was 1.5µm.These results demonstrate an effective prediction route for accu-rately controlling the dual-diffused zinc junction geometry in InP-based planar device processing.
基金Projects(5137424151275531)supported by the National Natural Science Foundation of ChinaProject(CX2014B059)supported by the Innovation Foundation for Postgraduate of Hunan Province,China
文摘Taking simultaneous variations in both particle volume and density into account, the radial mixing and segregation of binary granular bed in a rotating drum half loaded were investigated by a 3D discrete element method. Then, based on the competition theory of condensation and percolation, radial segregation due to differences in particle volume and/or density was analyzed. The results show that if either percolation effect induced by volume difference or condensation effect induced by density difference dominates in the active layer of moving bed, separation will occur. Controlling the volume ratio or density ratio of the two types of particles can achieve an equilibrium state between percolation and condensation, and then homogenous mixture can be obtained. When the percolation balances with the condensation, the relationship between volume ratioand density ratiopresents nearly a power function. Scaling up a rotating drum will not affect the mixing degree of the granular bed so long as the volume ratio and density ratio are predefined.
基金Project (Jinchuan 201114) supported by the Pre-Research Foundation of Jinchuan Group Ltd., ChinaProject (2011148) supported by the Analysis and Testing Foundation of Kunming University of Science and Technology, China
文摘CuO/γ-Al2O3 catalysts were prepared by impregnation with different CuO loadings. The dispersion of CuO supported on γ-Al2O3 support was studied using X-ray diffraction (XRD), scanning electron microscopy (SEM), and temperature programmed reduction (TPR). The dispersion threshold of CuO in γ-Al2O3 determined by X-ray quantitative analysis was 0.275 g/g, i.e., 0.275CuAl. Highly dispersed CuO or crystalline CuO would appear on the γ-Al2O3 support when CuO loading was below or more than its dispersion threshold. TPR experiments show that reduction peak temperature ranges of 0.1CuAl and pure CuO are 420-690 °C and 290-380 °C, respectively. 0.1CuAl is not easily reduced due to interaction between CuO and γ-Al2O3. 0.5CuAl shows a two-step reduction range during 210-300 °C and 410-730 °C, which confirms the existence of highly dispersed CuO and crystalline CuO. The sulfation experiments show the optimal CuO loading amount is far below its dispersion threshold, and copper oxide supported on γ-Al2O3 is in the form of submonolayer.
基金supported by the National Natural Science Foundation of China(21303186)the Strategic Priority Research Program of the Chinese Academy of Sciences(XDA07020300)~~
文摘MoS_2 samples with controllable morphologies and structures were synthesized using surfactantassisted hydrothermal processes.The effects of surfactants(PEG,PVP,P123,SDS,AOT,and CTAB)on the morphologies and structures of MoS_2 samples were investigated.The results revealed that spherical,bulk-like,and flower-like MoS_2 particles assembled by NH4~+-intercalated MoS_2 nano-sheets were synthesized.The morphologies of the MoS_2 samples and their structures(including the slab length and the number of stacked layers) of MoS_2 nano-sheets in these samples could be controlled by adjusting the surfactants.Mono-dispersed spherical MoS_2 particles could be synthesized with PEG via the creation of MoS_2 nano-sheets with slab lengths shorter than 15 nm and fewer than six stacked layers.Possible formation mechanisms of these MoS_2 samples created via surfactant-assisted hydrothermal processes are proposed.Further,the catalytic activities of MoS_2 samples for anthracene hydrogenation were evaluated in a slurry-bed reactor.The catalyst synthesized with the surfactant PEG exhibited the highest catalytic hydrogenation activity.Compared with the other catalysts,it had a smaller particle size,mono-dispersed spherical morphology,shorter slab length,and fewer stacked layers;these were all beneficial to exposing its active edges.This work provides an efficient approach to synthesize transition metal sulfides with controllable morphologies and structures.
基金The National Science Foundation of China(No.51276036,51306035)the Fundamental Research Funds for the Central Universities(No.KYLX_0114)
文摘A Markov chain-based stochastic model (MCM) is developed to simulate the movement of particles in a 2D bubbling fluidized bed (BFB). The state spaces are determined by the discretized physical cells of the bed, and the transition probability matrix is directly calculated by the results of a discrete element method (DEM) simulation. The Markov property of the BFB is discussed by the comparison results calculated from both static and dynamic transition probability matrices. The static matrix is calculated based on the Markov chain while the dynamic matrix is calculated based on the memory property of the particle movement. Results show that the difference in the trends of particle movement between the static and dynamic matrix calculation is very small. Besides, the particle mixing curves of the MCM and DEM have the same trend and similar numerical values, and the details show the time averaged characteristic of the MCM and also expose its shortcoming in describing the instantaneous particle dynamics in the BFB.
文摘To achieve high optical power as well as low vertical divergence angle,a new kind of optim ized large opti- cal cavity (L OC) structure is applied to a ridge waveguide 980 nm In Ga As/ Ga As/ Al Ga As m ulti- quantum well laser.The optical power density in the waveguide is successfully reduced.The maxim um output power is more than 40 0 m W with a slope efficiency of 0 .89W/ A and the far- field vertical divergence angle is lowered to 2 3°.
基金Projects (50974035,51074047) supported by the National Natural Science Foundation of ChinaProject (20090407) supported by the Doctoral Fund of Ministry of Education,ChinaProject (200921007) supported by Liaoning Key Science and Technology,China
文摘In gas injection refining processes,wide dispersion of small bubbles in the bath is indispensable for high refining efficiency.Eccentric mechanical stirring with unidirectional impeller rotation was tested using a water model for pursuing better bubble disintegration and dispersion.Effects of various factors on bubble disintegration and dispersion were investigated.These factors were stirring mode,eccentricity and rotation speed,nozzle structure,nozzle immersion depth,and gas flow rate.Gas injection from a nozzle at the end of the impeller shaft and from an immersed lance was studied.Under eccentric stirring,a vortex was formed away from the shaft.Small bubbles were produced in the strong turbulence or high shear stress field near the rotating impeller and moved in the direction to the vortex keeping up with the macroscopic flow induced by the mechanical stirring.Thus small bubbles could disperse widely in the bath under eccentric stirring with unidirectional rotation.