The molybdenum carbide(Mo_(2)C)has been regarded as one of the most cost-efficient and stable electrocatalyst for the hydrogen evolution reaction(HER)by the virtue of its Pt-like electronic structures.However,the inhe...The molybdenum carbide(Mo_(2)C)has been regarded as one of the most cost-efficient and stable electrocatalyst for the hydrogen evolution reaction(HER)by the virtue of its Pt-like electronic structures.However,the inherent limitation of high density of empty valence band significantly reduces its catalytic reactivity by reason of strong hydrogen desorption resistance.Herein,we propose a multiscale confinement synthesis method to design the nitrogen-rich Mo_(2)C for modulating the band structure via decomposing the pre-coordination bonded polymer in a pressure-tight tube sealing system.Pre-bonded c/N-Mo in the coordination precursor constructs a micro-confinement space,enabling the homogeneous nitrogenization in-situ happened during the formation of Mo_(2)C.Simultaneously,the evolved gases from the precursor decomposition in tube sealing system establish a macro-confinement environment,preventing the lattice N escape and further endowing a continuous nitridation.Combining the multiscale confinement effects,the nitrogen-rich Mo2C displays as high as 25%N-Mo concentration in carbide lattice,leading to a satisfactory band structure.Accordingly,the constructed nitrogen-rich Mo_(2)C reveals an adorable catalytic activity for HER in both alkaline and acid solution.It is anticipated that the multiscale confinement synthesis strategy presents guideline for the rational design of electrocatalysts and beyond.展开更多
The separation of C2H4from C_(2)H_(6)/C_(2)H_(4)mixture is of great importance but difficult and energy intensive. Adsorptive separation provides an alternative approach to ameliorate this situation. Here, we report a...The separation of C2H4from C_(2)H_(6)/C_(2)H_(4)mixture is of great importance but difficult and energy intensive. Adsorptive separation provides an alternative approach to ameliorate this situation. Here, we report a microporous metal–organic framework(MOF) BUT-315-a as a C_(2)H_(6)-selective adsorbent for the separation of C2H6/C2H4gas mixture. BUT-315-a combines good IAST selectivity of 2.35 with high C_(2)H_(6)uptake of 97.5 cm^(3)g^(-1), giving superior high separation potential ΔQ(2226 mmol L^(-1)) for equimolar C_(2)H_(6)/C_(2)H_(4) at 298 K. Impressively, such excellent performance can be preserved at higher temperatures of 313 and 323 K to accommodate industrial conditions. Efficient dynamic separation performance of BUT-315-a has been demonstrated by column breakthrough experiments under varied temperatures and gas ratios. Theoretical calculations further reveal multiple synergistic interactions between C_(2)H_(6) and the framework. This work highlights a new benchmark material for C_(2)H_(6)/C_(2)H_(4)separation and provides guidance for designing adsorbent for separation applications.展开更多
We investigate a novel form of non-uniform living turbulence at an extremely low Reynolds number using a bacterial suspension confined within a sessile droplet. This turbulence differs from homogeneous active turbulen...We investigate a novel form of non-uniform living turbulence at an extremely low Reynolds number using a bacterial suspension confined within a sessile droplet. This turbulence differs from homogeneous active turbulences in two or threedimensional geometries. The heterogeneity arises from a gradient of bacterial activity due to oxygen depletion along the droplet’s radial direction. Motile bacteria inject energy at individual scales, resulting in local anisotropic energy fluctuations that collectively give rise to isotropic turbulence. We find that the total kinetic energy and enstrophy decrease as distance from the drop contact line increases, due to the weakening of bacterial activity caused by oxygen depletion. While the balance between kinetic energy and enstrophy establishes a characteristic vortex scale depending on the contact angle of the sessile drop. The energy spectrum exhibits diverse scaling behaviors at large wavenumber, ranging from k-1/5to k-1,depending on the geometric confinement. Our findings demonstrate how spatial regulation of turbulence can be achieved by tuning the activity of driving units, offering insights into the dynamic behavior of living systems and the potential for controlling turbulence through gradient confinements.展开更多
We present findings on the effect of nanometer-sized silica-based pores on the glass transition of aqueous solutions of lithium bis(trifluoromethane)sulfonimide(LiTFSI)and lithium difluorosulfimide(LiFSI),respectively...We present findings on the effect of nanometer-sized silica-based pores on the glass transition of aqueous solutions of lithium bis(trifluoromethane)sulfonimide(LiTFSI)and lithium difluorosulfimide(LiFSI),respectively.Our experimental results demonstrate a clear dependence of the confinement effect on the anion type,particularly for water-rich solutions,in which the precipitation of crystalized ice under cooling process induces the formation of freeze-concentrated phase confined between pore wall and core ice.As this liquid layer becomes thinner,the freeze-concentrated phase experiences glass transition at increasingly higher temperatures in solutions of LiTFSI.However,differently,for solutions of LiFSI and LiCl,this secondary confinement has a negligible effect on the glass transition of solutions confined wherein.These different behaviors emphasize the obvious difference in the dynamic properties’response of LiTFSI and LiFSI solutions to spatial confinement and particularly to the presence of the hydrophilic pore wall.展开更多
A broadband(BB)mode is observed by collective Thomson scattering diagnostics in repeatable shots of EAST and analyzed for the first time.This BB mode usually grows during L–H transitions,featuring a BB quasi-coherent...A broadband(BB)mode is observed by collective Thomson scattering diagnostics in repeatable shots of EAST and analyzed for the first time.This BB mode usually grows during L–H transitions,featuring a BB quasi-coherent mode with increasing frequency.During H-mode operations,it is characterized by steady-state BB in the high-frequency range(f~200–2000 k Hz),at the electron scale(k_(θ)ρ_(s)=1–2),mainly driven by the density gradient,and is sensitive to the value ofηein the region of interest(ρ=0.4–0.8),wherehe=(R/L_(Te))/(R/L_(ne))is the ratio of the normalized electron temperature gradient and density gradient,and the regionρ=0.4–0.8 usually has a relatively low collisionality(v_(eff)<5).The frequency of BB is found to be dependent on the electron temperature and density gradient,which is a typical feature of electron-driven turbulence.A negative correlation between the energy confinement and the intensity of the BB turbulence during H-mode has been found,which indicates a strong electron thermal transport induced by the BB turbulence.The BB significantly decreases the electron temperature and causes flatter electron temperature profiles in the region of interest(ρ=0.4–0.8),thus makingηedecrease and the BB destabilize further.These characteristics of BB are related to the theoretical density gradient-driven trapped electron mode.It should be noted that this mode is not observed by other diagnostics in EAST,and shows very different features to the coherent modes in the edge.展开更多
Aggregation of polyoxometalates(POM)is largely responsible for the reduced performance of POM-based energy-storage systems.To address this challenge,here,the precise confinement of single Keggin-type POM molecule in a...Aggregation of polyoxometalates(POM)is largely responsible for the reduced performance of POM-based energy-storage systems.To address this challenge,here,the precise confinement of single Keggin-type POM molecule in a porous carbon(PC)of unimodal super-micropore(micro-PC)is realized.Such precise single-molecule confinement enables sufficient activity center exposure and maximum electron-transfer from micro-PC to POM,which well stabilizes the electron-accepting molecules and thoroughly activates its inherent multi-electron redox-activity.In particular,the redox-activities and electron-accepting properties of the confined POM molecule are revealed to be super-micropore pore size-dependent by experiment and spectroscopy as well as theoretical calculation.Meanwhile,the molecularly dispersed POM molecules confined steadily in the“cage”of micro-PC exhibit unprecedented large-negative-potential stability and multiple-peak redox-activity at an ultra-low loading of~11.4 wt%.As a result,the fabricated solid-state supercapacitor achieves a remarkable areal capacitance,ultrahigh energy and power density of 443 mF cm^(-2),0.12 mWh cm^(-2)and 21.1 mW cm^(-2),respectively.This work establishes a novel strategy for the precise confinement of single POM molecule,providing a versatile approach to inducing the intrinsic activity of POMs for advanced energy-storage systems.展开更多
The implosion plasma drive fusion pellet of inertial confinement is a concept related to nuclear fusion,a process in which atomic nuclei combine to form heavier nuclei,releasing a large amount of energy in the process...The implosion plasma drive fusion pellet of inertial confinement is a concept related to nuclear fusion,a process in which atomic nuclei combine to form heavier nuclei,releasing a large amount of energy in the process.The implosion plasma drive fusion pellet is a potential fuel source for achieving controlled nuclear fusion.ICF(inertial confinement fusion)is a technique used to achieve fusion by compressing a small target containing fusion fuel to extremely high densities and temperatures using lasers or other methods.The implosion plasma drive fusion pellet concept involves using a small pellet of deuterium and tritium(two isotopes of hydrogen)as fusion fuel,and then rapidly heating and compressing it using a pulsed power system.The implosion process creates a high-pressure plasma that ignites the fusion reactions,releasing energy in the form of neutrons and charged particles.The resulting energy can be captured and used for power generation.This technology is still in the experimental stage,and significant research and development is required to make it commercially viable.However,it has the potential to provide a virtually limitless source of clean energy with no greenhouse gas emissions or long-term radioactive waste.Be that as it may,ICF has to get exact control of the implosion process,mitigate insecurities,and create modern materials and advances to resist the extraordinary conditions of the combined response.展开更多
基金supported by the National Natural Science Foundation of China(52372201,52125202,52202247)the Natural Science Foundation of Jiangsu Province(1192261031693)the Fundamental Research Funds for the Central Universities(30919011110,1191030558)。
文摘The molybdenum carbide(Mo_(2)C)has been regarded as one of the most cost-efficient and stable electrocatalyst for the hydrogen evolution reaction(HER)by the virtue of its Pt-like electronic structures.However,the inherent limitation of high density of empty valence band significantly reduces its catalytic reactivity by reason of strong hydrogen desorption resistance.Herein,we propose a multiscale confinement synthesis method to design the nitrogen-rich Mo_(2)C for modulating the band structure via decomposing the pre-coordination bonded polymer in a pressure-tight tube sealing system.Pre-bonded c/N-Mo in the coordination precursor constructs a micro-confinement space,enabling the homogeneous nitrogenization in-situ happened during the formation of Mo_(2)C.Simultaneously,the evolved gases from the precursor decomposition in tube sealing system establish a macro-confinement environment,preventing the lattice N escape and further endowing a continuous nitridation.Combining the multiscale confinement effects,the nitrogen-rich Mo2C displays as high as 25%N-Mo concentration in carbide lattice,leading to a satisfactory band structure.Accordingly,the constructed nitrogen-rich Mo_(2)C reveals an adorable catalytic activity for HER in both alkaline and acid solution.It is anticipated that the multiscale confinement synthesis strategy presents guideline for the rational design of electrocatalysts and beyond.
基金the financial support of the National Natural Science Foundation of China (No. 22038001)。
文摘The separation of C2H4from C_(2)H_(6)/C_(2)H_(4)mixture is of great importance but difficult and energy intensive. Adsorptive separation provides an alternative approach to ameliorate this situation. Here, we report a microporous metal–organic framework(MOF) BUT-315-a as a C_(2)H_(6)-selective adsorbent for the separation of C2H6/C2H4gas mixture. BUT-315-a combines good IAST selectivity of 2.35 with high C_(2)H_(6)uptake of 97.5 cm^(3)g^(-1), giving superior high separation potential ΔQ(2226 mmol L^(-1)) for equimolar C_(2)H_(6)/C_(2)H_(4) at 298 K. Impressively, such excellent performance can be preserved at higher temperatures of 313 and 323 K to accommodate industrial conditions. Efficient dynamic separation performance of BUT-315-a has been demonstrated by column breakthrough experiments under varied temperatures and gas ratios. Theoretical calculations further reveal multiple synergistic interactions between C_(2)H_(6) and the framework. This work highlights a new benchmark material for C_(2)H_(6)/C_(2)H_(4)separation and provides guidance for designing adsorbent for separation applications.
基金Project supported by the National Natural Science Foundation of China (Grant Nos. 12174306 and 12004308)the Natural Science Basic Research Program of Shaanxi (Grant No. 2023-JC-JQ-02)。
文摘We investigate a novel form of non-uniform living turbulence at an extremely low Reynolds number using a bacterial suspension confined within a sessile droplet. This turbulence differs from homogeneous active turbulences in two or threedimensional geometries. The heterogeneity arises from a gradient of bacterial activity due to oxygen depletion along the droplet’s radial direction. Motile bacteria inject energy at individual scales, resulting in local anisotropic energy fluctuations that collectively give rise to isotropic turbulence. We find that the total kinetic energy and enstrophy decrease as distance from the drop contact line increases, due to the weakening of bacterial activity caused by oxygen depletion. While the balance between kinetic energy and enstrophy establishes a characteristic vortex scale depending on the contact angle of the sessile drop. The energy spectrum exhibits diverse scaling behaviors at large wavenumber, ranging from k-1/5to k-1,depending on the geometric confinement. Our findings demonstrate how spatial regulation of turbulence can be achieved by tuning the activity of driving units, offering insights into the dynamic behavior of living systems and the potential for controlling turbulence through gradient confinements.
基金Project supported by the National Natural Science Foundation of China(Grant Nos.11974385 and 91956101).
文摘We present findings on the effect of nanometer-sized silica-based pores on the glass transition of aqueous solutions of lithium bis(trifluoromethane)sulfonimide(LiTFSI)and lithium difluorosulfimide(LiFSI),respectively.Our experimental results demonstrate a clear dependence of the confinement effect on the anion type,particularly for water-rich solutions,in which the precipitation of crystalized ice under cooling process induces the formation of freeze-concentrated phase confined between pore wall and core ice.As this liquid layer becomes thinner,the freeze-concentrated phase experiences glass transition at increasingly higher temperatures in solutions of LiTFSI.However,differently,for solutions of LiFSI and LiCl,this secondary confinement has a negligible effect on the glass transition of solutions confined wherein.These different behaviors emphasize the obvious difference in the dynamic properties’response of LiTFSI and LiFSI solutions to spatial confinement and particularly to the presence of the hydrophilic pore wall.
基金supported by National Natural Science Foundation of China(No.11875286)the National Key R&D Program of China(No.2019YFE03010002)CAS President’s International Fellowship Initiative(No.2022VMB0007)。
文摘A broadband(BB)mode is observed by collective Thomson scattering diagnostics in repeatable shots of EAST and analyzed for the first time.This BB mode usually grows during L–H transitions,featuring a BB quasi-coherent mode with increasing frequency.During H-mode operations,it is characterized by steady-state BB in the high-frequency range(f~200–2000 k Hz),at the electron scale(k_(θ)ρ_(s)=1–2),mainly driven by the density gradient,and is sensitive to the value ofηein the region of interest(ρ=0.4–0.8),wherehe=(R/L_(Te))/(R/L_(ne))is the ratio of the normalized electron temperature gradient and density gradient,and the regionρ=0.4–0.8 usually has a relatively low collisionality(v_(eff)<5).The frequency of BB is found to be dependent on the electron temperature and density gradient,which is a typical feature of electron-driven turbulence.A negative correlation between the energy confinement and the intensity of the BB turbulence during H-mode has been found,which indicates a strong electron thermal transport induced by the BB turbulence.The BB significantly decreases the electron temperature and causes flatter electron temperature profiles in the region of interest(ρ=0.4–0.8),thus makingηedecrease and the BB destabilize further.These characteristics of BB are related to the theoretical density gradient-driven trapped electron mode.It should be noted that this mode is not observed by other diagnostics in EAST,and shows very different features to the coherent modes in the edge.
基金the National Natural Science Foundation of China(No.51902222,5197222 and 62174013)
文摘Aggregation of polyoxometalates(POM)is largely responsible for the reduced performance of POM-based energy-storage systems.To address this challenge,here,the precise confinement of single Keggin-type POM molecule in a porous carbon(PC)of unimodal super-micropore(micro-PC)is realized.Such precise single-molecule confinement enables sufficient activity center exposure and maximum electron-transfer from micro-PC to POM,which well stabilizes the electron-accepting molecules and thoroughly activates its inherent multi-electron redox-activity.In particular,the redox-activities and electron-accepting properties of the confined POM molecule are revealed to be super-micropore pore size-dependent by experiment and spectroscopy as well as theoretical calculation.Meanwhile,the molecularly dispersed POM molecules confined steadily in the“cage”of micro-PC exhibit unprecedented large-negative-potential stability and multiple-peak redox-activity at an ultra-low loading of~11.4 wt%.As a result,the fabricated solid-state supercapacitor achieves a remarkable areal capacitance,ultrahigh energy and power density of 443 mF cm^(-2),0.12 mWh cm^(-2)and 21.1 mW cm^(-2),respectively.This work establishes a novel strategy for the precise confinement of single POM molecule,providing a versatile approach to inducing the intrinsic activity of POMs for advanced energy-storage systems.
文摘The implosion plasma drive fusion pellet of inertial confinement is a concept related to nuclear fusion,a process in which atomic nuclei combine to form heavier nuclei,releasing a large amount of energy in the process.The implosion plasma drive fusion pellet is a potential fuel source for achieving controlled nuclear fusion.ICF(inertial confinement fusion)is a technique used to achieve fusion by compressing a small target containing fusion fuel to extremely high densities and temperatures using lasers or other methods.The implosion plasma drive fusion pellet concept involves using a small pellet of deuterium and tritium(two isotopes of hydrogen)as fusion fuel,and then rapidly heating and compressing it using a pulsed power system.The implosion process creates a high-pressure plasma that ignites the fusion reactions,releasing energy in the form of neutrons and charged particles.The resulting energy can be captured and used for power generation.This technology is still in the experimental stage,and significant research and development is required to make it commercially viable.However,it has the potential to provide a virtually limitless source of clean energy with no greenhouse gas emissions or long-term radioactive waste.Be that as it may,ICF has to get exact control of the implosion process,mitigate insecurities,and create modern materials and advances to resist the extraordinary conditions of the combined response.