A kinetic model is proposed for simulating the trajectory of a single milling ball in a planetary ball mill, and a model is also proposed for simulating the local energy transfer during the ball milling process under ...A kinetic model is proposed for simulating the trajectory of a single milling ball in a planetary ball mill, and a model is also proposed for simulating the local energy transfer during the ball milling process under no-slip conditions. Based on the kinematics of ball motion, the collision fi＇equency and power are described, and the normal impact forces and effective power are derived from analyses of collision geometry. The Hertzian impact theory is applied to formulate these models after having established some relationships among the geometric, dynamic, and thermophysical parameters. Simulation is carried out based on two models, and the effects of the rotation velocity of the planetary disk Ω and the vial-to-disk speed ratio ω/Ω on other kinetic parameters is investigated. As a result, the optimal ratio ω/Ω to obtain high impact energy in the standard operating condition at Ω = 800 rpm is estimated, and is equal to 1.15.展开更多
The electrocatalytic nitrate reduction reaction (NO_(3)RR) powered by renewable energy offers a promising approach for simultaneously reutilization of nitrate and synthesizing high-value products.Nevertheless,theoreti...The electrocatalytic nitrate reduction reaction (NO_(3)RR) powered by renewable energy offers a promising approach for simultaneously reutilization of nitrate and synthesizing high-value products.Nevertheless,theoretical understanding of reaction mechanism was relative illusive,which is indispensable to rationally design of efficient catalysts.Besides,tuning the reaction microenvironment along with the scale-up device development is essential to promote the industrial deployment of electrocatalytic nitrate conversion,while relative research was overlooked.In this regard,recent advances in ammonia synthesis are firstly summarized,including the identification of active sites,exploration of the underlying reaction mechanisms,electrolyzer design and technical-economic analysis.Furthermore,electrocatalytic C–N coupling based on NO_(3)RR to produce higher-value products such as urea and amino acids are also reviewed,to extend the application potential and economic feasibility.Finally,we highlight the existing challenges and the demand of future research for NO_(3)RR.This review anticipates to provide insights into synthesis of high-value products via NO_(3)RR,bridging the gap from laboratory research to industrial fabrication.展开更多
Petroleum coke and lignite are two important fossil fuels that have not been widely used in China. Petroleum coke-lignite slurry （PCLS）, a mixture of petro- leum coke, lignite, water, and additives, efficiently util...Petroleum coke and lignite are two important fossil fuels that have not been widely used in China. Petroleum coke-lignite slurry （PCLS）, a mixture of petro- leum coke, lignite, water, and additives, efficiently utilizes the two materials. In this study, we investigate the effects of the proportion （7） of petroleum coke on slurryability, rheo- logical behavior, stability, and increasing temperature characteristics of PCLSs. The results show that the fixed- viscosity solid concentration （COo） increases with increasing 7. The ~Oo of lignite-water slurry （LWS, ~ = 0） is 46.7 %, compared to 71.3 % for the petroleum coke-water slurry （PCWS, c~ --- i00 %）, while that of PCLS is in between the two values. The rheological behavior of PCLS perfectly fits the power-law model. The PCWS acts as a dilatant fluid. As decreases, the slurry behaves first as an approximate Newtonian fluid, and then turns into a pseudo-plastic fluid that exhibits shear-thinning behavior. With increasing ct, the rigid sedimentation and water separation ratio （WSR） increase, indicating a decrease in the stability of PCLS. When α is 60-70 %, the result is a high-quality slurry fuel for industrial applications, which has high slurryability （ω0 = 57-60 %）, good stability （WSR 〈 2 %）, and superior pseudo-plastic behavior （n = 0.9）.展开更多
Photothermal membrane distillation(MD)is a promising technology for desalination and water purification.However,solar-thermal conversion suffers from low energy efficiency(a typical solar-water efficiency of ~50%),whi...Photothermal membrane distillation(MD)is a promising technology for desalination and water purification.However,solar-thermal conversion suffers from low energy efficiency(a typical solar-water efficiency of ~50%),while complex modifications are needed to reduce membrane fouling.Here,we demonstrate a new concept of solar vapour gap membrane distillation(SVGMD)synergistically combining self-guided water transport,localized heating,and separation of membrane from feed solution.A free-standing,multifunctional light absorber based on graphene array is custom-designed to locally heat the thin water layer transporting through graphene nanochannels.The as-generated vapour passes through a gap and condenses,while salt/contaminants are rejected before reaching the membrane.The high solar-water efficiency(73.4% at 1 sun),clean water collection ratio(82.3%),excellent anti-fouling performance,and stable permeate flux in continuous operation over 72 h are simultaneously achieved.Meanwhile,SVGMD inherits the advantage of MD in microorganism removal and water collection,enabling the solar-water efficiency 3.5 times higher compared to state-of-the-art solar vapour systems.A scaled system to treat oil/seawater mixtures under natural sunlight is developed with a purified water yield of 92.8 kg m-2 day-1.Our results can be applied for diverse mixed-phase feeds,leading to the next-generation solar-driven MD technology.展开更多
We investigate the viscosity of silicon dioxide nanofluid at different particle sizes and pH values considering nanoparticle aggregation. The experimental and simulation results indicate that nanoparticle size is of c...We investigate the viscosity of silicon dioxide nanofluid at different particle sizes and pH values considering nanoparticle aggregation. The experimental and simulation results indicate that nanoparticle size is of crucial importance to the viscosity of the nanofluid due to aggregation. As the nanoparticle size decreases, the viscosity becomes much more dependent on the volume fraction. Moreover, when the nanoparticle diameter is smaller than 2Ohm, the viscosity is closely related to the pH of the nanofluid, and fluctuates with pH values from 5 and 7.展开更多
Hydrazine oxidation reaction(HzOR)assisted hydrogen evolution reaction(HER)offers a feasible path for low power consumption to hydrogen production.Unfortunately however,the total electrooxidation of hydrazine in anode...Hydrazine oxidation reaction(HzOR)assisted hydrogen evolution reaction(HER)offers a feasible path for low power consumption to hydrogen production.Unfortunately however,the total electrooxidation of hydrazine in anode and the dissociation kinetics of water in cathode are critically depend on the interaction between the reaction intermediates and surface of catalysts,which are still challenging due to the totally different catalytic mechanisms.Herein,the[W–O]group with strong adsorption capacity is introduced into CoP nanoflakes to fabricate bifunctional catalyst,which possesses excellent catalytic performances towards both HER(185.60 mV at 1000 mA cm^(−2))and HzOR(78.99 mV at 10,00 mA cm^(−2))with the overall electrolyzer potential of 1.634 V lower than that of the water splitting system at 100 mA cm^(−2).The introduction of[W–O]groups,working as the adsorption sites for H2O dissociation and N2H4 dehydrogenation,leads to the formation of porous structure on CoP nanoflakes and regulates the electronic structure of Co through the linked O in[W–O]group as well,resultantly boosting the hydrogen production and HzOR.Moreover,a proof-of-concept direct hydrazine fuel cell-powered H_(2) production system has been assembled,realizing H_(2)evolution at a rate of 3.53 mmol cm^(−2)h^(−1)at room temperature without external electricity supply.展开更多
Electric double-layer capacitors(EDLCs) are advanced electrochemical devices for energy storage and have attracted strong interest due to their outstanding properties. Rational optimization of electrode–electrolyte i...Electric double-layer capacitors(EDLCs) are advanced electrochemical devices for energy storage and have attracted strong interest due to their outstanding properties. Rational optimization of electrode–electrolyte interactions is of vital importance to enhance device performance for practical applications. Molecular dynamics(MD) simulations could provide theoretical guidelines for the optimal design of electrodes and the improvement of capacitive performances, e.g., energy density and power density. Here we discuss recent MD simulation studies on energy storage performance of electrode materials containing porous to nanostructures. The energy storage properties are related to the electrode structures, including electrode geometry and electrode modifications. Altering electrode geometry, i.e., pore size and surface topography,can influence EDL capacitance. We critically examine different types of electrode modifications, such as altering the arrangement of carbon atoms, doping heteroatoms and defects, which can change the quantum capacitance. The enhancement of power density can be achieved by the intensified ion dynamics and shortened ion pathway.Rational control of the electrode morphology helps improve the ion dynamics by decreasing the ion diffusion pathway. Tuning the surface properties(e.g., the affinity between the electrode and the ions) can affect the ionpacking phenomena. Our critical analysis helps enhance the energy and power densities of EDLCs by modulating the corresponding electrode structures and surface properties.展开更多
In this work, a novel direct current （DC） atmospheric pressure rotating gliding arc （RGA） plasma reactor has been developed for plasma-assisted chemical reactions. The influence of the gas composition and the gas ...In this work, a novel direct current （DC） atmospheric pressure rotating gliding arc （RGA） plasma reactor has been developed for plasma-assisted chemical reactions. The influence of the gas composition and the gas flow rate on the arc dynamic behaviour and the formation of reactive species in the N2 and air gliding arc plasmas has been investigated by means of electrical signals, high speed photography, and optical emission spectroscopic diagnostics. Compared to conventional gliding arc reactors with knife-shaped electrodes which generally require a high flow rate （e.g., 10-20 L/min） to maintain a long arc length and reasonable plasma discharge zone, in this RGA system, a lower gas flow rate （e.g., 2 L/min） can also generate a larger effective plasma reaction zone with a longer arc length for chemical reactions. Two different motion patterns can be clearly observed in the N2 and air RGA plasmas. The time-resolved arc voltage signals show that three different arc dynamic modes, the arc restrike mode, takeover mode, and combined modes, can be clearly identified in the RGA plasmas. The occurrence of different motion and arc dynamic modes is strongly dependent on the composition of the working gas and gas flow rate.展开更多
In this study, the effects of particle size distribution （PSD）, chemical composition and pore structure of petroleum coke on the slurryability of petroleum coke water slurry （PCWS） were investigated. Four petroleu...In this study, the effects of particle size distribution （PSD）, chemical composition and pore structure of petroleum coke on the slurryability of petroleum coke water slurry （PCWS） were investigated. Four petroleum cokes were studied, and they showed completely different slurryability. The solid concentration at fixed viscosity （i.e. apparent viscosity of 1000 mPa） （SCFV） of four PCWSs is different from each other, with the highest value of 70.9%, and lowest of 62.1%. The apparent viscosity of the four PCWSs all increased with an increase of the solid concentration. The results showed that the PSD, inherent moisture content, specific surface area and pore volume of petroleum coke were key factors to affect the slurryability. The slurryability was enhanced with increasing PSD range and particle packing fraction, and with decreasing inherent moisture content, specific surface area and pore volume.展开更多
In this Letter we outline a dielectric multilayer spectrally selective filter designed for solar energy applications.The optical performance of this 78-layer interference filter constructed by TiOx and SiO_(2) is pres...In this Letter we outline a dielectric multilayer spectrally selective filter designed for solar energy applications.The optical performance of this 78-layer interference filter constructed by TiOx and SiO_(2) is presented.A hybrid system combining photovoltaic cells with a solar-powered Stirling engine using the designed filter is analyzed.The calculated results show the advantages of this spectrally selective method for solar power generation.展开更多
Metal-Organic Frameworks(MOFs)have been developed as solid sorbents for CO_(2) capture applications and their properties can be controlled by tuning the chemical blocks of their crystalline units.A number of MOFs(e.g....Metal-Organic Frameworks(MOFs)have been developed as solid sorbents for CO_(2) capture applications and their properties can be controlled by tuning the chemical blocks of their crystalline units.A number of MOFs(e.g.,HKUST-1)have been developed but the question remains how to deploy them for gas-solid contact.Unfortunately,the direct use of MOFs as nanocrystals would lead to serious problems and risks.Here,for the first time,we report a novel MOF-based hybrid sorbent that is produced via an innovative in-situ microencapsulated synthesis.Using a custom-made double capillary microfluidic assembly,double emulsions of the MOF precursor solutions and UV-curable silicone shell fluid are produced.Subsequently,HKUST-1 MOF is successfully synthesized within the droplets enclosed in the gas permeable microcapsules.The developed MOF-bearing microcapsules uniquely allow the deployment of functional nanocrystals without the challenge of handling ultrafine particles,and further,can selectively reject undesired compounds to protect encapsulated MOFs.展开更多
In this work, a plasma-solution system was applied to the degradation of Acid Orange 7 （AO？）. The effects of initial concentration and type of feed gases （air, oxygen, nitrogen or argon） were studied. As the init...In this work, a plasma-solution system was applied to the degradation of Acid Orange 7 （AO？）. The effects of initial concentration and type of feed gases （air, oxygen, nitrogen or argon） were studied. As the initial concentration increased from 100 mg/L to 160 mg/L, the discolouration rate of AO7 decreased from 99.3% to 95.9%, whereas the COD removal rate decreased from 37.9% to 22.6%. Air provided the best discolouration and COD removal rates （99.3% and 3？.9%, respectively）. In the presence of a zero-valent iron （ZVI） catalyst, the AO？ COD removal rate increased to 76.4%. The degradation products were analysed by a GC-MS, revealing that the degradation of the dye molecule was initiated through the cleavage of the -N=N- bond before finally being converted to organic acids.展开更多
Several typical ash samples from a 0.25 MW test furnace fired black liquor coal slurry were selected for investigation. The phases and compounds containing sodium in ash samples were acquired from X-ray diffraction an...Several typical ash samples from a 0.25 MW test furnace fired black liquor coal slurry were selected for investigation. The phases and compounds containing sodium in ash samples were acquired from X-ray diffraction analyses. As well, detailed analyses of the amounts of major mineral elements along thickness gradients of representative ash samples were carried out. The elements, including Na, Si, A1, S and C1 were analyzed by the advanced electron probe microanalyzer equipment, which provid evidence and interpretation for the analytical results of XRD. The findings indicate that the occurrence form of sodium has experi- enced important changes during the combustion of black liquor coal slurry, which translated into nepheline, thenardite, sodium sulfate, sodium chloride, sodium silicoaluminate, hanyne and other phases containing sodium, from NaOH, Na2CO3 and Na2S in raw fuel. Of all the sodium compounds, nepheline, thenardite and sodium sulfate are the most important forms of Na in solid com- bustion residues. Such a transformation of Na during the combustion of black liquor coal slurry resulted in a considerable impact on ash deposition and is not only different from the raw coal and papermaldng black liquors, but is also affected by local circum- stances in the combustion furnace. Amounts of Na, S and C1 in ash deposits from low temperature zones were larger than those from high temperature zones. Our findings should provide important theoretical instructions for industrial applications of black liquor coal slurry.展开更多
This paper presents a reconstruction model of three-dimensional temperature distribution in furnace based on radiative energy images captured by charge-coupled device （CCD） cameras within the visible wavelength rang...This paper presents a reconstruction model of three-dimensional temperature distribution in furnace based on radiative energy images captured by charge-coupled device （CCD） cameras within the visible wavelength range. Numerical simulation case was used in this study and a zigzag eccentric temperature distribution was assumed to verify the model. Least square QR-factorization （LSQR） method was introduced to deal with reconstruction equation. It is found that the reconstructed temperature distributions in low-temperature areas had some fluctuations and high-temperature areas were reconstructed well. The whole reconstruction relative error was mainly due to errors in low-temperature areas and the relative error for highest-temperature reconstruction was quite small.展开更多
The effects of feed gas flow rate and operating current on the electrical characteristics and dynamic behavior of a rotating gliding arc （RGA） plasma codriven by a magnetic field and tangential flow were investigate...The effects of feed gas flow rate and operating current on the electrical characteristics and dynamic behavior of a rotating gliding arc （RGA） plasma codriven by a magnetic field and tangential flow were investigated.The operating current has been shown to significantly affect the time-resolved voltage waveforms of the discharge,particularly at flow rate =21 min^-1.When the current was lower than 140 mA,sinusoidal waveforms with regular variation periods of 13.5-17.0 ms can be observed （flow rate =21 min^-1）.The restrike mode characterized by serial sudden drops of voltage appeared under all studied conditions.Increasing the flow rate from 8 to 121 min^-1 （at the same current） led to a shift of arc rotation mode which would then result in a significant drop of discharge voltage （around 120-200 V）.For a given flow rate,the reduction of current resulted in a nearly linear increase of voltage.展开更多
The electrical and plasma parameters of a low pressure inductively coupled argon plasma are investigated over a wide range of parameters（RF power, flow rate and pressure） by diverse characterizations. The external a...The electrical and plasma parameters of a low pressure inductively coupled argon plasma are investigated over a wide range of parameters（RF power, flow rate and pressure） by diverse characterizations. The external antenna voltage and current increase with the augment of RF power, whereas decline with the enhancement of gas pressure and flow rate conversely.Compared with gas flow rate and pressure, the power transfer efficiency is significantly improved by RF power, and achieved its maximum value of 0.85 after RF power injected excess125 W. Optical emission spectroscopy（OES） provides the local mean values of electron excited temperature and electron density in inductively coupled plasma（ICP） post regime, which vary in a range of 0.81 eV to 1.15 eV and 3.7×10^（16）m^（-3）to 8.7×10^（17）m^（-3）respectively. Numerical results of the average magnitudes of electron temperature and electron density in twodimensional distribution exhibit similar variation trend with the experimental results under different operating condition by using COMSOL Multiphysics. By comprehensively understanding the characteristics in a low pressure ICP, optimized operating conditions could be anticipated aiming at different academic and industrial applications.展开更多
Ozone production utilizing surface dielectric barrier discharge（SDBD） was experimental studied for different flow patterns considering the influences of transversal flow, lateral flow and different lateral flow posi...Ozone production utilizing surface dielectric barrier discharge（SDBD） was experimental studied for different flow patterns considering the influences of transversal flow, lateral flow and different lateral flow positions. Results show that the flow patterns have a remarkable impact on the ozone yield by affecting the uniformity and turbulence of gas flow. Meanwhile, distributing the O2 flow rate according to the intensity of the plasma reaction would also increase the generation efficiency of SDBD for ozone production. By improving the uniformity and introducing the lateral flow to the transversal flow, the highest ozone yield was obtained in flow pattern ‘F’. In this case, the ozone yield increased by 28.4% to 131 g kWh-1 from 102.8 g k Wh-1 in flow pattern ‘A’.展开更多
The use of atmospheric rotating gliding arc(RGA)plasma is proposed as a facile,scalable and catalyst-free approach to synthesizing hydrogen(H2)and graphene sheets from coalbed methane(CBM).CH4 is used as a CBM surroga...The use of atmospheric rotating gliding arc(RGA)plasma is proposed as a facile,scalable and catalyst-free approach to synthesizing hydrogen(H2)and graphene sheets from coalbed methane(CBM).CH4 is used as a CBM surrogate.Based on a previous investigation of discharge properties,product distribution and energy efficiency,the operating parameters such as CH4 concentration,applied voltage and gas flow rate can effectively affect the CH4 conversion rate,the selectivity of H2 and the properties of solid generated carbon.Nevertheless,the basic properties of RGA plasma and its role in CH4 conversion are scarcely mentioned.In the present work,a 3D RGA model,with a detailed nonequilibrium CH4/Ar plasma chemistry,is developed to validate the previous experiments on CBM conversion,aiming in particular at the distribution of H2 and other gas products.Our results demonstrate that the dynamics of RGA is derived from the joint effects of electron convection,electron migration and electron diffusion,and is prominently determined by the variation of the gas flow rate and applied voltage.Subsequently,a combined experimental and chemical kinetical simulation is performed to analyze the selectivity of gas products in an RGA reaction,taking into consideration the formation and loss pathways of crucial targeted substances(such as CH4,C2H2,H2 and H radicals)and corresponding contribution rates.Additionally,the effects of operating conditions on the properties of solid products are investigated by scanning electron microscopy(SEM)and Raman spectroscopy.The results show that increasing the applied voltage and decreasing CH4 concentration will change the solid carbon from its initial spherical structure into folded multilayer graphene sheets,while the size of the graphene sheets is slightly affected by the change in gas flow rate.展开更多
One-step controllable synthesis of vertical graphene nanosheets （VGs） and high-value gases was achieved using inductively coupled plasma enhanced chemical vapor deposition （ICPECVD）. The basic physical properties ...One-step controllable synthesis of vertical graphene nanosheets （VGs） and high-value gases was achieved using inductively coupled plasma enhanced chemical vapor deposition （ICPECVD）. The basic physical properties of the ICPECVD process were revealed via electrical diagnosis and optical emission spectroscopy. The coil current and voltage increased linearly with the augmenting of injected power, and CH, C2, H2 and H were detected at a wavelength from 300 to 700 nm, implying the generation of abundant graphene-building species. The morphology and structure of solid carbon products, graphene nanosheets, were systemically characterized in terms of the variations of operating conditions, such as pressure, temperature, gas proportion, etc. The results indicated that an appropriate operating condition was indispensable for the growth process of graphene nanosheets. In the present work, the optimized result was achieved at the pressure, heating temperature, applied power and gas proportion of 600 mTorr, 800 ~C, 500 W and 20：20：15, respectively, and the augmenting of both CH4 and H2 concentrations had a positive effect on the etching of amorphous carbon. Additionally, H2 and C2 hydrocarbons were detected as the main exhaust gases. The selectivity of H2 and C2H2, measured in exhaust gases, reached up to 52% and 8%, respectively, which implied a process of free radical reactions and electron collision dissociation. Based on a comprehensive investigation of spectral and electrical parameters and synthesized products, the reaction mechanism of collision, dissociation, diffusion, etc, in ICPECVD could be speculated, providing a probable guide for experimental and industrial applications.展开更多
Solid-state polymer electrolytes(SPEs)have attracted increasing attention due to good interfacial contact,light weight,and easy manufacturing.However,the practical application of SPEs such as the most widely studied p...Solid-state polymer electrolytes(SPEs)have attracted increasing attention due to good interfacial contact,light weight,and easy manufacturing.However,the practical application of SPEs such as the most widely studied poly(ethylene oxide)(PEO)in high-energy solid polymer batteries is still challenging,and the reasons are yet elusive.Here,it is found that the mismatch between PEO and 4.2 V-class cathodes is beyond the limited electrochemical window of PEO in the solid Li Ni_(1/3)Mn_(1/3)Co_(1/3)O_(2)(NMC)-PEO batteries.The initial oxidation of PEO initiates remarkable surface reconstruction of NMC grains in solid batteries that are different from the situation in liquid electrolytes.Well-aligned nanovoids are observed in NMC grains during the diffusion of surface reconstruction layers towards the bulk in solid batteries.The substantial interphasial degradation,therefore,blocks smooth Li+transport across the NMC-PEO interface and causes performance degradation.A thin yet effective Li F-containing protection layer on NMC can effectively stabilize the NMC-PEO interface with a greatly improved lifespan of NMC|PEO|Li batteries.This work deepens the understanding of degradations in high-voltage solid-state polymer batteries.展开更多
基金Project supported by the Major State Basic Research Development Program of China (Grant No. 2011CB201500)the Science and Technology Project of Zhejiang Province, China (Grant No. 2009C13004)+2 种基金the National Key Technology R&D Program of China(Grant No. 2007BAC27B04-4)the Program of Introducing Talents of Disciplinary to University, China (Grant No. B08026)Y. C. Tang Disciplinary Development Fund of Zhejiang University, China
文摘A kinetic model is proposed for simulating the trajectory of a single milling ball in a planetary ball mill, and a model is also proposed for simulating the local energy transfer during the ball milling process under no-slip conditions. Based on the kinematics of ball motion, the collision fi＇equency and power are described, and the normal impact forces and effective power are derived from analyses of collision geometry. The Hertzian impact theory is applied to formulate these models after having established some relationships among the geometric, dynamic, and thermophysical parameters. Simulation is carried out based on two models, and the effects of the rotation velocity of the planetary disk Ω and the vial-to-disk speed ratio ω/Ω on other kinetic parameters is investigated. As a result, the optimal ratio ω/Ω to obtain high impact energy in the standard operating condition at Ω = 800 rpm is estimated, and is equal to 1.15.
基金the support from Key R&D Program of Zhejiang(2024SSYS0064)the Fundamental Research Funds for the Central Universities (2022ZFJH04)。
文摘The electrocatalytic nitrate reduction reaction (NO_(3)RR) powered by renewable energy offers a promising approach for simultaneously reutilization of nitrate and synthesizing high-value products.Nevertheless,theoretical understanding of reaction mechanism was relative illusive,which is indispensable to rationally design of efficient catalysts.Besides,tuning the reaction microenvironment along with the scale-up device development is essential to promote the industrial deployment of electrocatalytic nitrate conversion,while relative research was overlooked.In this regard,recent advances in ammonia synthesis are firstly summarized,including the identification of active sites,exploration of the underlying reaction mechanisms,electrolyzer design and technical-economic analysis.Furthermore,electrocatalytic C–N coupling based on NO_(3)RR to produce higher-value products such as urea and amino acids are also reviewed,to extend the application potential and economic feasibility.Finally,we highlight the existing challenges and the demand of future research for NO_(3)RR.This review anticipates to provide insights into synthesis of high-value products via NO_(3)RR,bridging the gap from laboratory research to industrial fabrication.
基金the National Basic Research Program of China (Grant No. 2010CB227001)
文摘Petroleum coke and lignite are two important fossil fuels that have not been widely used in China. Petroleum coke-lignite slurry （PCLS）, a mixture of petro- leum coke, lignite, water, and additives, efficiently utilizes the two materials. In this study, we investigate the effects of the proportion （7） of petroleum coke on slurryability, rheo- logical behavior, stability, and increasing temperature characteristics of PCLSs. The results show that the fixed- viscosity solid concentration （COo） increases with increasing 7. The ~Oo of lignite-water slurry （LWS, ~ = 0） is 46.7 %, compared to 71.3 % for the petroleum coke-water slurry （PCWS, c~ --- i00 %）, while that of PCLS is in between the two values. The rheological behavior of PCLS perfectly fits the power-law model. The PCWS acts as a dilatant fluid. As decreases, the slurry behaves first as an approximate Newtonian fluid, and then turns into a pseudo-plastic fluid that exhibits shear-thinning behavior. With increasing ct, the rigid sedimentation and water separation ratio （WSR） increase, indicating a decrease in the stability of PCLS. When α is 60-70 %, the result is a high-quality slurry fuel for industrial applications, which has high slurryability （ω0 = 57-60 %）, good stability （WSR 〈 2 %）, and superior pseudo-plastic behavior （n = 0.9）.
基金supported by the National Natural Science Foundation of China (No. 51722604)the National Program for Support of Top-notch Young Professionals+1 种基金the financial support by the startup funding from the University of Nevadathe Australian Research Council for partial support
文摘Photothermal membrane distillation(MD)is a promising technology for desalination and water purification.However,solar-thermal conversion suffers from low energy efficiency(a typical solar-water efficiency of ~50%),while complex modifications are needed to reduce membrane fouling.Here,we demonstrate a new concept of solar vapour gap membrane distillation(SVGMD)synergistically combining self-guided water transport,localized heating,and separation of membrane from feed solution.A free-standing,multifunctional light absorber based on graphene array is custom-designed to locally heat the thin water layer transporting through graphene nanochannels.The as-generated vapour passes through a gap and condenses,while salt/contaminants are rejected before reaching the membrane.The high solar-water efficiency(73.4% at 1 sun),clean water collection ratio(82.3%),excellent anti-fouling performance,and stable permeate flux in continuous operation over 72 h are simultaneously achieved.Meanwhile,SVGMD inherits the advantage of MD in microorganism removal and water collection,enabling the solar-water efficiency 3.5 times higher compared to state-of-the-art solar vapour systems.A scaled system to treat oil/seawater mixtures under natural sunlight is developed with a purified water yield of 92.8 kg m-2 day-1.Our results can be applied for diverse mixed-phase feeds,leading to the next-generation solar-driven MD technology.
基金Supported by the National Natural Science Foundation of China under Grant No 50676082.
文摘We investigate the viscosity of silicon dioxide nanofluid at different particle sizes and pH values considering nanoparticle aggregation. The experimental and simulation results indicate that nanoparticle size is of crucial importance to the viscosity of the nanofluid due to aggregation. As the nanoparticle size decreases, the viscosity becomes much more dependent on the volume fraction. Moreover, when the nanoparticle diameter is smaller than 2Ohm, the viscosity is closely related to the pH of the nanofluid, and fluctuates with pH values from 5 and 7.
基金support of this research by National Natural Science Foundation of China(52172110)Key Research Program of Frontier Sciences,Chinese Academy of Sciences(ZDBS-LY-SLH029)+1 种基金the“Scientific and Technical Innovation Action Plan”Hong Kong,Macao and Taiwan Science&Technology Cooperation Project of Shanghai Science and Technology Committee(21520760500)BL14W1 beamline of Shanghai Synchrotron Radiation Facility(SSRF).
文摘Hydrazine oxidation reaction(HzOR)assisted hydrogen evolution reaction(HER)offers a feasible path for low power consumption to hydrogen production.Unfortunately however,the total electrooxidation of hydrazine in anode and the dissociation kinetics of water in cathode are critically depend on the interaction between the reaction intermediates and surface of catalysts,which are still challenging due to the totally different catalytic mechanisms.Herein,the[W–O]group with strong adsorption capacity is introduced into CoP nanoflakes to fabricate bifunctional catalyst,which possesses excellent catalytic performances towards both HER(185.60 mV at 1000 mA cm^(−2))and HzOR(78.99 mV at 10,00 mA cm^(−2))with the overall electrolyzer potential of 1.634 V lower than that of the water splitting system at 100 mA cm^(−2).The introduction of[W–O]groups,working as the adsorption sites for H2O dissociation and N2H4 dehydrogenation,leads to the formation of porous structure on CoP nanoflakes and regulates the electronic structure of Co through the linked O in[W–O]group as well,resultantly boosting the hydrogen production and HzOR.Moreover,a proof-of-concept direct hydrazine fuel cell-powered H_(2) production system has been assembled,realizing H_(2)evolution at a rate of 3.53 mmol cm^(−2)h^(−1)at room temperature without external electricity supply.
基金supported by the National Natural Science Foundation of China (No. 51722604)Zhejiang Provincial Natural Science Foundation of China (No. LR17E060002)
文摘Electric double-layer capacitors(EDLCs) are advanced electrochemical devices for energy storage and have attracted strong interest due to their outstanding properties. Rational optimization of electrode–electrolyte interactions is of vital importance to enhance device performance for practical applications. Molecular dynamics(MD) simulations could provide theoretical guidelines for the optimal design of electrodes and the improvement of capacitive performances, e.g., energy density and power density. Here we discuss recent MD simulation studies on energy storage performance of electrode materials containing porous to nanostructures. The energy storage properties are related to the electrode structures, including electrode geometry and electrode modifications. Altering electrode geometry, i.e., pore size and surface topography,can influence EDL capacitance. We critically examine different types of electrode modifications, such as altering the arrangement of carbon atoms, doping heteroatoms and defects, which can change the quantum capacitance. The enhancement of power density can be achieved by the intensified ion dynamics and shortened ion pathway.Rational control of the electrode morphology helps improve the ion dynamics by decreasing the ion diffusion pathway. Tuning the surface properties(e.g., the affinity between the electrode and the ions) can affect the ionpacking phenomena. Our critical analysis helps enhance the energy and power densities of EDLCs by modulating the corresponding electrode structures and surface properties.
基金supported by National Natural Science Foundation of China(No.51576174)the Specialized Research Fund for the Doctoral Program of Higher Education of China(No.20120101110099)the Fundamental Research Funds for the Central Universities(No.2015FZA4011)
文摘In this work, a novel direct current （DC） atmospheric pressure rotating gliding arc （RGA） plasma reactor has been developed for plasma-assisted chemical reactions. The influence of the gas composition and the gas flow rate on the arc dynamic behaviour and the formation of reactive species in the N2 and air gliding arc plasmas has been investigated by means of electrical signals, high speed photography, and optical emission spectroscopic diagnostics. Compared to conventional gliding arc reactors with knife-shaped electrodes which generally require a high flow rate （e.g., 10-20 L/min） to maintain a long arc length and reasonable plasma discharge zone, in this RGA system, a lower gas flow rate （e.g., 2 L/min） can also generate a larger effective plasma reaction zone with a longer arc length for chemical reactions. Two different motion patterns can be clearly observed in the N2 and air RGA plasmas. The time-resolved arc voltage signals show that three different arc dynamic modes, the arc restrike mode, takeover mode, and combined modes, can be clearly identified in the RGA plasmas. The occurrence of different motion and arc dynamic modes is strongly dependent on the composition of the working gas and gas flow rate.
基金the financial support from National Key Basic Research Program Project (No. 2010CB227001)
文摘In this study, the effects of particle size distribution （PSD）, chemical composition and pore structure of petroleum coke on the slurryability of petroleum coke water slurry （PCWS） were investigated. Four petroleum cokes were studied, and they showed completely different slurryability. The solid concentration at fixed viscosity （i.e. apparent viscosity of 1000 mPa） （SCFV） of four PCWSs is different from each other, with the highest value of 70.9%, and lowest of 62.1%. The apparent viscosity of the four PCWSs all increased with an increase of the solid concentration. The results showed that the PSD, inherent moisture content, specific surface area and pore volume of petroleum coke were key factors to affect the slurryability. The slurryability was enhanced with increasing PSD range and particle packing fraction, and with decreasing inherent moisture content, specific surface area and pore volume.
基金Supported by the Research Foundation of Science and Technology Department of Zhejiang Province(2009C21023).
文摘In this Letter we outline a dielectric multilayer spectrally selective filter designed for solar energy applications.The optical performance of this 78-layer interference filter constructed by TiOx and SiO_(2) is presented.A hybrid system combining photovoltaic cells with a solar-powered Stirling engine using the designed filter is analyzed.The calculated results show the advantages of this spectrally selective method for solar power generation.
基金National Science Foundation (CBET 1927336)Saudi Aramco,and the Lenfest Center for Sustainable Energy at the Earth Institute at Columbia University for financially supporting this work+3 种基金performed at GeoSoilEnviroCARS (The University of Chicago,Sector 13)Advanced Photon Source (APS),Argonne National Laboratory.GeoSoilEnviroCARS is supported by the National Science Foundation-Earth Sciences (EAR-1634415)the Department of Energy-GeoSciences (DE-FG02-94ER14466)the Advanced Photon Source,a U.S.Department of Energy (DOE)Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No.DE-AC02-06CH11357.
文摘Metal-Organic Frameworks(MOFs)have been developed as solid sorbents for CO_(2) capture applications and their properties can be controlled by tuning the chemical blocks of their crystalline units.A number of MOFs(e.g.,HKUST-1)have been developed but the question remains how to deploy them for gas-solid contact.Unfortunately,the direct use of MOFs as nanocrystals would lead to serious problems and risks.Here,for the first time,we report a novel MOF-based hybrid sorbent that is produced via an innovative in-situ microencapsulated synthesis.Using a custom-made double capillary microfluidic assembly,double emulsions of the MOF precursor solutions and UV-curable silicone shell fluid are produced.Subsequently,HKUST-1 MOF is successfully synthesized within the droplets enclosed in the gas permeable microcapsules.The developed MOF-bearing microcapsules uniquely allow the deployment of functional nanocrystals without the challenge of handling ultrafine particles,and further,can selectively reject undesired compounds to protect encapsulated MOFs.
基金supported by National Natural Science Foundation of China(Nos.50908237,51076142)the Open Foundation of the State Key Laboratory of Clean Energy Utilization of China(No.ZJUCEU2009008)
文摘In this work, a plasma-solution system was applied to the degradation of Acid Orange 7 （AO？）. The effects of initial concentration and type of feed gases （air, oxygen, nitrogen or argon） were studied. As the initial concentration increased from 100 mg/L to 160 mg/L, the discolouration rate of AO7 decreased from 99.3% to 95.9%, whereas the COD removal rate decreased from 37.9% to 22.6%. Air provided the best discolouration and COD removal rates （99.3% and 3？.9%, respectively）. In the presence of a zero-valent iron （ZVI） catalyst, the AO？ COD removal rate increased to 76.4%. The degradation products were analysed by a GC-MS, revealing that the degradation of the dye molecule was initiated through the cleavage of the -N=N- bond before finally being converted to organic acids.
基金Projects 2004CB217701 supported by the National Basic Research Program of China 2005-1 by the Scientific Research Foundation of the Ministry ofEducation of Hebei Province
文摘Several typical ash samples from a 0.25 MW test furnace fired black liquor coal slurry were selected for investigation. The phases and compounds containing sodium in ash samples were acquired from X-ray diffraction analyses. As well, detailed analyses of the amounts of major mineral elements along thickness gradients of representative ash samples were carried out. The elements, including Na, Si, A1, S and C1 were analyzed by the advanced electron probe microanalyzer equipment, which provid evidence and interpretation for the analytical results of XRD. The findings indicate that the occurrence form of sodium has experi- enced important changes during the combustion of black liquor coal slurry, which translated into nepheline, thenardite, sodium sulfate, sodium chloride, sodium silicoaluminate, hanyne and other phases containing sodium, from NaOH, Na2CO3 and Na2S in raw fuel. Of all the sodium compounds, nepheline, thenardite and sodium sulfate are the most important forms of Na in solid com- bustion residues. Such a transformation of Na during the combustion of black liquor coal slurry resulted in a considerable impact on ash deposition and is not only different from the raw coal and papermaldng black liquors, but is also affected by local circum- stances in the combustion furnace. Amounts of Na, S and C1 in ash deposits from low temperature zones were larger than those from high temperature zones. Our findings should provide important theoretical instructions for industrial applications of black liquor coal slurry.
基金Project supported by the State Key Program of National Natural Science Foundation of China (Grant No 60534030)Program for Changjiang Scholars and Innovative Research Team in University (Grant No IRT0434)
文摘This paper presents a reconstruction model of three-dimensional temperature distribution in furnace based on radiative energy images captured by charge-coupled device （CCD） cameras within the visible wavelength range. Numerical simulation case was used in this study and a zigzag eccentric temperature distribution was assumed to verify the model. Least square QR-factorization （LSQR） method was introduced to deal with reconstruction equation. It is found that the reconstructed temperature distributions in low-temperature areas had some fluctuations and high-temperature areas were reconstructed well. The whole reconstruction relative error was mainly due to errors in low-temperature areas and the relative error for highest-temperature reconstruction was quite small.
基金supported by National Natural Science Foundation of China(51576174)
文摘The effects of feed gas flow rate and operating current on the electrical characteristics and dynamic behavior of a rotating gliding arc （RGA） plasma codriven by a magnetic field and tangential flow were investigated.The operating current has been shown to significantly affect the time-resolved voltage waveforms of the discharge,particularly at flow rate =21 min^-1.When the current was lower than 140 mA,sinusoidal waveforms with regular variation periods of 13.5-17.0 ms can be observed （flow rate =21 min^-1）.The restrike mode characterized by serial sudden drops of voltage appeared under all studied conditions.Increasing the flow rate from 8 to 121 min^-1 （at the same current） led to a shift of arc rotation mode which would then result in a significant drop of discharge voltage （around 120-200 V）.For a given flow rate,the reduction of current resulted in a nearly linear increase of voltage.
基金supported by National Natural Science Foundation of China(No.51576174)
文摘The electrical and plasma parameters of a low pressure inductively coupled argon plasma are investigated over a wide range of parameters（RF power, flow rate and pressure） by diverse characterizations. The external antenna voltage and current increase with the augment of RF power, whereas decline with the enhancement of gas pressure and flow rate conversely.Compared with gas flow rate and pressure, the power transfer efficiency is significantly improved by RF power, and achieved its maximum value of 0.85 after RF power injected excess125 W. Optical emission spectroscopy（OES） provides the local mean values of electron excited temperature and electron density in inductively coupled plasma（ICP） post regime, which vary in a range of 0.81 eV to 1.15 eV and 3.7×10^（16）m^（-3）to 8.7×10^（17）m^（-3）respectively. Numerical results of the average magnitudes of electron temperature and electron density in twodimensional distribution exhibit similar variation trend with the experimental results under different operating condition by using COMSOL Multiphysics. By comprehensively understanding the characteristics in a low pressure ICP, optimized operating conditions could be anticipated aiming at different academic and industrial applications.
基金supported by National Natural Science Foundation of China(No.51776185)Zhejiang Provincial Natural Science Foundation(LR16E060001)
文摘Ozone production utilizing surface dielectric barrier discharge（SDBD） was experimental studied for different flow patterns considering the influences of transversal flow, lateral flow and different lateral flow positions. Results show that the flow patterns have a remarkable impact on the ozone yield by affecting the uniformity and turbulence of gas flow. Meanwhile, distributing the O2 flow rate according to the intensity of the plasma reaction would also increase the generation efficiency of SDBD for ozone production. By improving the uniformity and introducing the lateral flow to the transversal flow, the highest ozone yield was obtained in flow pattern ‘F’. In this case, the ozone yield increased by 28.4% to 131 g kWh-1 from 102.8 g k Wh-1 in flow pattern ‘A’.
基金supported by the Foundation for Innovative Research Groups of National Natural Science Foundation of China (No. 51621005)China Postdoctoral Science Foundation (No. 2018M630672)
文摘The use of atmospheric rotating gliding arc(RGA)plasma is proposed as a facile,scalable and catalyst-free approach to synthesizing hydrogen(H2)and graphene sheets from coalbed methane(CBM).CH4 is used as a CBM surrogate.Based on a previous investigation of discharge properties,product distribution and energy efficiency,the operating parameters such as CH4 concentration,applied voltage and gas flow rate can effectively affect the CH4 conversion rate,the selectivity of H2 and the properties of solid generated carbon.Nevertheless,the basic properties of RGA plasma and its role in CH4 conversion are scarcely mentioned.In the present work,a 3D RGA model,with a detailed nonequilibrium CH4/Ar plasma chemistry,is developed to validate the previous experiments on CBM conversion,aiming in particular at the distribution of H2 and other gas products.Our results demonstrate that the dynamics of RGA is derived from the joint effects of electron convection,electron migration and electron diffusion,and is prominently determined by the variation of the gas flow rate and applied voltage.Subsequently,a combined experimental and chemical kinetical simulation is performed to analyze the selectivity of gas products in an RGA reaction,taking into consideration the formation and loss pathways of crucial targeted substances(such as CH4,C2H2,H2 and H radicals)and corresponding contribution rates.Additionally,the effects of operating conditions on the properties of solid products are investigated by scanning electron microscopy(SEM)and Raman spectroscopy.The results show that increasing the applied voltage and decreasing CH4 concentration will change the solid carbon from its initial spherical structure into folded multilayer graphene sheets,while the size of the graphene sheets is slightly affected by the change in gas flow rate.
基金supported by National Natural Science Foundation of China(No.51576174)China Postdoctoral Science Foundation Funded Project(No.2018M630672)
文摘One-step controllable synthesis of vertical graphene nanosheets （VGs） and high-value gases was achieved using inductively coupled plasma enhanced chemical vapor deposition （ICPECVD）. The basic physical properties of the ICPECVD process were revealed via electrical diagnosis and optical emission spectroscopy. The coil current and voltage increased linearly with the augmenting of injected power, and CH, C2, H2 and H were detected at a wavelength from 300 to 700 nm, implying the generation of abundant graphene-building species. The morphology and structure of solid carbon products, graphene nanosheets, were systemically characterized in terms of the variations of operating conditions, such as pressure, temperature, gas proportion, etc. The results indicated that an appropriate operating condition was indispensable for the growth process of graphene nanosheets. In the present work, the optimized result was achieved at the pressure, heating temperature, applied power and gas proportion of 600 mTorr, 800 ~C, 500 W and 20：20：15, respectively, and the augmenting of both CH4 and H2 concentrations had a positive effect on the etching of amorphous carbon. Additionally, H2 and C2 hydrocarbons were detected as the main exhaust gases. The selectivity of H2 and C2H2, measured in exhaust gases, reached up to 52% and 8%, respectively, which implied a process of free radical reactions and electron collision dissociation. Based on a comprehensive investigation of spectral and electrical parameters and synthesized products, the reaction mechanism of collision, dissociation, diffusion, etc, in ICPECVD could be speculated, providing a probable guide for experimental and industrial applications.
基金supported by the National Natural Science Foundation of China (U21A2075, 22179117)the Fujian Science & Technology Innovation Laboratory for Energy Devices of China (21CLAB) (21C-OP-202107)the Program of Zhejiang University and Program of State Key Laboratory of Clean Energy Utilization at Zhejiang (ZJUCEU2020005)
文摘Solid-state polymer electrolytes(SPEs)have attracted increasing attention due to good interfacial contact,light weight,and easy manufacturing.However,the practical application of SPEs such as the most widely studied poly(ethylene oxide)(PEO)in high-energy solid polymer batteries is still challenging,and the reasons are yet elusive.Here,it is found that the mismatch between PEO and 4.2 V-class cathodes is beyond the limited electrochemical window of PEO in the solid Li Ni_(1/3)Mn_(1/3)Co_(1/3)O_(2)(NMC)-PEO batteries.The initial oxidation of PEO initiates remarkable surface reconstruction of NMC grains in solid batteries that are different from the situation in liquid electrolytes.Well-aligned nanovoids are observed in NMC grains during the diffusion of surface reconstruction layers towards the bulk in solid batteries.The substantial interphasial degradation,therefore,blocks smooth Li+transport across the NMC-PEO interface and causes performance degradation.A thin yet effective Li F-containing protection layer on NMC can effectively stabilize the NMC-PEO interface with a greatly improved lifespan of NMC|PEO|Li batteries.This work deepens the understanding of degradations in high-voltage solid-state polymer batteries.
