Sustainable nitrogen fixation driven by renewable energy sources under mild conditions has been widely sought to replace the industrial Haber-Bosch process.The fixation of nitrogen in the form of NO_(x)^(-)and NH_4^(+...Sustainable nitrogen fixation driven by renewable energy sources under mild conditions has been widely sought to replace the industrial Haber-Bosch process.The fixation of nitrogen in the form of NO_(x)^(-)and NH_4^(+)into aqueous solutions using electricity-driven gas-liquid discharge plasma is considered a promising prescription.In this paper,a scalable bubble discharge excited by nanosecond pulse power is employed for nitrogen fixation in the liquid phase.The nitrogen fixation performance and the mechanisms are analyzed by varying the power supply parameters,working gas flow rate and composition.The results show that an increase in voltage and frequency can result in an enhanced NO_(3)^(-)yield.Increases in the gas flow rate can result in inadequate activation of the working gas,which together with more inefficient mass transfer efficiencies can reduce the yield.The addition of O_(2) effectively elevates NO_(3)^(-)production while simultaneously inhibiting NH_4^(+) production.The addition of H_(2)O vapor increases the production of OH and H,thereby promoting the generation of reactive nitrogen and enhancing the yield of nitrogen fixation.However,the excessive addition of O_(2) and H_(2)O vapor results in negative effect on the yield of nitrogen fixation,due to the significant weakening of the discharge intensity.The optimal nitrogen fixation yield was up to 16.5 μmol/min,while the optimal energy consumption was approximately 21.3 MJ/mol in this study.Finally,the mechanism related to nitrogen fixation is discussed through the optical emission spectral(OES) information in conjunction with the simulation of energy loss paths in the plasma by BOLSIG+.The work advances knowledge of the effect of parameter variations on nitrogen fixation by gas-liquid discharge for higher yield and energy production.展开更多
Gas-solid fluidized beds have found extensive utilization in frontline manufacturing,in particular as low-velocity beds.The fluidization status,the bubbling or turbulent flow regime and the transition in between,deter...Gas-solid fluidized beds have found extensive utilization in frontline manufacturing,in particular as low-velocity beds.The fluidization status,the bubbling or turbulent flow regime and the transition in between,determine the system performance in practical applications.Though the convoluted hydrodynamics are quantitively evaluated through numerous data-processing methodologies,none of them alone can reflect all the critical information to identify the transition from the bubbling to the turbulent regime.Accordingly,this study was to exploit a coupling data processing methodology,in the combination of standard deviation,power spectrum density,probability density function,wavelet transform,and wavelet multiresolution method,to jointly explain the micro-flow structure at the regime transition from bubbling to turbulent fluidization.The transient differential pressure fluctuation was measured for the evaluation in a fluidized bed(0.267 m i.d.×2.5 m height)with FCC catalysts(d_(p)=65μm,ρ_(p)=1780kg/m^(3))at different superficial gas velocities(0.02–1.4 m/s).The results show that the onset of turbulent fluidization starts earlier in the top section of the bed than in the bottom section.The wavelet decomposition displays that the fluctuation of differential pressure mainly concentrates on the sub-signals with an intermediate frequency band.These sub-signals could be synthesized into three types of scales(micro-scale,meso-scale,and macro-scale),representing the multi-scale hydrodynamics in the fluidized bed.The micro-scale signal has the characteristic information of bubbling fluidization,and the characteristic information of turbulent fluidization is mainly represented by the meso-scale signal.This work provides a systematic comprehension of fluidization status assessment and serves as an impetus for more coupling analysis in this sector.展开更多
To the Editor:Patients with severe persistent asthma experience greater morbidity with more impairment in quality of life despite higher use of health care resources and being treated with existing asthma treatments s...To the Editor:Patients with severe persistent asthma experience greater morbidity with more impairment in quality of life despite higher use of health care resources and being treated with existing asthma treatments such as inhaled corticosteroids and b-agonists,and sometimes oral corticosteroid(OCS)therapy.Type-2(T2)high asthma has been identified as a phenotype that responds to targeted T2 biologic therapies such as anti-IgE,anti-interleukin(IL)5,or anti-IL5Ra and anti-IL4Ra monoclonal antibodies,which are currently available in Europe and North America,and are currently introduced in the rest of the world.[1]展开更多
A facile synthetic strategy was developed for insitu preparation of two-dimensional (2D)highly crystalline tungsten nitride (WN)nanosheets with controllable morphology as oxygen reduction reaction (ORR)catalysts.The d...A facile synthetic strategy was developed for insitu preparation of two-dimensional (2D)highly crystalline tungsten nitride (WN)nanosheets with controllable morphology as oxygen reduction reaction (ORR)catalysts.The dependence of the crystal structure and morphology of WN on K2SO4content,pH,and pyrolysis temperature was thoroughly examined.The electrocatalytic performance of WN toward ORR in an alkaline electrolyte indicated that K+plays an important role in the control of size and shape in the hydrothermal and nitridation process,thereby promoting the formation of plate-like WO3and 2D WN nanosheets.The WN nanosheets,with largely exposed edge sites,provide abundant catalytic active sites and allow fast charge transfer.Furthermore,they exhibit high stability for ORR and methanol tolerance.展开更多
基金National Natural Science Foundation of China (Grant Nos. 52277151 and 51907088)。
文摘Sustainable nitrogen fixation driven by renewable energy sources under mild conditions has been widely sought to replace the industrial Haber-Bosch process.The fixation of nitrogen in the form of NO_(x)^(-)and NH_4^(+)into aqueous solutions using electricity-driven gas-liquid discharge plasma is considered a promising prescription.In this paper,a scalable bubble discharge excited by nanosecond pulse power is employed for nitrogen fixation in the liquid phase.The nitrogen fixation performance and the mechanisms are analyzed by varying the power supply parameters,working gas flow rate and composition.The results show that an increase in voltage and frequency can result in an enhanced NO_(3)^(-)yield.Increases in the gas flow rate can result in inadequate activation of the working gas,which together with more inefficient mass transfer efficiencies can reduce the yield.The addition of O_(2) effectively elevates NO_(3)^(-)production while simultaneously inhibiting NH_4^(+) production.The addition of H_(2)O vapor increases the production of OH and H,thereby promoting the generation of reactive nitrogen and enhancing the yield of nitrogen fixation.However,the excessive addition of O_(2) and H_(2)O vapor results in negative effect on the yield of nitrogen fixation,due to the significant weakening of the discharge intensity.The optimal nitrogen fixation yield was up to 16.5 μmol/min,while the optimal energy consumption was approximately 21.3 MJ/mol in this study.Finally,the mechanism related to nitrogen fixation is discussed through the optical emission spectral(OES) information in conjunction with the simulation of energy loss paths in the plasma by BOLSIG+.The work advances knowledge of the effect of parameter variations on nitrogen fixation by gas-liquid discharge for higher yield and energy production.
基金support from the China Scholarship Council Foundation,and the Science Foundation of China University of Petroleum,Beijing(grant No.2462015YQ0301)。
文摘Gas-solid fluidized beds have found extensive utilization in frontline manufacturing,in particular as low-velocity beds.The fluidization status,the bubbling or turbulent flow regime and the transition in between,determine the system performance in practical applications.Though the convoluted hydrodynamics are quantitively evaluated through numerous data-processing methodologies,none of them alone can reflect all the critical information to identify the transition from the bubbling to the turbulent regime.Accordingly,this study was to exploit a coupling data processing methodology,in the combination of standard deviation,power spectrum density,probability density function,wavelet transform,and wavelet multiresolution method,to jointly explain the micro-flow structure at the regime transition from bubbling to turbulent fluidization.The transient differential pressure fluctuation was measured for the evaluation in a fluidized bed(0.267 m i.d.×2.5 m height)with FCC catalysts(d_(p)=65μm,ρ_(p)=1780kg/m^(3))at different superficial gas velocities(0.02–1.4 m/s).The results show that the onset of turbulent fluidization starts earlier in the top section of the bed than in the bottom section.The wavelet decomposition displays that the fluctuation of differential pressure mainly concentrates on the sub-signals with an intermediate frequency band.These sub-signals could be synthesized into three types of scales(micro-scale,meso-scale,and macro-scale),representing the multi-scale hydrodynamics in the fluidized bed.The micro-scale signal has the characteristic information of bubbling fluidization,and the characteristic information of turbulent fluidization is mainly represented by the meso-scale signal.This work provides a systematic comprehension of fluidization status assessment and serves as an impetus for more coupling analysis in this sector.
基金supported by grants from AstraZeneca,China,and the National Natural Science Foundation of China(No.82070026).
文摘To the Editor:Patients with severe persistent asthma experience greater morbidity with more impairment in quality of life despite higher use of health care resources and being treated with existing asthma treatments such as inhaled corticosteroids and b-agonists,and sometimes oral corticosteroid(OCS)therapy.Type-2(T2)high asthma has been identified as a phenotype that responds to targeted T2 biologic therapies such as anti-IgE,anti-interleukin(IL)5,or anti-IL5Ra and anti-IL4Ra monoclonal antibodies,which are currently available in Europe and North America,and are currently introduced in the rest of the world.[1]
基金supported by the National Natural Science Foundation of China(21306119)the Key Research and Development Projects in Sichuan Province(2017GZ0397,2017CC0017)the Science and Technology Project of Chengdu(2015-HM01-00531-SF)
文摘A facile synthetic strategy was developed for insitu preparation of two-dimensional (2D)highly crystalline tungsten nitride (WN)nanosheets with controllable morphology as oxygen reduction reaction (ORR)catalysts.The dependence of the crystal structure and morphology of WN on K2SO4content,pH,and pyrolysis temperature was thoroughly examined.The electrocatalytic performance of WN toward ORR in an alkaline electrolyte indicated that K+plays an important role in the control of size and shape in the hydrothermal and nitridation process,thereby promoting the formation of plate-like WO3and 2D WN nanosheets.The WN nanosheets,with largely exposed edge sites,provide abundant catalytic active sites and allow fast charge transfer.Furthermore,they exhibit high stability for ORR and methanol tolerance.