Direct methanol fuel cells(DMFC) are widely considered to be an ideal green energy conversion device but their widespread applications are limited by the high price of the Pt-based catalysts and the instability in ter...Direct methanol fuel cells(DMFC) are widely considered to be an ideal green energy conversion device but their widespread applications are limited by the high price of the Pt-based catalysts and the instability in terms of surface CO toxicity in long-term operation.Herein,the PtFe alloy nanoparticles(NPs) with small particle size(~4.12 nm) supported on carbon black catalysts with different Pt/Fe atomic ratios(Pt_(1)Fe_(2)/C,Pt_(3)Fe_(4)/C,Pt_(1)Fe_(1)/C,and Pt_(2)Fe_(1)/C) are successfully prepared for enhanced anti-CO poisoning during methanol oxidation reaction(MOR).The optimal atomic ratio of Pt/Fe for the MOR is 1:2,and the mass activity of Pt_(1)Fe_(2)/C(5.40 A mg_(Pt)^(-1)) is 13.5 times higher than that of conventional commercial Pt/C(Pt/C-JM)(0.40 A mg_(Pt)^(-1)).The introduction of Fe into the Pt lattice forms the PtFe alloy phase,and the electron density of Pt is reduced after forming the PtFe alloy.In-situ Fourier transform infrared results indicate that the addition of oxyphilic metal Fe has reduced the adsorption of reactant molecules on Pt during the MOR.The doping of Fe atoms helps to desorb toxic intermediates and regenerate Pt active sites,promoting the cleavage of C-O bonds with good selectivity of CO_(2)(58.1%).Moreover,the Pt_(1)Fe_(2)/C catalyst exhibits higher CO tolerance,methanol electrooxidation activity,and long-term stability than other Pt_(x)Fe_(y)/C catalysts.展开更多
Metal(aluminum and boron)based energetic materials have been wildly applied in various fields including aerospace,explosives and micro-devices due to their high energy density.Unfortunately,the low combustion efficien...Metal(aluminum and boron)based energetic materials have been wildly applied in various fields including aerospace,explosives and micro-devices due to their high energy density.Unfortunately,the low combustion efficiency and reactivity of metal fuels,especially boron(B),severely limit their practical applications.Herein,multi-component 3D microspheres of HMX/B/Al/PTFE(HBA)have been designed and successfully prepared by emulsion and solvent evaporation method to achieve superior energy and combustion reactivity.The reactivity and energy output of HBA are systematically measured by ignitionburning test,constant-volume explosion vessel system and bomb calorimetry.Due to the increased interfacial contact and reaction area,HBA shows higher flame propagation rate,faster pressurization rate and larger combustion heat of 29.95 cm/s,1077 kPa/s,and 6164.43 J/g,which is 1.5 times,3.5 times,and 1.03 times of the physical mixed counterpart(HBA-P).Meanwhile,HBA also shows enhanced energy output and reactivity than 3D microspheres of HMX/B/PTFE(HB)resulting from the high reactivity of Al.The reaction mechanism of 3D microspheres is comprehensively investigated through combustion emission spectral and thermal analysis(TG-DSC-MS).The superior reactivity and energy of HBA originate from the surface etching of fluorine to the inert shell(Al_(2)O_(3) and B_(2)O_(3))and the initiation effect of Al to B.This work offers a promising approach to design and prepare high-performance energetic materials for the practical applications.展开更多
液滴撞击固体表面是自然界的常见现象,研究超疏水表面的液滴撞击对其润湿性的影响,对于超疏水性材料的潜在应用具有重要的科学意义。采用3、10、20 min氧等离子体处理(OPT)和1 min八氟环丁烷等离子体聚合沉积(PPD)的等离子体方法改性聚...液滴撞击固体表面是自然界的常见现象,研究超疏水表面的液滴撞击对其润湿性的影响,对于超疏水性材料的潜在应用具有重要的科学意义。采用3、10、20 min氧等离子体处理(OPT)和1 min八氟环丁烷等离子体聚合沉积(PPD)的等离子体方法改性聚四氟乙烯(PTFE)表面,获得具有不同尺寸和间距的微/纳米锥的超疏水PTFE表面,研究射频等离子体改性PTFE表面的液滴静态接触角、滚动角及液滴撞击动力学行为,分析在不同个数液滴撞击后PTFE表面的润湿性和液滴撞击行为变化,确定PTFE表面液滴撞击起电效应的影响机制。结果表明:通过1~9个液滴撞击后,PTFE表面的静态接触角随撞击液滴数量增加而减小,导致静态接触角低于150°;液滴滚动角随撞击液滴数量增加而增大,造成液滴滚动角高于10°。撞击液滴的接触时间随撞击液滴数量增加而增大,回弹系数随撞击液滴数量增加而减小。随撞击液滴数量增加,回弹液滴的正电荷和PTFE表面的负电压增大,PTFE表面的负电荷对液滴产生强吸引作用,导致低粘附超疏水性被破坏。3 min OPT和1 min PPD改性PTFE表面的纳米锥间距小,密度大,表面负电荷量增加明显,造成PTFE表面的疏水性降低的程度最显著。研究结果可为改善超疏水稳定性的表面织构设计提供理论依据。展开更多
基金supported by the National Natural Science Foundation of China(22162012 and 22202089)the Youth Jinggang Scholars Program in Jiangxi Province([2019]57)+6 种基金the Thousand Talents Plan of Jiangxi Province(jxsq2019201083)the Natural Science Foundation of Jiangxi Province for Distinguished Young Scholars(20224ACB213005)the Program of Qingjiang Excellent Young Talents,Jiangxi University of Science and Technology(JXUSTQJBJ2019002)the Research Foundation of Education Bureau of Jiangxi Province of China(GJJ210833)the Foundation of State Key Laboratory of Physical Chemistry of Solid Surfaces(202022)the China Postdoctoral Science Foundation(2021M693893)the Jiangxi Provincial Key Laboratory of Functional Molecular Materials Chemistry(20212BCD42018)。
文摘Direct methanol fuel cells(DMFC) are widely considered to be an ideal green energy conversion device but their widespread applications are limited by the high price of the Pt-based catalysts and the instability in terms of surface CO toxicity in long-term operation.Herein,the PtFe alloy nanoparticles(NPs) with small particle size(~4.12 nm) supported on carbon black catalysts with different Pt/Fe atomic ratios(Pt_(1)Fe_(2)/C,Pt_(3)Fe_(4)/C,Pt_(1)Fe_(1)/C,and Pt_(2)Fe_(1)/C) are successfully prepared for enhanced anti-CO poisoning during methanol oxidation reaction(MOR).The optimal atomic ratio of Pt/Fe for the MOR is 1:2,and the mass activity of Pt_(1)Fe_(2)/C(5.40 A mg_(Pt)^(-1)) is 13.5 times higher than that of conventional commercial Pt/C(Pt/C-JM)(0.40 A mg_(Pt)^(-1)).The introduction of Fe into the Pt lattice forms the PtFe alloy phase,and the electron density of Pt is reduced after forming the PtFe alloy.In-situ Fourier transform infrared results indicate that the addition of oxyphilic metal Fe has reduced the adsorption of reactant molecules on Pt during the MOR.The doping of Fe atoms helps to desorb toxic intermediates and regenerate Pt active sites,promoting the cleavage of C-O bonds with good selectivity of CO_(2)(58.1%).Moreover,the Pt_(1)Fe_(2)/C catalyst exhibits higher CO tolerance,methanol electrooxidation activity,and long-term stability than other Pt_(x)Fe_(y)/C catalysts.
基金the National Natural Science Foundation of China(Grant Nos.T2222027,12202416 and 12272359).
文摘Metal(aluminum and boron)based energetic materials have been wildly applied in various fields including aerospace,explosives and micro-devices due to their high energy density.Unfortunately,the low combustion efficiency and reactivity of metal fuels,especially boron(B),severely limit their practical applications.Herein,multi-component 3D microspheres of HMX/B/Al/PTFE(HBA)have been designed and successfully prepared by emulsion and solvent evaporation method to achieve superior energy and combustion reactivity.The reactivity and energy output of HBA are systematically measured by ignitionburning test,constant-volume explosion vessel system and bomb calorimetry.Due to the increased interfacial contact and reaction area,HBA shows higher flame propagation rate,faster pressurization rate and larger combustion heat of 29.95 cm/s,1077 kPa/s,and 6164.43 J/g,which is 1.5 times,3.5 times,and 1.03 times of the physical mixed counterpart(HBA-P).Meanwhile,HBA also shows enhanced energy output and reactivity than 3D microspheres of HMX/B/PTFE(HB)resulting from the high reactivity of Al.The reaction mechanism of 3D microspheres is comprehensively investigated through combustion emission spectral and thermal analysis(TG-DSC-MS).The superior reactivity and energy of HBA originate from the surface etching of fluorine to the inert shell(Al_(2)O_(3) and B_(2)O_(3))and the initiation effect of Al to B.This work offers a promising approach to design and prepare high-performance energetic materials for the practical applications.
文摘液滴撞击固体表面是自然界的常见现象,研究超疏水表面的液滴撞击对其润湿性的影响,对于超疏水性材料的潜在应用具有重要的科学意义。采用3、10、20 min氧等离子体处理(OPT)和1 min八氟环丁烷等离子体聚合沉积(PPD)的等离子体方法改性聚四氟乙烯(PTFE)表面,获得具有不同尺寸和间距的微/纳米锥的超疏水PTFE表面,研究射频等离子体改性PTFE表面的液滴静态接触角、滚动角及液滴撞击动力学行为,分析在不同个数液滴撞击后PTFE表面的润湿性和液滴撞击行为变化,确定PTFE表面液滴撞击起电效应的影响机制。结果表明:通过1~9个液滴撞击后,PTFE表面的静态接触角随撞击液滴数量增加而减小,导致静态接触角低于150°;液滴滚动角随撞击液滴数量增加而增大,造成液滴滚动角高于10°。撞击液滴的接触时间随撞击液滴数量增加而增大,回弹系数随撞击液滴数量增加而减小。随撞击液滴数量增加,回弹液滴的正电荷和PTFE表面的负电压增大,PTFE表面的负电荷对液滴产生强吸引作用,导致低粘附超疏水性被破坏。3 min OPT和1 min PPD改性PTFE表面的纳米锥间距小,密度大,表面负电荷量增加明显,造成PTFE表面的疏水性降低的程度最显著。研究结果可为改善超疏水稳定性的表面织构设计提供理论依据。
