This study demonstrated that as-synthesized nano Fe/Cu bimetals could achieve significant enhancement in the degradation of diclofenac(DCF),as compared to much slow removal of DCF by Cu(Ⅱ) or zero valent iron nanopar...This study demonstrated that as-synthesized nano Fe/Cu bimetals could achieve significant enhancement in the degradation of diclofenac(DCF),as compared to much slow removal of DCF by Cu(Ⅱ) or zero valent iron nanoparticles(nZVI),respectively.Further observations on the evolution of O_(2) activation process by nano Fe/Cu bimetals was conducted stretching to the preparation phase(started by nZVI/Cu2+).Interesting breakpoints we re observed with obvious sudden increase in the DCF degradation efficiency and decrease in solution pH,as the original nZVI just consumed up to Fe(Ⅱ) and Cu(II) appeared again.It suggested that the four-electrons reaction of O_(2) and Cu-deposited nZVI would occur to generate water prior to the breakpoints,while Cu(0) and Fe(Ⅱ) would play most important role in activation of O_(2) afterwards.Through the electron spin resonance(ESR) analysis and quenching experiments.·OH was identified as the responsible reactive species.Further time-dependent quantifications in the cases of Cu(0)/Fe(Ⅱ) systems we re carried out.It was found that the ’OH accumulation was positively and linearly correlated with nCu dose,Fe(Ⅱ) consumption,and Fe(II) dose,respectively.Since either Cu(O) or Fe(Ⅱ)would be inefficient in activating oxygen to produce ·OH,a stage-evolution mechanism of O_(2) activated by nano Fe/Cu bimetals was proposed involving:(a) Rapid consumption of Fe(0) and release of Fe(Ⅱ) based on the Cu-Fe galvanic corrosion,(b) adsorption and transformation of O_(2) to O_(2)2 at the nCu surface,and(c) Fe(Ⅱ)-catalyzed activation of the adsorbed O_(2)2 to ·OH.展开更多
Two nanostructured A1-Cu-Fe alloys, A164Cu24Fe12 and A162.5Cu25.2Fe12.3, have been studied. Icosahedral quasicrystalline （ψ） A164CH24FeI2 and crystalline cubic （ β） AI62.sCu25.2Fe12.3 cylindrical ingots were fir...Two nanostructured A1-Cu-Fe alloys, A164Cu24Fe12 and A162.5Cu25.2Fe12.3, have been studied. Icosahedral quasicrystalline （ψ） A164CH24FeI2 and crystalline cubic （ β） AI62.sCu25.2Fe12.3 cylindrical ingots were first produced using normal casting techniques. High-energy mechanical milling was then conducted to obtain β icosahedral and β intermetallic nanostructured powders. Electrochemical impedance spectroscopy, linear polarization resistance, and potentiodynamic polarization were used to investigate the electrochemical corrosion characteristics of the powders in solutions with different pH values. Current density （icorr）, polarization resistance （Rp）, and impedance modulus （121） were determined. The results showed that regardless of pH value, increasing the solution temperature enhanced the corrosion resistance of the both phases. However, the electrochemical behavior of the phase indicated that its stability depends on the submerged exposure time in neutral and alkaline environments. This behavior was related to the type of corrosion products present on the surfaces of the particles along with the diffusion and charge-transfer mechanisms of the corrosion process.展开更多
基金the National Natural Science Foundation of China(Nos.21677055 and 21407052)National Key Research and Development Program of China(No.2019YFC1805204)+1 种基金Project of Three Gorges Corporation(No.JDZC-FW-20-001)the Fundamental Research Funds for the Central Universities,HUST(No.2017KFXKJC004)。
文摘This study demonstrated that as-synthesized nano Fe/Cu bimetals could achieve significant enhancement in the degradation of diclofenac(DCF),as compared to much slow removal of DCF by Cu(Ⅱ) or zero valent iron nanoparticles(nZVI),respectively.Further observations on the evolution of O_(2) activation process by nano Fe/Cu bimetals was conducted stretching to the preparation phase(started by nZVI/Cu2+).Interesting breakpoints we re observed with obvious sudden increase in the DCF degradation efficiency and decrease in solution pH,as the original nZVI just consumed up to Fe(Ⅱ) and Cu(II) appeared again.It suggested that the four-electrons reaction of O_(2) and Cu-deposited nZVI would occur to generate water prior to the breakpoints,while Cu(0) and Fe(Ⅱ) would play most important role in activation of O_(2) afterwards.Through the electron spin resonance(ESR) analysis and quenching experiments.·OH was identified as the responsible reactive species.Further time-dependent quantifications in the cases of Cu(0)/Fe(Ⅱ) systems we re carried out.It was found that the ’OH accumulation was positively and linearly correlated with nCu dose,Fe(Ⅱ) consumption,and Fe(II) dose,respectively.Since either Cu(O) or Fe(Ⅱ)would be inefficient in activating oxygen to produce ·OH,a stage-evolution mechanism of O_(2) activated by nano Fe/Cu bimetals was proposed involving:(a) Rapid consumption of Fe(0) and release of Fe(Ⅱ) based on the Cu-Fe galvanic corrosion,(b) adsorption and transformation of O_(2) to O_(2)2 at the nCu surface,and(c) Fe(Ⅱ)-catalyzed activation of the adsorbed O_(2)2 to ·OH.
基金CONACYT support-Call 2010 Postdoctoral and sabbatical linked to strengthening the quality of national graduate mode A
文摘Two nanostructured A1-Cu-Fe alloys, A164Cu24Fe12 and A162.5Cu25.2Fe12.3, have been studied. Icosahedral quasicrystalline （ψ） A164CH24FeI2 and crystalline cubic （ β） AI62.sCu25.2Fe12.3 cylindrical ingots were first produced using normal casting techniques. High-energy mechanical milling was then conducted to obtain β icosahedral and β intermetallic nanostructured powders. Electrochemical impedance spectroscopy, linear polarization resistance, and potentiodynamic polarization were used to investigate the electrochemical corrosion characteristics of the powders in solutions with different pH values. Current density （icorr）, polarization resistance （Rp）, and impedance modulus （121） were determined. The results showed that regardless of pH value, increasing the solution temperature enhanced the corrosion resistance of the both phases. However, the electrochemical behavior of the phase indicated that its stability depends on the submerged exposure time in neutral and alkaline environments. This behavior was related to the type of corrosion products present on the surfaces of the particles along with the diffusion and charge-transfer mechanisms of the corrosion process.
