电纺Fe/N/C纳米纤维催化剂及其氧还原性能
|
摘要
大量研究已表明Fe/N/C是极具前景的氧还原非贵金属催化剂。为发展快速、规模化的制备工艺,以聚酰胺酸、乙酰丙酮铁和三聚氰胺为原料,通过静电纺丝技术制备了一系列氮掺杂碳纳米纤维负载的Fe催化剂(Fe/N/CNF),通过XRD、XPS、SEM、TEM等表征技术测试了催化剂的物相、组分及微观形貌,并通过电化学测试方法研究了Fe含量对其氧还原反应活性的影响。在酸性电解质中,Fe/N/CNFs-3(Fe载量为3%,质量分数)催化剂呈现了良好的氧还原活性,经过5 000圈的循环伏安扫描,其初始电压和半波电位比商业化Pt/C催化剂的仅仅低34和120 m V,呈现了良好的稳定性。
Fe/N/C catalyst is considered as a very promising catalyst for oxygen reduction reaction. To develop a facile mass production method, a series of Fe-and N-doped nano carbon fiber(Fe/N/C) catalysts were synthesized via electrospinning the mixture of poly(amic acid)(PAA) nanofiber-supported iron acetylacetonate [Fe(acac)_3] and melamine. The composition and microstructural properties of prepared catalysts were identified by several characterization techniques including XRD, XPS,BET, SEM and TEM. The influence of the Fe loading on the performance of ORR was also investigated electrochemically in acid media. The onset and half-wave potential for Fe/N/CNFs-3(3% Fe) catalyst are just 34 and 120 m V lower than those of the commercial Pt/C catalyst, respectively. Moreover, the prepared catalyst exhibits comparable durability with the Pt/C catalyst during potential cycle testing.
Fe/N/C catalyst is considered as a very promising catalyst for oxygen reduction reaction. To develop a facile mass production method, a series of Fe-and N-doped nano carbon fiber(Fe/N/C) catalysts were synthesized via electrospinning the mixture of poly(amic acid)(PAA) nanofiber-supported iron acetylacetonate [Fe(acac)_3] and melamine. The composition and microstructural properties of prepared catalysts were identified by several characterization techniques including XRD, XPS,BET, SEM and TEM. The influence of the Fe loading on the performance of ORR was also investigated electrochemically in acid media. The onset and half-wave potential for Fe/N/CNFs-3(3% Fe) catalyst are just 34 and 120 m V lower than those of the commercial Pt/C catalyst, respectively. Moreover, the prepared catalyst exhibits comparable durability with the Pt/C catalyst during potential cycle testing.
引文
[1] STEELE B C H, HEINZEL A. Materials for fuel-cell technologies[J]. Nature, 2001, 414(6861):345-352.
[2] TAHIR M, MAHMOOD N, ZHU J, et al. One dimensional graphitic carbon nitrides as effective metal-free oxygen reduction catalysts[J]. Scientific Reports, 2015, 5:12389.
[3] WANG Y C, LAI Y J, SONG L, et al. S-doping of an Fe/N/C ORR catalyst for polymer electrolyte membrane fuel cells with high power density[J]. Angewandte Chemie International Edition, 2015,127(34):10045-10048.
[4] LIU K, KATTEL S, MAO V, et al. Electrochemical and computational study of oxygen reduction reaction on nonprecious transition metal/nitrogen doped carbon nanofibers in acid medium[J]. Journal of Physical Chemistry C, 2016, 120(3):1586-1596.
[5] JIANG W J, GU L, LI L, et al. Understanding the high activity of Fe-N-C electrocatalysts in oxygen reduction:Fe/Fe3C nanoparticles boost the activity of Fe-Nx[J]. Journal of the American Chemical Society, 2016, 138(10):3570-3578.
[6] MALDONADO S, STEVENSON K J. Influence of nitrogen doping on oxygen reduction electrocatalysis at carbon nanofiber electrodes[J]. The Journal of Physical Chemistry B, 2005, 109(10):4707-4716.
[7] ZHONG R S, QIN Y H, NIU D F, et al. Effect of carbon nanofiber surface functional groups on oxygen reduction in alkaline solution[J]. Journal of Power Sources, 2013, 225:192-199.
[8] CHEN M, LIU J, ZHOU W, et al. Nitrogen-doped graphene-supported transition-metals carbide electrocatalysts for oxygen reduction reaction[J]. Scientific Reports, 2015(5):10389.
[9] LIN L, ZHU Q, XU A W. Noble-metal-free Fe-N/C catalyst for highly efficient oxygen reduction reaction under both alkaline and acidic conditions[J]. Journal of the American Chemical Society,2014, 136(31):11027-11033.
[10] NIU W, LI L, LIU X, et al. Mesoporous N-doped carbons prepared with thermally removable nanoparticle templates:an efficient electrocatalyst for oxygen reduction reaction[J]. Journal of the American Chemical Society, 2015, 137(16):5555-5562.
[2] TAHIR M, MAHMOOD N, ZHU J, et al. One dimensional graphitic carbon nitrides as effective metal-free oxygen reduction catalysts[J]. Scientific Reports, 2015, 5:12389.
[3] WANG Y C, LAI Y J, SONG L, et al. S-doping of an Fe/N/C ORR catalyst for polymer electrolyte membrane fuel cells with high power density[J]. Angewandte Chemie International Edition, 2015,127(34):10045-10048.
[4] LIU K, KATTEL S, MAO V, et al. Electrochemical and computational study of oxygen reduction reaction on nonprecious transition metal/nitrogen doped carbon nanofibers in acid medium[J]. Journal of Physical Chemistry C, 2016, 120(3):1586-1596.
[5] JIANG W J, GU L, LI L, et al. Understanding the high activity of Fe-N-C electrocatalysts in oxygen reduction:Fe/Fe3C nanoparticles boost the activity of Fe-Nx[J]. Journal of the American Chemical Society, 2016, 138(10):3570-3578.
[6] MALDONADO S, STEVENSON K J. Influence of nitrogen doping on oxygen reduction electrocatalysis at carbon nanofiber electrodes[J]. The Journal of Physical Chemistry B, 2005, 109(10):4707-4716.
[7] ZHONG R S, QIN Y H, NIU D F, et al. Effect of carbon nanofiber surface functional groups on oxygen reduction in alkaline solution[J]. Journal of Power Sources, 2013, 225:192-199.
[8] CHEN M, LIU J, ZHOU W, et al. Nitrogen-doped graphene-supported transition-metals carbide electrocatalysts for oxygen reduction reaction[J]. Scientific Reports, 2015(5):10389.
[9] LIN L, ZHU Q, XU A W. Noble-metal-free Fe-N/C catalyst for highly efficient oxygen reduction reaction under both alkaline and acidic conditions[J]. Journal of the American Chemical Society,2014, 136(31):11027-11033.
[10] NIU W, LI L, LIU X, et al. Mesoporous N-doped carbons prepared with thermally removable nanoparticle templates:an efficient electrocatalyst for oxygen reduction reaction[J]. Journal of the American Chemical Society, 2015, 137(16):5555-5562.