物理化学学报 >> 2016, Vol. 32 >> Issue (6): 1473-1481.doi: 10.3866/PKU.WHXB201603112

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新型耐甲醇氧还原电催化剂——氮掺杂中空碳微球@铂纳米粒子复合材料

田春霞,杨军帅,李丽,张小华,陈金华*()   

  • 收稿日期:2016-01-15 发布日期:2016-06-03
  • 通讯作者: 陈金华 E-mail:chenjinhua@hnu.edu.cn
  • 基金资助:
    The project was supported by the Program for Changjiang Scholars and Innovative Research Team in University, China(IRT1238);NationalNatural Science Foundation of China(21275041, J1210040, J1103312);长江学者和创新团队发展计划(IRT1238);国家自然科学基金(21275041, J1210040, J1103312)

New Methanol-Tolerant Oxygen Reduction Electrocatalyst——Nitrogen-Doped Hollow Carbon Microspheres@Platinum Nanoparticles Hybrids

Chun-Xia TIAN,Jun-Shuai YANG,Li LI,Xiao-Hua ZHANG,Jin-Hua CHEN*()   

  • Received:2016-01-15 Published:2016-06-03
  • Contact: Jin-Hua CHEN E-mail:chenjinhua@hnu.edu.cn
  • Supported by:
    The project was supported by the Program for Changjiang Scholars and Innovative Research Team in University, China(IRT1238);NationalNatural Science Foundation of China(21275041, J1210040, J1103312);长江学者和创新团队发展计划(IRT1238);国家自然科学基金(21275041, J1210040, J1103312)

摘要:

通过模板法制备了一种新型耐甲醇氧还原电催化剂——氮掺杂中空碳微球@铂纳米粒子复合材料(HNCMS@PtNPs)。首先,将铂纳米粒子负载于氨基化二氧化硅微球上,获得PtNPs/SiO2复合材料。然后通过多巴胺自聚合反应在PtNPs/SiO2复合材料上包裹聚多巴胺(PDA)膜,将其在氮气气氛中直接进行碳化处理并通过氢氟酸溶液刻蚀去除SiO2,获得了内嵌有PtNPs的氮掺杂中空碳微球,标记为HNCMS@PtNPs复合材料。采用扫描电子显微镜、透射电子显微镜、X射线衍射仪、拉曼光谱仪、比表面积分析仪和X射线光电子能谱仪对HNCMS@PtNPs复合材料的形貌和结构进行了表征。采用循环伏安法和线性扫描伏安法研究了HNCMS@PtNPs复合材料的电催化氧还原性能。结果表明:HNCMS@PtNPs催化剂的Pt载量高达11.9%(w,质量分数),对氧还原反应具有高电催化活性、高稳定性和优良的抗甲醇性能,是一种具有应用潜力的直接甲醇燃料电池(DMFCs)阴极电催化剂。

关键词: Pt纳米粒子, 氮掺杂, 空心碳微球, 氧还原反应, 抗甲醇

Abstract:

A new methanol-tolerant oxygen reduction electrocatalyst,nitrogen-doped hollow carbon microspheres@platinum nanoparticles hybrids (HNCMS@Pt NPs),has been synthesized by a facile template route.In brief,Pt NPs were loaded on the surface of NH2-functionalized SiO2 microspheres (Pt NPs/SiO2).Then, the Pt NPs/SiO2 hybrids were wrapped by polydopamine (PDA) film.After direct carbonization of PDA-wrapped Pt NPs/SiO2 hybrids under a nitrogen atmosphere and further treatment in a hydrofluoric acid solution,Pt NPs embedded within nitrogen-doped hollow carbon microsphere (HNCMS) were obtained and labeled as HNCMS@Pt NPs.Scanning electron microscopy,transmission electron microscopy,X-ray diffraction,Raman spectroscopy,specific surface area analysis,and X-ray photoelectron spectroscopy were used to characterize the HNCMS@Pt NPs hybrids.The electrochemical properties of the HNCMS@Pt NPs hybrids for oxygen reduction reaction have also been investigated by cyclic voltammetry and linear sweep voltammetry.The results show that the Pt loading mass in the HNCMS@Pt NPs hybrids is up to 11.9%(w,mass fraction).Furthermore, the as-prepared HNCMS@Pt NPs catalyst exhibits good electrocatalytic activity,high stability,and excellent methanol-tolerance toward oxygen reduction reactions,implying potential applications in practical direct 1473 methanol fuel cells (DMFCs) as methanol-tolerant cathodic catalysts.

Key words: Pt nanoparticle, Nitrogen-doping, Hollow carbon microsphere, Oxygen-reduction reaction, Methanol-tolerance

MSC2000: 

  • O646