金属—石墨烯纳米复合催化剂的制备及在燃料电池中的应用
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摘要
燃料电池是一种把化学能直接转化为电能的能源转化装置,具有无污染、能量转化率高、使用范围广等优点,是未来人类社会重要的能源方式之一。目前,在燃料电池中,常见的阴阳极催化剂大都是Pt催化剂,但传统的Pt催化剂存在很多不足,影响了其商品化进程,因此,选择和制备高性能的电催化剂是燃料电池中重要研究课题。通常会将Pt基催化剂负载到导电的高比表面积的碳载体上,碳载体的种类、表面性质等在很大程度上影响着Pt基催化剂的分散程度、颗粒大小和尺寸等,从而影响催化剂的催化性能。石墨烯(Graphene)是新近发现的一种具有二维平面结构的碳纳米材料,它的特殊单原子层结构使其具有许多独特的物理化学性质,如较大的比表面积和优良的电子传导能力等,因此有望作为金属催化剂载体应用于生物电催化、燃料电池等领域。本文制备了一系列金属-graphene纳米复合催化剂,将其用于有机小分子(葡萄糖、甲醇)的氧化反应和氧气的还原反应,研究了金属-graphene纳米复合催化剂的电催化性能,具体内容如下：
1.制备了Au-graphene纳米复合催化剂,并将其用于催化氧气的还原反应和葡萄糖的氧化反应。利用电化学沉积法制备了Au-graphene纳米复合催化剂,并利用扫描电子显微镜(SEM),电子能谱(EDS),X-射线粉末衍射(XRD)和电化学方法等对其进行了表征。通过调节电沉积的时间和反应溶液中前驱体AuCl4-的浓度可以得到形貌和尺寸可控的Au纳米粒子。以氧气还原反应和葡萄糖氧化反应为模型,利用循环伏安法对制备的纳米复合催化剂的电催化性能进行了研究,结果表明,与单独的Au纳米粒子和graphene相比,Au-graphene纳米复合催化剂的电催化活性更高,表明在电催化过程中,Au纳米粒子和graphene起到了协同催化作用。该研究为金属-graphene纳米复合催化剂的制备提供了简单易行的方法,且该复合催化剂在燃料电池和生物电催化等相关领域有着广阔的应用前景。
2.制备了一种新型的双金属-graphene纳米复合催化剂,并研究了其电催化特征。利用电沉积方法把Pt-Au纳米结构沉积到了石墨烯的表面,制备了Pt-Au-graphene纳米催化剂,并利用扫描电子显微镜(SEM)、电子能谱(EDS)、X-射线粉末衍射(XRD)和电化学方法等对其进行了表征。通过调节Pt和Au前驱体的原子比可得到形貌和组分可控的Pt-Au-graphene纳米催化剂。利用循环伏安法和线性扫描伏安法研究了Pt-Au-graphene纳米催化剂对氧气还原反应(ORR)和甲醇氧化反应(MOR)的电催化性能,结果表明,Pt-Au-graphene纳米催化剂对ORR和MOR都显示出比Au-graphene和Pt-graphene催化剂更高的催化性能,且当Pt/Au原子比为2：1时,Pt-Au-graphene纳米催化剂的催化活性最高。同时,在催化MOR过程中,graphene表面的含氧官能团可以有效地移除MOR过程中的副产物(如CO等),有效地提高了Pt-Au-graphene纳米催化剂的稳定性。因此,我们制备的Pt-Au-graphene纳米催化剂对ORR和MOR都显示出很高的电催化活性,且可以大大提高Pt的利用率。本章为制备形貌和组分可控的双金属Pt-M催化剂提供了一个简便易行的方法,有望应用于燃料电池领域。
3.研究了Pt-Ni催化剂的结构、组分以及催化剂载体对其催化性能的影响,特别研究了催化剂中Ni的协同催化作用。Pt基催化剂的结构、组分以及催化剂载体的性质对催化剂的催化性能有很大影响,因此通过控制催化剂的结构和组分特征,从而制备新型高效的催化剂,为降低Pt的用量和提高催化剂的催化性能提供了可能性。通过同时还原Ni2+、PtCl62-和氧化石墨烯(GO),利用一步化学还原法制备了Pt-Ni-graphene纳米催化剂,并利用透射电子显微镜(TEM)、紫外光谱(UV-vis).X-射线光电子能谱(XPS)、电子能谱(EDS)、X-射线粉末衍射(XRD)对其进行了表征。以甲醇氧化反应(MOR)为模型,对该催化剂的催化性能进行了研究,系统研究了催化剂的结构、组分以及催化剂载体对催化剂催化性能的影响,实验结果表明,当催化剂中Pt/Ni原子比为1：1时,Pt-Ni-graphene纳米催化剂显示出最高的电催化活性；XPS能谱表明,由于Ni的参与会改变Pt原子的电子结构,同时催化剂中存在的Ni的氧化物会和Pt催化剂起到协同的催化作用,因此Pt-Ni催化剂比纯Pt催化剂显示出更高的催化活性；同时,不同的催化剂载体对其催化活性也有很大影响,利用拉曼光谱和XPS能谱对不同的催化剂载体(graphene、SWNTs、Vulcan XC-72)进行了表征,并比较了这三种物质作为催化剂载体时,Pt/Ni原子比为1：1时Pt-Ni催化剂的催化性能,结果表明,Pt-Ni-graphene催化剂与其他两种催化剂相比表现出更高的电催化活性,这是由于graphene表面丰富的含氧官能团会移除催化过程中产生的一些副产物,从而有效地提高了Pt-Ni催化剂的催化性能。
4.制备了具有独特空心结构的Pt-Ni合金催化剂,并将其负载到graphene表面研究了该催化剂的催化性能。不同形貌的Pt基催化剂会影响其比表面积、表面原子结构,从而会影响催化剂的催化性能。利用连续还原法制备了空心结构的Pt-Ni-graphene复合催化剂,并利用透射电子显微镜(TEM)、电子能谱(EDS)、X-射线粉末衍射(XRD)等表征手段对其进行了表征。为了研究该空心结构Pt-Ni合金的形成机理,同时利用TEM观察了Pt-Ni合金的形成过程,并研究了不同Pt/Ni原子比及不同的表面活性剂对Pt-Ni合金形貌的影响。最后以甲醇氧化反应(MOR)为模型,研究了该Pt-Ni-graphene催化剂的催化性能,并将其与实心Pt-Ni-graphene以及商业化的Pt/C催化剂进行比较,结果表明,空心结构的Pt-Ni-graphene表现出最高的电催化活性,这可能是由于Pt-Ni合金独特的空心结构以及graphene高的电导率和大的比表面积引起的。
Future energy concerns demand a transition from fossil fuels to new energy sources that are more environmentally benign and renewable. A promising route for accomplishing this goal is to use fuel cells to convert the chemical energy of fuel directly into electricity. In this sense, fue cells have received much attention because of several advantages, including high conversion efficiency, low pollution, and high power density, for a wide range of applications. The Pt catalysts are the most popular and effective electrocatalysts for both the anode and the cathode of fuel cell, however, Pt catalysts usually suffer from several disadvantages blocking the commercialization of fuel cells. To enhance the activity of catalysts and lower the use of noble metals, it is highly desirable to load catalysts on the surface of suitable supporting materials. Graphene, a recently discovered carbon nanomaterial with carbon atoms tightly packed into a two dimensional honeycomb lattice, possesses many novel and unique physical and chemical properties because of its unusual monolayer atomic structure. Because of its novel properties such as large specific surface area, high electrical conductivities, graphene has found potential applications in the field of fuel cells. In this paper, we synthesized a series of metal-graphene nanocatalysts, the electrocatalytic characteristics of the nanocatalysts were studied by voltammetry with organic molecular (glucose, methanol) oxidation reaction and the oxygen reduction reaction as model reactions. The main results are as follows:
1. A gold nanoparticles (Au NPs)-graphene nanocomposite (Au-graphene nanocomposite) was prepared by electrochemically depositing Au NPs on the surface of graphene sheets, and characterized by scanning electron microscopy (SEM), energy-dispersive spectroscopy (EDS), X-ray powder diffraction (XRD), and electrochemical methods. The morphology and size of the Au NPs could be easily controlled by adjusting the electrodeposition time and the concentration of precursor (AuCl4-). The electrocatalytic activities of the nanocomposites toward oxygen reduction and glucose oxidation were investigated by cyclic voltammetry. The results indicated that the nanocomposites had a higher catalytic activity than the Au NPs or graphene alone, indicative the synergistic effect of graphene and Au NPs. Therefore, this study has provided a general route for fabrication of graphene-based noble metal nanomaterials composite, which could be potential utility to fuel cells and bioelectroanalytical chemistry.
2. Bimetallic catalysts have proven superior to single metal catalysts in this respect. This chapter reports the preparation, characterization, and electrocatalytic characteristics of a new bimetallic nanocatalyst. The catalyst, Pt-Au-graphene, was synthesized by electrodeposition of Pt-Au nano structures on the surface of graphene sheets, and characterized by scanning electron microscopy (SEM), energy-dispersive spectroscopy (EDS), X-ray powder diffraction (XRD), and voltammetry. The morphology and composition of the nanocatalyst can be easily controlled by adjusting the molar ratio between Pt and Au precursors. The electrocatalytic characteristics of the nanocatalysts for oxygen reduction reaction (ORR) and methanol oxidation reaction (MOR) were systematically investigated by cyclic voltammetry. The Pt-Au-graphene catalysts exhibits higher catalytic activity than Au-graphene and Pt-graphene catalysts for both the ORR and MOR, and the highest activity is obtained at a Pt/Au molar ratio of2:1. Moreover, graphene can significantly enhance the long-term stability of the nanocatalyst toward MOR by effectively removing the accumulated carbonaceous species formed in the oxidation of methanol from the surface of the catalyst. Therefore, this chapter has demonstrated that a higher performance of ORR and MOR could be realized at the Pt-Au-graphene electrocatalyst while Pt utilization also could be greatly diminished. This method may open a general approach for the morphology-controlled synthesis of bimetallic Pt-M nanocatalysts, which can be expected to have promising applications in fuel cells.
3. The structure, composition, and support material significantly affect the catalytic characteristics of Pt-based nanocatalysts. Fine control of the structural and compositional features is highly favorable for the creation of new Pt-based nanocatalysts with enhanced catalytic performance and improved Pt utilization. This chapter reports on a systematic and comparative study of the effects of structure, composition, and carbon support properties on the electrocatalytic activity and stability of Pt-Ni bimetallic catalysts for methanol oxidation, particularly the promoting effect of Ni on Pt. Graphene-supported Pt-Ni alloy nanocatalysts were prepared by a facile, one-step chemical reduction of graphene oxide and the precursors of Ni2+and PtCl62-. The nanocatalysts were characterized by transmission electron microscopy (TEM), ultraviolet-visible spectrophotometry (UV-vis), X-ray photoelectron spectroscopy (XPS), energy-dispersive X-ray spectroscopy (EDS), and X-ray diffraction (XRD). The electrocatalytic characteristics of the nanocatalysts
were studied by voltammetry with methanol oxidation as a model reaction to evaluate
the effects of the structure, surface composition, and electronic characteristics of the
catalyst on the electrochemical activity. The catalyst with a Pt/Ni molar ratio of1:1
exhibited the highest electrocatalytic activity for the methanol oxidation reaction with
greatly lowered Pt utilization. The mechanism of the promoting effect of Ni on Pt is
explained based on the modification of the electronic characteristics of the surface Pt
atoms (Pt4f) by Ni atoms due to the shift in the electron transfer from Ni to Pt and the
synergistic roles of Pt and nickel hydroxides on the surfaces of the catalysts. The
effects of the different carbon supports (i.e., graphene, single-walled carbon
nanotubes, and Vulcan XC-72carbon) on the electrocatalytic characteristics of the
nanocatalysts are investigated by Raman and XPS experiments. The results
demonstrate that the graphene-supported Pt-Ni catalyst has the highest
electrocatalytic activity of the three carbon materials due to abundant
oxygen-containing groups on the graphene surface, which can remove the poisoned
intermediates and improve the electrocatalytic activity of the catalysts.4. Size and shaped-controlled synthesis of nanocatalysts has attracted much
attention because their catalytic performance is highly dependent on the surface areas,
surface atomic structures, and shapes. A novel graphene-supported hollow Pt-Ni
alloy nanostructure was first fabricated by galvanic displacement. The resulted hollow
Pt-Ni-graphene nanostructures were characterized by transmission electron
microscopy (TEM), energy-dispersive X-ray spectroscopy (EDS), and X-ray
diffraction (XRD). In order to investigate the growth mechanism, the formation
process of the Pt-Ni nanostructures were monitored by TEM, and the effects of the
molar ratio of the precursors (the ratio of the K2PtCl6to NiCl2·6H2O) and capping
agent were also investigated by TEM. The electrocatalytic characteristics of the
hollow Pt-Ni-graphene nanocatalysts were studied with methanol oxidation as a
model reaction, and the results indicating that the resulted hollow Pt-Ni-graphene
nanocatalysts exhibit more excellent electrocatalytic performance for methanol than
the solid Pt-Ni-graphene, and commercial Pt/C catalysts, which might be due to the
hollow structures of the nanocatalysts and the high electrical conductivity and large
specific area of the graphene sheets
1.制备了Au-graphene纳米复合催化剂,并将其用于催化氧气的还原反应和葡萄糖的氧化反应。利用电化学沉积法制备了Au-graphene纳米复合催化剂,并利用扫描电子显微镜(SEM),电子能谱(EDS),X-射线粉末衍射(XRD)和电化学方法等对其进行了表征。通过调节电沉积的时间和反应溶液中前驱体AuCl4-的浓度可以得到形貌和尺寸可控的Au纳米粒子。以氧气还原反应和葡萄糖氧化反应为模型,利用循环伏安法对制备的纳米复合催化剂的电催化性能进行了研究,结果表明,与单独的Au纳米粒子和graphene相比,Au-graphene纳米复合催化剂的电催化活性更高,表明在电催化过程中,Au纳米粒子和graphene起到了协同催化作用。该研究为金属-graphene纳米复合催化剂的制备提供了简单易行的方法,且该复合催化剂在燃料电池和生物电催化等相关领域有着广阔的应用前景。
2.制备了一种新型的双金属-graphene纳米复合催化剂,并研究了其电催化特征。利用电沉积方法把Pt-Au纳米结构沉积到了石墨烯的表面,制备了Pt-Au-graphene纳米催化剂,并利用扫描电子显微镜(SEM)、电子能谱(EDS)、X-射线粉末衍射(XRD)和电化学方法等对其进行了表征。通过调节Pt和Au前驱体的原子比可得到形貌和组分可控的Pt-Au-graphene纳米催化剂。利用循环伏安法和线性扫描伏安法研究了Pt-Au-graphene纳米催化剂对氧气还原反应(ORR)和甲醇氧化反应(MOR)的电催化性能,结果表明,Pt-Au-graphene纳米催化剂对ORR和MOR都显示出比Au-graphene和Pt-graphene催化剂更高的催化性能,且当Pt/Au原子比为2：1时,Pt-Au-graphene纳米催化剂的催化活性最高。同时,在催化MOR过程中,graphene表面的含氧官能团可以有效地移除MOR过程中的副产物(如CO等),有效地提高了Pt-Au-graphene纳米催化剂的稳定性。因此,我们制备的Pt-Au-graphene纳米催化剂对ORR和MOR都显示出很高的电催化活性,且可以大大提高Pt的利用率。本章为制备形貌和组分可控的双金属Pt-M催化剂提供了一个简便易行的方法,有望应用于燃料电池领域。
3.研究了Pt-Ni催化剂的结构、组分以及催化剂载体对其催化性能的影响,特别研究了催化剂中Ni的协同催化作用。Pt基催化剂的结构、组分以及催化剂载体的性质对催化剂的催化性能有很大影响,因此通过控制催化剂的结构和组分特征,从而制备新型高效的催化剂,为降低Pt的用量和提高催化剂的催化性能提供了可能性。通过同时还原Ni2+、PtCl62-和氧化石墨烯(GO),利用一步化学还原法制备了Pt-Ni-graphene纳米催化剂,并利用透射电子显微镜(TEM)、紫外光谱(UV-vis).X-射线光电子能谱(XPS)、电子能谱(EDS)、X-射线粉末衍射(XRD)对其进行了表征。以甲醇氧化反应(MOR)为模型,对该催化剂的催化性能进行了研究,系统研究了催化剂的结构、组分以及催化剂载体对催化剂催化性能的影响,实验结果表明,当催化剂中Pt/Ni原子比为1：1时,Pt-Ni-graphene纳米催化剂显示出最高的电催化活性；XPS能谱表明,由于Ni的参与会改变Pt原子的电子结构,同时催化剂中存在的Ni的氧化物会和Pt催化剂起到协同的催化作用,因此Pt-Ni催化剂比纯Pt催化剂显示出更高的催化活性；同时,不同的催化剂载体对其催化活性也有很大影响,利用拉曼光谱和XPS能谱对不同的催化剂载体(graphene、SWNTs、Vulcan XC-72)进行了表征,并比较了这三种物质作为催化剂载体时,Pt/Ni原子比为1：1时Pt-Ni催化剂的催化性能,结果表明,Pt-Ni-graphene催化剂与其他两种催化剂相比表现出更高的电催化活性,这是由于graphene表面丰富的含氧官能团会移除催化过程中产生的一些副产物,从而有效地提高了Pt-Ni催化剂的催化性能。
4.制备了具有独特空心结构的Pt-Ni合金催化剂,并将其负载到graphene表面研究了该催化剂的催化性能。不同形貌的Pt基催化剂会影响其比表面积、表面原子结构,从而会影响催化剂的催化性能。利用连续还原法制备了空心结构的Pt-Ni-graphene复合催化剂,并利用透射电子显微镜(TEM)、电子能谱(EDS)、X-射线粉末衍射(XRD)等表征手段对其进行了表征。为了研究该空心结构Pt-Ni合金的形成机理,同时利用TEM观察了Pt-Ni合金的形成过程,并研究了不同Pt/Ni原子比及不同的表面活性剂对Pt-Ni合金形貌的影响。最后以甲醇氧化反应(MOR)为模型,研究了该Pt-Ni-graphene催化剂的催化性能,并将其与实心Pt-Ni-graphene以及商业化的Pt/C催化剂进行比较,结果表明,空心结构的Pt-Ni-graphene表现出最高的电催化活性,这可能是由于Pt-Ni合金独特的空心结构以及graphene高的电导率和大的比表面积引起的。
Future energy concerns demand a transition from fossil fuels to new energy sources that are more environmentally benign and renewable. A promising route for accomplishing this goal is to use fuel cells to convert the chemical energy of fuel directly into electricity. In this sense, fue cells have received much attention because of several advantages, including high conversion efficiency, low pollution, and high power density, for a wide range of applications. The Pt catalysts are the most popular and effective electrocatalysts for both the anode and the cathode of fuel cell, however, Pt catalysts usually suffer from several disadvantages blocking the commercialization of fuel cells. To enhance the activity of catalysts and lower the use of noble metals, it is highly desirable to load catalysts on the surface of suitable supporting materials. Graphene, a recently discovered carbon nanomaterial with carbon atoms tightly packed into a two dimensional honeycomb lattice, possesses many novel and unique physical and chemical properties because of its unusual monolayer atomic structure. Because of its novel properties such as large specific surface area, high electrical conductivities, graphene has found potential applications in the field of fuel cells. In this paper, we synthesized a series of metal-graphene nanocatalysts, the electrocatalytic characteristics of the nanocatalysts were studied by voltammetry with organic molecular (glucose, methanol) oxidation reaction and the oxygen reduction reaction as model reactions. The main results are as follows:
1. A gold nanoparticles (Au NPs)-graphene nanocomposite (Au-graphene nanocomposite) was prepared by electrochemically depositing Au NPs on the surface of graphene sheets, and characterized by scanning electron microscopy (SEM), energy-dispersive spectroscopy (EDS), X-ray powder diffraction (XRD), and electrochemical methods. The morphology and size of the Au NPs could be easily controlled by adjusting the electrodeposition time and the concentration of precursor (AuCl4-). The electrocatalytic activities of the nanocomposites toward oxygen reduction and glucose oxidation were investigated by cyclic voltammetry. The results indicated that the nanocomposites had a higher catalytic activity than the Au NPs or graphene alone, indicative the synergistic effect of graphene and Au NPs. Therefore, this study has provided a general route for fabrication of graphene-based noble metal nanomaterials composite, which could be potential utility to fuel cells and bioelectroanalytical chemistry.
2. Bimetallic catalysts have proven superior to single metal catalysts in this respect. This chapter reports the preparation, characterization, and electrocatalytic characteristics of a new bimetallic nanocatalyst. The catalyst, Pt-Au-graphene, was synthesized by electrodeposition of Pt-Au nano structures on the surface of graphene sheets, and characterized by scanning electron microscopy (SEM), energy-dispersive spectroscopy (EDS), X-ray powder diffraction (XRD), and voltammetry. The morphology and composition of the nanocatalyst can be easily controlled by adjusting the molar ratio between Pt and Au precursors. The electrocatalytic characteristics of the nanocatalysts for oxygen reduction reaction (ORR) and methanol oxidation reaction (MOR) were systematically investigated by cyclic voltammetry. The Pt-Au-graphene catalysts exhibits higher catalytic activity than Au-graphene and Pt-graphene catalysts for both the ORR and MOR, and the highest activity is obtained at a Pt/Au molar ratio of2:1. Moreover, graphene can significantly enhance the long-term stability of the nanocatalyst toward MOR by effectively removing the accumulated carbonaceous species formed in the oxidation of methanol from the surface of the catalyst. Therefore, this chapter has demonstrated that a higher performance of ORR and MOR could be realized at the Pt-Au-graphene electrocatalyst while Pt utilization also could be greatly diminished. This method may open a general approach for the morphology-controlled synthesis of bimetallic Pt-M nanocatalysts, which can be expected to have promising applications in fuel cells.
3. The structure, composition, and support material significantly affect the catalytic characteristics of Pt-based nanocatalysts. Fine control of the structural and compositional features is highly favorable for the creation of new Pt-based nanocatalysts with enhanced catalytic performance and improved Pt utilization. This chapter reports on a systematic and comparative study of the effects of structure, composition, and carbon support properties on the electrocatalytic activity and stability of Pt-Ni bimetallic catalysts for methanol oxidation, particularly the promoting effect of Ni on Pt. Graphene-supported Pt-Ni alloy nanocatalysts were prepared by a facile, one-step chemical reduction of graphene oxide and the precursors of Ni2+and PtCl62-. The nanocatalysts were characterized by transmission electron microscopy (TEM), ultraviolet-visible spectrophotometry (UV-vis), X-ray photoelectron spectroscopy (XPS), energy-dispersive X-ray spectroscopy (EDS), and X-ray diffraction (XRD). The electrocatalytic characteristics of the nanocatalysts
were studied by voltammetry with methanol oxidation as a model reaction to evaluate
the effects of the structure, surface composition, and electronic characteristics of the
catalyst on the electrochemical activity. The catalyst with a Pt/Ni molar ratio of1:1
exhibited the highest electrocatalytic activity for the methanol oxidation reaction with
greatly lowered Pt utilization. The mechanism of the promoting effect of Ni on Pt is
explained based on the modification of the electronic characteristics of the surface Pt
atoms (Pt4f) by Ni atoms due to the shift in the electron transfer from Ni to Pt and the
synergistic roles of Pt and nickel hydroxides on the surfaces of the catalysts. The
effects of the different carbon supports (i.e., graphene, single-walled carbon
nanotubes, and Vulcan XC-72carbon) on the electrocatalytic characteristics of the
nanocatalysts are investigated by Raman and XPS experiments. The results
demonstrate that the graphene-supported Pt-Ni catalyst has the highest
electrocatalytic activity of the three carbon materials due to abundant
oxygen-containing groups on the graphene surface, which can remove the poisoned
intermediates and improve the electrocatalytic activity of the catalysts.4. Size and shaped-controlled synthesis of nanocatalysts has attracted much
attention because their catalytic performance is highly dependent on the surface areas,
surface atomic structures, and shapes. A novel graphene-supported hollow Pt-Ni
alloy nanostructure was first fabricated by galvanic displacement. The resulted hollow
Pt-Ni-graphene nanostructures were characterized by transmission electron
microscopy (TEM), energy-dispersive X-ray spectroscopy (EDS), and X-ray
diffraction (XRD). In order to investigate the growth mechanism, the formation
process of the Pt-Ni nanostructures were monitored by TEM, and the effects of the
molar ratio of the precursors (the ratio of the K2PtCl6to NiCl2·6H2O) and capping
agent were also investigated by TEM. The electrocatalytic characteristics of the
hollow Pt-Ni-graphene nanocatalysts were studied with methanol oxidation as a
model reaction, and the results indicating that the resulted hollow Pt-Ni-graphene
nanocatalysts exhibit more excellent electrocatalytic performance for methanol than
the solid Pt-Ni-graphene, and commercial Pt/C catalysts, which might be due to the
hollow structures of the nanocatalysts and the high electrical conductivity and large
specific area of the graphene sheets
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