负载贵金属催化剂的新型碳基复合材料制备及性能研究
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摘要
具有贵金属@贱金属核壳结构的催化剂因其核和壳性能的互补性,可大幅度提高贵金属的催化活性,从而降低催化剂的成本,普遍应用于电化学催化、有机催化等领域,尤其是对燃料电池普及推广方面具有重要的应用价值,有望成为其大规模产业化的希望之所在。然而,小纳米尺度的核壳催化剂因为粒径小,其表面原子比例高,表面能大,有很高的配位不饱和度,在合成反应和催化剂的循环使用过程中有明显的团聚现象,这使得催化剂的活性面积和催化的选择性大幅度下降。将纳米催化剂粒子负载到载体上有助于这一问题的解决,载体的结构和性质也是影响催化剂活性和用量的关键因素之一。因此开发新型的催化剂载体也是提高贵金属催化活性、促进贵金属催化剂走向实用化的有效途径之一。本论文以新型的碳材料多壁碳纳米管(MWCNTs)和石墨烯为载体,负载贵金属纳米粒子及贵金属@贱金属核壳结构的纳米粒子制备纳米复合物,重点研究了催化剂粒径、载体表面功能化以及核壳结构的相互作用等因素对提高贵金属催化性能的影响,主要结果如下：
1.采用两步法即浸渍法还原法和置换法成功制备了Ni@Pd核壳结构均匀分散在多壁碳纳米管(MWCNTs)上,采用XRD、TEM、HRTEM、EDS等方法对该复合催化材料进行表征分析。从TEM图可见平均粒径为3.4nmNi@Pd核壳结构均匀分散在多壁碳纳米管的表面上,无团聚现象。XRD结果表明,Ni@Pd/MWCNTs中Pd(111)特征衍射峰与Pd/MWCNTs中Pd(111)特征衍射峰相比出现了明显的正位移,表明Ni原子进入了Pd原子的晶格使得Pd的晶格间距变窄。HRTEM可以清楚可见核Ni(111)条纹间距0.203nm和Pd(111)壳条纹间距0.224nm的形成。该核壳结构纳米复合物被用于燃料电池中乙醇的电催化氧化,电化学实验结果表明,对于乙醇的阳极氧化反应,该核壳催化剂的相同负载量Pd的催化活性分别为Pd/MWCNTs催化剂的2.3倍。尤为重要的是Ni和Pd的相互作用使得该催化剂对乙醇氧化中间体具有很好的去除能力。另外,核壳结构降低了贵金属Pd的用量,增大了贵金属有效催化活性面积。
2.采用微波法将Ni还原负载到碳纳米管上,再用置换法将Pd均匀分散在Ni/多壁碳纳米管(Ni/MWCNTs上),采用XRD、TEM、HRTEM、EDS等方法对该复合催化材料进行表征分析,TEM结果表明平均粒径为4nmNi@Pd均匀分散在碳纳米管上,把合成的Ni@Pd/MWCNTs复合物应用于苯甲醇的选择性氧化,在水溶液中,以双氧水作为氧化剂在80℃条件下用Ni@Pd/MWCNTs (Pd:0.2mmol)为催化剂苯甲醛的选择性达到98%,苯甲醇的转化率高达99%,并且该催化剂因为具有磁性容易被回收循环使用。
3.采用微波法和置换法两步法成功合成了核壳Ni@Pd纳米粒子负载到石墨烯载体上形成Ni@Pd/graphene.采用XRD、TEM、HRTEM、EDS、Raman、 FTIR等方法对该复合催化材料进行表征分析。乙二醇微波还原法将将镍离子在180℃微波条件下还原成镍纳米粒子并且均匀分布在碳纳米管的表面,然后用置换法得到平均粒径为4.0的Ni@Pd纳米粒子。循环伏安研究结果表明,该催化剂的相同负载量Pd的催化活性分别为Pd/graphene催化剂的3倍,说明Ni的加入使金属Pd的表面特征发生了改变,Pd壳增大了有效活性表面积从而使得Ni@Pd/graphene相对Pd/graphenes具有更高的氧还原电催化活性和抗CO中毒性。
4.用改进的Hummers法合成氧化石墨烯,表面有大量的含氧基团,这些含氧基团使得石墨烯片层之间分开,金属前驱体很容易分散在石墨烯的表面,然而,氧化石墨烯和金属前驱体在被还原形成金属/石墨烯纳米复合物的过程中,石墨烯表面大量的含氧基团也被还原,结果导致石墨片层之间发生不可逆转的团聚,石墨烯表面和金属的作用力减弱,很难直接将贵金属纳米粒子可控的分散负载到其表面,为了解决这一问题,本文采用用聚二甲基二丙烯基氯化铵(PDDA)和二甲基二丙烯基氯化铵(DMDAAC)等功能化试剂对石墨烯的表面进行了修饰,为了高密度,高分散的负载小粒径的贵金属纳米粒子提供有效的方法。
5.采用乙二醇微波还原法制备了高金属含量(85wt%) Pd/DMDAAC-graphene催化剂。采用XRD、TEM、HRTEM、EDS、Raman、FTIR、UV-vis等方法对该复合催化材料进行表征分析,发现DMDAAC功能化的石墨烯可促进平均粒径为1.8nmPd纳米粒子较均匀地分散,从而大幅度提高催化剂的有效比表面积。循环伏安法结果表明,相同量分散到DMDAAC-graphene修饰电极上的Pd纳米颗粒比分散到未修饰石墨烯修饰电极上的Pd纳米颗粒对乙醇的电催化氧化有更高的催化活性和抗毒性,因此可以推断DMDAAC功能化试剂修饰石墨烯不仅能高密度的分散贵金属纳米粒子,还有助于反应中间产物的转化。
6.同样采用乙二醇微波还原法,通过反应条件的控制,制备了粒径范围小的Pt/PDDA-graphene催化剂,粒径分布图表明平均粒径为1.4nmPt高密度的分散在功能化的表面上,没有团聚现象。循环伏安法和计时电流结果表明,在电催化氧化甲醇时Pt/PDDA-G催化剂与相同Pt量的Pt/graphene催化剂和商业Pt/C催化剂具有更高的活性、稳定性和抗中间产物的毒化能力。这是因为PDDA修饰的石墨烯表面更有利于反应过程中中间产物的转化,使得Pt有更好的抗CO等的毒化性能。
Core-shell structure with low noble metal catalysts is a new type of catalysts in recent years.They enhance the catalytic activity of noble metal and reduce the cost of the catalyst due to the interactions between core and shell. They are widely used in electro catalysis, heterogeneous catalysis and biosensing, especially in potential applications of fuel cells. So they are considered to be the very promising catalysts for large-scale commercialization. But the core shell nano scale catalysts are very easy agglomeration in catalytic synthesis reaction and cyclic use due to the small particle size and higher coordination unsaturation surface atoms, which greatly reduces the activity area and selectivity. To solve this problem, the carrier is often used to as the particle supporter. So the structure and properties of the carrier is the key factor also affecting the activity of catalytic synthesis reaction. Therefore the development of a new catalyst support is one of the effective ways to improve the catalytic performance of noble metal catalysts.
In this thesis, a series of new nanocomposites were synthesized using multi walled carbon nanotubes (MWCNTs) and graphene as carriers to support noble metal and core shell structure. The performance of noble metal catalyst was improved through the functional carrier and the synergistic effect of the core and shell.The results are as follows.
1. Ni@Pd nanoparticles with core/shell structure uniformly dispersed on multi-walled carbon nanotubes (Ni@Pd/MWCNTs) is successfully prepared via a two-step strategy:impregnation-reduction methodand replacement method. The Ni@Pd/MWCNTs composite was characterized by transmission electronmicroscopy (TEM), energy-dispersive X-ray spectroscopy (EDS) and X-ray diffraction (XRD) analysis.It shows a uniform dispersion of Ni@Pd nanoparticles with core/shell structure on MWCNTs with the average particle size of3.4nm. XRD show that positive shift of the Pd peaks occurs obviously on the Ni@Pd/MWCNTs comparing with the Pd/MWCNTs, indicating the Ni atoms enter into the Pd crystals which caused the narrow transformation of the Pd crystal lattice distance. The single crystalline Ni@Pd particles are confirmed, the lattice planes with a interlayer distance of0.203nm in the core are indexed to Ni (111) crystal planes, the outer layer with the lattice space of0.224nm corresponds to Pd (111) crystal planes. The Ni@Pd/MWCNTs composite was used as electrocatalyst for alcohol oxidation in alkaline media for fuel cells. The electrocatalytic activity of ethanol oxidation on Ni@Pd/MWCNTs is2.3times higher than that of Pd/MWCNTs electrocatalyst at the same Pd loadings. The enhanced electrocatalytic properties could be attributed to not only the electric synergistic effect between Pd and Ni, but also the high use ratio of Pd for its shell structure.
2. Well dispersed Ni@Pd bimetallic nanoparticles on multi-walled carbon nanotubes (Ni@Pd/MWCNTs) are prepared and used as catalysts for the oxidation of benzyl alcohol. Scanning electron microscopy, transmission electron microscopy, energy-dispersive X-ray spectroscopy analysis, and X-ray diffraction were performed to characterise the synthesized catalyst. The results show a uniform dispersion of Ni@Pd nanoparticles on MWCNTs with an average particle size of4.0nm. The as synthesised catalyst was applied to the oxidation of benzyl alcohol. A99%conversion of benzyl alcohol and a98%selectivity of benzaldehyde were achieved by using the Ni@Pd/MWCNTs (Pd:0.2mmol) catalyst with water as a solvent and H2O2as oxidant at80℃. The catalytic activity of Ni@Pd/MWCNTs towards benzyl alcohol is higher than that of a Pd/MWCNTs catalyst at the same Pd loadings. The catalyst can be easily separated due to its magnetic properties.
3. The uniform dispersion of new highly active Ni@Pd core-shell nanoparticle catalysts supported on graphene (Ni@Pd/graphene) was prepared via a two-step procedure involving a microwave synthesis method and a replacement method. Several characterization tools, such as X-ray powder diffraction (XRD), transmission electron microscopy (TEM), energy-dispersive X-ray spectroscopy (EDS) and Fourier transform infrared spectroscopy (FTIR) were employed to study the phase structures, morphologies and properties of the Ni@Pd/graphene composite. The results indicated that a uniform dispersion of Ni@Pd core-shell structure nanoparticles on graphene have an average particle size of4nm. The Ni@Pd/graphene composite was used as an electrocatalyst for alcohol oxidation in alkaline media for fuel cells. The electrocatalytic activity of Ni@Pd/graphene for ethanol oxidation is3times higher than that of the Pd/grapheme electrocatalyst at the same Pd loading. The enhanced electrocatalytic properties could be attributed not only to the electric synergistic effect between Pd, Ni and graphene, but also the high use ratio of Pd due to its shell structure.
4. The over oxidation of graphene nanosheets were produced by the modify Hummers method with strong oxidants. Abundant oxygen-containing functional groups were present in grapheme oxide, which enable the solubilization of oxidized graphene sheets and thus allow for the intercalation of molecules such as metal precursors into the interlayer space of GO(grapheme oxide). Unfortunately, when the metal ions and GO are mixed and co-reduced to form metal-graphene composite, the subsequent chemical reduction of GO (with metal ions) is required, which makes the abundant oxygen-containing functional groups lost and tends to form irreversible agglomerates or even restack to form graphite. The weak interaction between metal and graphite surfers results in a severe agglomeration of catalytic metal nanoparticles and leads to the loss of its advantage of an ultra-high surface area. To solve this problem, some other intermediates such as poly diallyldimethylammonium chloride (PDDA) and Dimethyldiallylammonium chloride (DMDAAC) have to be introduced.
5. Dimethyldiallylammonium chloride modified reduced graphene oxide supported Pd nanoparticles (Pd/DMDAAC-RGO) were fabricated by polyol microwave heating method. The Pd/DMDAAC-RGOhybrid was characterized by transmission electromicroscopy (TEM), energy-dispersive X-ray spec-troscopy (EDS), X-ray diffraction (XRD) analysis and electrochemical tests. High Pd metal loadings, up to80wt.%with a mean size of1.8nm, were densely in situ decorated on DMDAAC-modified RGO surfaces.Compared with traditional carbon-based Pd catalysts, Pd/DMDAAC-RGO exhibits better activity and stability for ethanol oxidation in alkaline media with the same Pd content on the electrode. This improvedactivity indicates that DMDAAC plays a crucial role in the dispersion and stabilization of Pd nanoparti-cles on RGO sheets and DMDAAC-RGO are able to an alternative support for Pd immobilization in directethanol fuel cells and other catalytic devices.
6. A simple one-pot micro wave-poly ol reduced method was used to anchor platinum nanoparticles on graphene with the aid of PDDA, forming a Pt/PDDA-G hybrid (Pt/PDDA-G). High Pt metal loadings, up to85wt.%with a mean size of1.4nm, were densely in situ decorated on PDDA-modified grapheme surfaces. The electrochemical tests showed that the activity and stability of Pt supported on PDDA-graphene hybrid substrates for methanol oxidation were better than that of Pt supported on graphene sheets, also better than the widely used Pt/carbon black electrocatalysts with the same Pt content on the electrode. This improved activity indicates that PDDA plays a crucial role in the highly dispersion and stabilization of Pt nanoparticles on graphene and PDDA-G are able to an alternative support for Pt immobilization in direct methanol fuel cells.
1.采用两步法即浸渍法还原法和置换法成功制备了Ni@Pd核壳结构均匀分散在多壁碳纳米管(MWCNTs)上,采用XRD、TEM、HRTEM、EDS等方法对该复合催化材料进行表征分析。从TEM图可见平均粒径为3.4nmNi@Pd核壳结构均匀分散在多壁碳纳米管的表面上,无团聚现象。XRD结果表明,Ni@Pd/MWCNTs中Pd(111)特征衍射峰与Pd/MWCNTs中Pd(111)特征衍射峰相比出现了明显的正位移,表明Ni原子进入了Pd原子的晶格使得Pd的晶格间距变窄。HRTEM可以清楚可见核Ni(111)条纹间距0.203nm和Pd(111)壳条纹间距0.224nm的形成。该核壳结构纳米复合物被用于燃料电池中乙醇的电催化氧化,电化学实验结果表明,对于乙醇的阳极氧化反应,该核壳催化剂的相同负载量Pd的催化活性分别为Pd/MWCNTs催化剂的2.3倍。尤为重要的是Ni和Pd的相互作用使得该催化剂对乙醇氧化中间体具有很好的去除能力。另外,核壳结构降低了贵金属Pd的用量,增大了贵金属有效催化活性面积。
2.采用微波法将Ni还原负载到碳纳米管上,再用置换法将Pd均匀分散在Ni/多壁碳纳米管(Ni/MWCNTs上),采用XRD、TEM、HRTEM、EDS等方法对该复合催化材料进行表征分析,TEM结果表明平均粒径为4nmNi@Pd均匀分散在碳纳米管上,把合成的Ni@Pd/MWCNTs复合物应用于苯甲醇的选择性氧化,在水溶液中,以双氧水作为氧化剂在80℃条件下用Ni@Pd/MWCNTs (Pd:0.2mmol)为催化剂苯甲醛的选择性达到98%,苯甲醇的转化率高达99%,并且该催化剂因为具有磁性容易被回收循环使用。
3.采用微波法和置换法两步法成功合成了核壳Ni@Pd纳米粒子负载到石墨烯载体上形成Ni@Pd/graphene.采用XRD、TEM、HRTEM、EDS、Raman、 FTIR等方法对该复合催化材料进行表征分析。乙二醇微波还原法将将镍离子在180℃微波条件下还原成镍纳米粒子并且均匀分布在碳纳米管的表面,然后用置换法得到平均粒径为4.0的Ni@Pd纳米粒子。循环伏安研究结果表明,该催化剂的相同负载量Pd的催化活性分别为Pd/graphene催化剂的3倍,说明Ni的加入使金属Pd的表面特征发生了改变,Pd壳增大了有效活性表面积从而使得Ni@Pd/graphene相对Pd/graphenes具有更高的氧还原电催化活性和抗CO中毒性。
4.用改进的Hummers法合成氧化石墨烯,表面有大量的含氧基团,这些含氧基团使得石墨烯片层之间分开,金属前驱体很容易分散在石墨烯的表面,然而,氧化石墨烯和金属前驱体在被还原形成金属/石墨烯纳米复合物的过程中,石墨烯表面大量的含氧基团也被还原,结果导致石墨片层之间发生不可逆转的团聚,石墨烯表面和金属的作用力减弱,很难直接将贵金属纳米粒子可控的分散负载到其表面,为了解决这一问题,本文采用用聚二甲基二丙烯基氯化铵(PDDA)和二甲基二丙烯基氯化铵(DMDAAC)等功能化试剂对石墨烯的表面进行了修饰,为了高密度,高分散的负载小粒径的贵金属纳米粒子提供有效的方法。
5.采用乙二醇微波还原法制备了高金属含量(85wt%) Pd/DMDAAC-graphene催化剂。采用XRD、TEM、HRTEM、EDS、Raman、FTIR、UV-vis等方法对该复合催化材料进行表征分析,发现DMDAAC功能化的石墨烯可促进平均粒径为1.8nmPd纳米粒子较均匀地分散,从而大幅度提高催化剂的有效比表面积。循环伏安法结果表明,相同量分散到DMDAAC-graphene修饰电极上的Pd纳米颗粒比分散到未修饰石墨烯修饰电极上的Pd纳米颗粒对乙醇的电催化氧化有更高的催化活性和抗毒性,因此可以推断DMDAAC功能化试剂修饰石墨烯不仅能高密度的分散贵金属纳米粒子,还有助于反应中间产物的转化。
6.同样采用乙二醇微波还原法,通过反应条件的控制,制备了粒径范围小的Pt/PDDA-graphene催化剂,粒径分布图表明平均粒径为1.4nmPt高密度的分散在功能化的表面上,没有团聚现象。循环伏安法和计时电流结果表明,在电催化氧化甲醇时Pt/PDDA-G催化剂与相同Pt量的Pt/graphene催化剂和商业Pt/C催化剂具有更高的活性、稳定性和抗中间产物的毒化能力。这是因为PDDA修饰的石墨烯表面更有利于反应过程中中间产物的转化,使得Pt有更好的抗CO等的毒化性能。
Core-shell structure with low noble metal catalysts is a new type of catalysts in recent years.They enhance the catalytic activity of noble metal and reduce the cost of the catalyst due to the interactions between core and shell. They are widely used in electro catalysis, heterogeneous catalysis and biosensing, especially in potential applications of fuel cells. So they are considered to be the very promising catalysts for large-scale commercialization. But the core shell nano scale catalysts are very easy agglomeration in catalytic synthesis reaction and cyclic use due to the small particle size and higher coordination unsaturation surface atoms, which greatly reduces the activity area and selectivity. To solve this problem, the carrier is often used to as the particle supporter. So the structure and properties of the carrier is the key factor also affecting the activity of catalytic synthesis reaction. Therefore the development of a new catalyst support is one of the effective ways to improve the catalytic performance of noble metal catalysts.
In this thesis, a series of new nanocomposites were synthesized using multi walled carbon nanotubes (MWCNTs) and graphene as carriers to support noble metal and core shell structure. The performance of noble metal catalyst was improved through the functional carrier and the synergistic effect of the core and shell.The results are as follows.
1. Ni@Pd nanoparticles with core/shell structure uniformly dispersed on multi-walled carbon nanotubes (Ni@Pd/MWCNTs) is successfully prepared via a two-step strategy:impregnation-reduction methodand replacement method. The Ni@Pd/MWCNTs composite was characterized by transmission electronmicroscopy (TEM), energy-dispersive X-ray spectroscopy (EDS) and X-ray diffraction (XRD) analysis.It shows a uniform dispersion of Ni@Pd nanoparticles with core/shell structure on MWCNTs with the average particle size of3.4nm. XRD show that positive shift of the Pd peaks occurs obviously on the Ni@Pd/MWCNTs comparing with the Pd/MWCNTs, indicating the Ni atoms enter into the Pd crystals which caused the narrow transformation of the Pd crystal lattice distance. The single crystalline Ni@Pd particles are confirmed, the lattice planes with a interlayer distance of0.203nm in the core are indexed to Ni (111) crystal planes, the outer layer with the lattice space of0.224nm corresponds to Pd (111) crystal planes. The Ni@Pd/MWCNTs composite was used as electrocatalyst for alcohol oxidation in alkaline media for fuel cells. The electrocatalytic activity of ethanol oxidation on Ni@Pd/MWCNTs is2.3times higher than that of Pd/MWCNTs electrocatalyst at the same Pd loadings. The enhanced electrocatalytic properties could be attributed to not only the electric synergistic effect between Pd and Ni, but also the high use ratio of Pd for its shell structure.
2. Well dispersed Ni@Pd bimetallic nanoparticles on multi-walled carbon nanotubes (Ni@Pd/MWCNTs) are prepared and used as catalysts for the oxidation of benzyl alcohol. Scanning electron microscopy, transmission electron microscopy, energy-dispersive X-ray spectroscopy analysis, and X-ray diffraction were performed to characterise the synthesized catalyst. The results show a uniform dispersion of Ni@Pd nanoparticles on MWCNTs with an average particle size of4.0nm. The as synthesised catalyst was applied to the oxidation of benzyl alcohol. A99%conversion of benzyl alcohol and a98%selectivity of benzaldehyde were achieved by using the Ni@Pd/MWCNTs (Pd:0.2mmol) catalyst with water as a solvent and H2O2as oxidant at80℃. The catalytic activity of Ni@Pd/MWCNTs towards benzyl alcohol is higher than that of a Pd/MWCNTs catalyst at the same Pd loadings. The catalyst can be easily separated due to its magnetic properties.
3. The uniform dispersion of new highly active Ni@Pd core-shell nanoparticle catalysts supported on graphene (Ni@Pd/graphene) was prepared via a two-step procedure involving a microwave synthesis method and a replacement method. Several characterization tools, such as X-ray powder diffraction (XRD), transmission electron microscopy (TEM), energy-dispersive X-ray spectroscopy (EDS) and Fourier transform infrared spectroscopy (FTIR) were employed to study the phase structures, morphologies and properties of the Ni@Pd/graphene composite. The results indicated that a uniform dispersion of Ni@Pd core-shell structure nanoparticles on graphene have an average particle size of4nm. The Ni@Pd/graphene composite was used as an electrocatalyst for alcohol oxidation in alkaline media for fuel cells. The electrocatalytic activity of Ni@Pd/graphene for ethanol oxidation is3times higher than that of the Pd/grapheme electrocatalyst at the same Pd loading. The enhanced electrocatalytic properties could be attributed not only to the electric synergistic effect between Pd, Ni and graphene, but also the high use ratio of Pd due to its shell structure.
4. The over oxidation of graphene nanosheets were produced by the modify Hummers method with strong oxidants. Abundant oxygen-containing functional groups were present in grapheme oxide, which enable the solubilization of oxidized graphene sheets and thus allow for the intercalation of molecules such as metal precursors into the interlayer space of GO(grapheme oxide). Unfortunately, when the metal ions and GO are mixed and co-reduced to form metal-graphene composite, the subsequent chemical reduction of GO (with metal ions) is required, which makes the abundant oxygen-containing functional groups lost and tends to form irreversible agglomerates or even restack to form graphite. The weak interaction between metal and graphite surfers results in a severe agglomeration of catalytic metal nanoparticles and leads to the loss of its advantage of an ultra-high surface area. To solve this problem, some other intermediates such as poly diallyldimethylammonium chloride (PDDA) and Dimethyldiallylammonium chloride (DMDAAC) have to be introduced.
5. Dimethyldiallylammonium chloride modified reduced graphene oxide supported Pd nanoparticles (Pd/DMDAAC-RGO) were fabricated by polyol microwave heating method. The Pd/DMDAAC-RGOhybrid was characterized by transmission electromicroscopy (TEM), energy-dispersive X-ray spec-troscopy (EDS), X-ray diffraction (XRD) analysis and electrochemical tests. High Pd metal loadings, up to80wt.%with a mean size of1.8nm, were densely in situ decorated on DMDAAC-modified RGO surfaces.Compared with traditional carbon-based Pd catalysts, Pd/DMDAAC-RGO exhibits better activity and stability for ethanol oxidation in alkaline media with the same Pd content on the electrode. This improvedactivity indicates that DMDAAC plays a crucial role in the dispersion and stabilization of Pd nanoparti-cles on RGO sheets and DMDAAC-RGO are able to an alternative support for Pd immobilization in directethanol fuel cells and other catalytic devices.
6. A simple one-pot micro wave-poly ol reduced method was used to anchor platinum nanoparticles on graphene with the aid of PDDA, forming a Pt/PDDA-G hybrid (Pt/PDDA-G). High Pt metal loadings, up to85wt.%with a mean size of1.4nm, were densely in situ decorated on PDDA-modified grapheme surfaces. The electrochemical tests showed that the activity and stability of Pt supported on PDDA-graphene hybrid substrates for methanol oxidation were better than that of Pt supported on graphene sheets, also better than the widely used Pt/carbon black electrocatalysts with the same Pt content on the electrode. This improved activity indicates that PDDA plays a crucial role in the highly dispersion and stabilization of Pt nanoparticles on graphene and PDDA-G are able to an alternative support for Pt immobilization in direct methanol fuel cells.
引文
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