微波辐照快速合成Pd/石墨烯纳米复合材料及其对甲醇氧化的电催化性能
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摘要
通过微波辅助"一锅合成"的方法,利用环境友好、价格低廉的表没食子儿茶素(EGCG)为还原剂,快速制备了钯/石墨烯(Pd/GN)纳米复合材料,通过控制反应物比例和微波辐照时间对负载在石墨烯上的Pd纳米粒子的尺寸及负载量进行调控。实验结果表明,此Pd/GN纳米复合结构中,Pd纳米粒子均匀分散在石墨烯表面,当氧化石墨(GO)添加量为0.25 m L、微波辐照时间为1 min时,Pd纳米粒子的平均粒径约为10 nm。电化学测试结果表明,Pd/GN复合材料催化剂的电化学活性面积(ECSA)达到60. 5 m~2/g,为商用Pd/C催化剂ECSA(30.7 m~2/g)的1.97倍。另外,在碱性条件下,通过循环伏安法(CV)和计时电流法(CA)研究了Pd/GN的电化学催化甲醇氧化过程,结果表明,与商业Pd/C催化剂相比,Pd/GN催化剂的电催化活性和稳定性都大大提高,当催化剂负载量为15.5μg/cm2时,氧化电流密度峰值达到7.95 mA/cm~2。合成的Pd/GN材料具有优异电催化性能,在甲醇燃料电池领域有良好的应用前景。
Palladium/graphene nanocomposites (Pd/GN) were synthesized through a rapid,microwave irradiation,"one pot"method with epigallocatechin gallate (EGCG) as a reducing agent. The loading amount and size of Pd nanoparticles in Pd/Graphene nanocomposites could be controlled by the irradiation time and the ratio of the graphite oxide (GO) and H_2PdCl_4. Results showed that Pd nanoparticles were well dispersed on the surface of graphene in Pd/GN nanocomposite. When the additive amount of graphene oxide (GO) was 0.25 mL and the microwave irradiation time was 1 min,the size of Pd nanoparticles was about 10 nm. The electro-catalytic activity of the as-prepared Pd/GN towards the oxidation of methanol was studied by cyclic voltammetry (CV) and chronoamperometry (CA) methods. The electrochemical active area (ECSA) value of Pd/GN nanocomposite catalysts was about 60. 5 m~2/g,which was 1. 97 times higher than that of the commercial Pd/C catalyst (30. 7 m~2/g). The peak current density on the Pd/GN catalyst for methanol oxidation was much larger than that of Pd/C catalyst in the alkaline conditions. When the loading amount of the Pd/GN catalyst was about 15. 5 μg/cm~2,the value of the oxidation peak current density reached 7.95 m A/cm~2. All the experimental results indicated that the Pd/GN catalyst significantly enhanced catalytic activity and stability than the commercial Pd/C catalyst.
Palladium/graphene nanocomposites (Pd/GN) were synthesized through a rapid,microwave irradiation,"one pot"method with epigallocatechin gallate (EGCG) as a reducing agent. The loading amount and size of Pd nanoparticles in Pd/Graphene nanocomposites could be controlled by the irradiation time and the ratio of the graphite oxide (GO) and H_2PdCl_4. Results showed that Pd nanoparticles were well dispersed on the surface of graphene in Pd/GN nanocomposite. When the additive amount of graphene oxide (GO) was 0.25 mL and the microwave irradiation time was 1 min,the size of Pd nanoparticles was about 10 nm. The electro-catalytic activity of the as-prepared Pd/GN towards the oxidation of methanol was studied by cyclic voltammetry (CV) and chronoamperometry (CA) methods. The electrochemical active area (ECSA) value of Pd/GN nanocomposite catalysts was about 60. 5 m~2/g,which was 1. 97 times higher than that of the commercial Pd/C catalyst (30. 7 m~2/g). The peak current density on the Pd/GN catalyst for methanol oxidation was much larger than that of Pd/C catalyst in the alkaline conditions. When the loading amount of the Pd/GN catalyst was about 15. 5 μg/cm~2,the value of the oxidation peak current density reached 7.95 m A/cm~2. All the experimental results indicated that the Pd/GN catalyst significantly enhanced catalytic activity and stability than the commercial Pd/C catalyst.
引文
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16 Dreyer D R,Park S J,Bielawski C W,Ruoff R S.Chem.Soc.Rev.,2010,39:228-240
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19 ZHAO Hong-Cai,ZHANG Pu,LI She-Hong,LUO Hong-Xia.Chinese J.Anal.Chem.,2017,45(6):830-836赵鸿彩,张璞,李社红,罗红霞.分析化学,2017,45(6):830-836
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24 MIAO Hui,XIA Juan,JIN Feng,SUN Lin,CUI Yu-Min,LI Hui-Quan,DING Jian.Chinese Journal of Luminescence,2016,37(2):165-173苗慧,夏娟,金凤,孙林,崔玉民,李慧泉,丁建.发光学报,2016,37(2):165-173
25 JING Tao,DAI Ying,MA Xiao-Juan,HUANG Bai-Biao.Chinese Optic.,2016,9(1):1-15荆涛,戴瑛,马晓娟,黄柏标.中国光学,2016,9(1):1-15
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27 Liu M R,Peng C,Yang W K,Guo J J,Zheng Y X,Chen P Q,Huang T T,Xu J.Electrochim.Acta,2015,178:838-84628 Zhang Y T,Chang G,Shu H H,Oyama M,Liu X,He Y B.J.Power Sources,2014,262:279-285
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30 Ga J,Liu F,Ma N,Wang Z,Zhang X.Chem.Mater.,2010,22(7):2213-2218
31 Tung V C,Allen M J,Yang Y,Kaner R B.Nat.Nanotechnol.,2008,4:25-29
32 Liao R,Tang Z,Lei Y,Guo B.J.Phys.Chem.C,2011,115:20740-20746
33 Zou M,Zhu H,Wang P,Bao S,Du M,Zhang M.Nano,2014,9(3):1450031