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强耦合PdM(M = Sn,Pb)/N掺杂石墨烯纳米复合材料对小分子有机化合物的多源协同电催化氧化作用

Multisource Synergistic Electrocatalytic Oxidation Effect of Strongly Coupled PdM (M = Sn, Pb)/N-doped Graphene Nanocomposite on Small Organic Molecules.

作者信息

Wu Peng, Huang Yiyin, Kang Longtian, Wu Maoxiang, Wang Yaobing

机构信息

State Key Laboratory of Structural Chemistry; Key Laboratory of design and assembly of functional nanostructures, Fujian Institute of Research on the Structure of Matter, Chinese Academy of Sciences, YangQiao West Road 155#, Fuzhou, 350002, P. R. China.

出版信息

Sci Rep. 2015 Oct 5;5:14173. doi: 10.1038/srep14173.

Abstract

A series of palladium-based catalysts of metal alloying (Sn, Pb) and/or (N-doped) graphene support with regular enhanced electrocatalytic activity were investigated. The peak current density (118.05 mA cm(-2)) of PdSn/NG is higher than the sum current density (45.63 + 47.59 mA cm(-2)) of Pd/NG and PdSn/G. It reveals a synergistic electrocatalytic oxidation effect in PdSn/N-doped graphene Nanocomposite. Extend experiments show this multisource synergetic catalytic effect of metal alloying and N-doped graphene support in one catalyst on small organic molecule (methanol, ethanol and Ethylene glycol) oxidation is universal in PdM(M = Sn, Pb)/NG catalysts. Further, The high dispersion of small nanoparticles, the altered electron structure and Pd(0)/Pd(II) ratio of Pd in catalysts induced by strong coupled the metal alloying and N-doped graphene are responsible for the multisource synergistic catalytic effect in PdM(M = Sn, Pb) /NG catalysts. Finally, the catalytic durability and stability are also greatly improved.

摘要

研究了一系列具有规则增强电催化活性的金属合金化(Sn、Pb)和/或(N掺杂)石墨烯载体的钯基催化剂。PdSn/NG的峰值电流密度(118.05 mA cm(-2))高于Pd/NG和PdSn/G的总电流密度(45.63 + 47.59 mA cm(-2))。这揭示了PdSn/N掺杂石墨烯纳米复合材料中的协同电催化氧化效应。扩展实验表明,在一种催化剂中金属合金化和N掺杂石墨烯载体对小分子有机化合物(甲醇、乙醇和乙二醇)氧化的这种多源协同催化效应在PdM(M = Sn、Pb)/NG催化剂中是普遍存在的。此外,金属合金化与N掺杂石墨烯的强耦合所诱导的催化剂中小纳米颗粒的高分散性、电子结构的改变以及Pd的Pd(0)/Pd(II)比率,是PdM(M = Sn、Pb)/NG催化剂中多源协同催化效应的原因。最后,催化耐久性和稳定性也得到了极大提高。

https://cdn.ncbi.nlm.nih.gov/pmc/blobs/c46d/4593028/d28184f9905c/srep14173-f1.jpg

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