氮掺杂碳纳米笼担载的铂基高效甲醇氧化电催化剂
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摘要
高性能甲醇氧化电催化剂的制备是直接甲醇燃料电池实用化进程中的一大挑战。本文以高比表面积的介观结构氮掺杂碳纳米笼(hNCNC)为新型载体~(1,2),利用掺杂氮的配位和锚定作用,通过简便的微波辅助多元醇还原法,制得了颗粒高度分散、粒径均匀(3.3 nm)、负载量为20 wt.%的Pt/hNCNC催化剂。该催化剂对甲醇氧化反应表现出优异的电催化活性和稳定性,显著优于负载于形貌相似的碳纳米笼(hCNC)~3及商用活性炭XC-72上的对照组催化剂。该催化剂的高活性的主要原因是氮掺杂位增强了Pt与载体的相互作用,有利于Pt纳米粒子在载体表面的高分散锚定,从而使Pt/hNCNC催化剂具有更高的电化学活性表面积~4。该研究展示了新型hNCNC载体及其担载的铂基电催化剂在直接甲醇燃料电池中的应用前景。
Hierarchical nitrogen-doped carbon nanocages(hNCNC) with large specific surface area were used as a new support to immobilize Pt nanoparticles via a microwave-assistant polyol method. The as-constructed Pt/hNCNC catalyst with a loading of 20 wt.% consists of high dispersed Pt nanoparticles with the average size of 3.3 nm, which are smaller than the Pt nanoparticles supported on hierarchical carbon nanocages(hCNC) and commercial Vulcan XC-72 with the same loading. Accordingly, the Pt/hNCNC possesses a larger electrochemical surface area than Pt/hCNC and Pt/XC-72. The Pt/hNCNC catalyst exhibits an excellent electrocatalytic activity and stability toward methanol oxidation, obviously superior to the control catalysts, which could be attributed to the enhanced interaction between Pt species and hNCNC due to the anchoring function of nitrogen dopants.
引文
[1]Chen,S.;Bi,J.;Zhao,Y.;Yang,L.;Zhang,C.;Ma,Y.;Wu,Q.Wang,X.;Hu,Z.Adv.Mater.2012,24:5593.
    [2]Zhao,J.;Lai,H.;Lyu,Z.;Jiang,Y.;Xie,K.;Wang,X.;Wu,Q.;Yang,L.;Jin,Z.;Ma,Y.;Liu,J.;Hu,Z.Adv.Mater.2015,27:3541.
    [3]Xie,K.;Qin,X.;Wang,X.;Wang,Y.;Tao,H.;Wu,Q.;Yang,L.;Hu,Z.Adv.Mater.2012,24:347.
    [4]Jiang,X.;Wang,X.;Wu,Q.;Wang,Y.;Ma,Y.;Wang,X.;Hu,Z.Chin.J.Catal.(Accepted).

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