Making ultrafine and highly-dispersive multimetallic nanoparticles in three-dimensional graphene with supercritical fluid as excellent electrocatalyst for oxygen reduction reaction

Making ultrafine and highly-dispersive multimetallic nanoparticles in three-dimensional graphene with supercritical fluid as excellent electrocatalyst for oxygen reduction reaction
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用超临界流体在三维石墨烯中制备超细、高分散的多金属纳米粒子作为氧还原反应的优异电催化剂

DOI:
10.1039/c6ta08508c
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发表时间:
2016-11
影响因子:
11.9
通讯作者:
杨娟
杨娟
中科院分区:
材料科学2区
文献类型:
--
作者:
周亚洲;Clive H Yen;程晓农;Chien M. Wai;杨娟

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三维石墨烯具有高比表面积、大孔容和优异的电学性能,是设计多孔电极材料的理想载体。然而,所报道的多孔电极材料的电化学性能仍需要进一步改进。当前的挑战是如何在3D石墨烯中存款具有可控结构、负载和组成的所需纳米颗粒(NPs),同时保持高分散性。在这里,我们展示了一种改进的超临界流体(SCF)技术,以解决这个问题,通过控制SCF系统。利用这种上级方法,成功合成了一系列具有超细尺寸、高分散性和成分可控性的Pt基/3D石墨烯材料。具体地,所得到的Pt 40 Fe 60/3D石墨烯显示出对于氧还原反应(ORR)的电催化性能的显著增强,包括质量活性的14.2倍增强(1.70A mgPt-1)、比活性的11.9倍增强(1.55mA cm-2)以及与Pt/C催化剂相比更高的耐久性。经过仔细比较,Pt 40 Fe 60/3D石墨烯催化剂显示出比大多数报道的类似3D石墨烯基催化剂更高的ORR活性。通过这种方法成功合成这种有吸引力的材料也为开发广泛应用的3D石墨烯铺平了道路。
Three-dimensional (3D) graphene showed an advanced support for designing porous electrode materials due to its high specific surface area, large pore volume, and excellent electronic property. However, the electrochemical properties of reported porous electrode materials still need to be improved further. The current challenge is how to deposit desirable nanoparticles (NPs) with controllable structure, loading and composition in 3D graphene while maintaining the high dispersion. Herein, we demonstrate a modified supercritical fluid (SCF) technique to address this issue by controlling the SCF system. Using this superior method, a series of Pt-based/3D graphene materials with the ultrafine-sized, highly dispersive and controllable composition multimetallic NPs were successfully synthesized. Specifically, the resultant Pt40Fe60/3D graphene showed a significant enhancement in electrocatalytic performance for the oxygen reduction reaction (ORR), including a factor of 14.2 enhancement in mass activity (1.70 A mgPt−1), a factor of 11.9 enhancement in specific activity (1.55 mA cm−2), and higher durability compared with that of Pt/C catalyst. After careful comparison, the Pt40Fe60/3D graphene catalyst shows the higher ORR activity than most of the reported similar 3D graphene-based catalysts. The successful synthesis of such attractive materials by this method also paves the way to develop 3D graphene in widespread applications.
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