Understanding Pt Nanoparticle Anchoring on Graphene Supports through Surface Functionalization

被引:168
作者
Xing, Le [1 ]
Yang, Fan [1 ]
Rasouli, Somaye [2 ]
Qiu, Yang [3 ]
Li, Zhe-Fei [1 ]
Uzunoglu, Aytekin [4 ]
Sun, Cheng-Jun [6 ]
Liu, Yuzi [7 ]
Ferreira, Paulo [2 ]
Li, Wenzhen [3 ]
Ren, Yang [6 ]
Stanciu, Lia A. [4 ,5 ]
Xie, Jian [1 ]
机构
[1] Indiana Univ Purdue Univ, Purdue Sch Engn & Technol, Dept Mech Engn, Indianapolis, IN 46202 USA
[2] Univ Texas Austin, Mat Sci & Engn Program, Austin, TX 78712 USA
[3] Iowa State Univ, Biorenewables Res Lab, Dept Chem & Biol Engn, Ames, IA 50011 USA
[4] Purdue Univ, Sch Mat Engn, W Lafayette, PA 47907 USA
[5] Purdue Univ, Weldon Sch Biomed Engn, W Lafayette, PA 47907 USA
[6] Argonne Natl Lab, Adv Photon Source, 9700 S Cass Ave, Argonne, IL 60439 USA
[7] Argonne Natl Lab, Ctr Nanoscale Mat, 9700 S Cass Ave, Argonne, IL 60439 USA
来源
ACS CATALYSIS | 2016年 / 6卷 / 04期
关键词
surface functionalization; graphene; metal-support interaction; catalyst durability; oxygen reduction reaction; PEMFC; FUEL-CELL ELECTROCATALYST; OXYGEN REDUCTION ACTIVITY; PLATINUM NANOPARTICLES; DEGRADATION MECHANISMS; ELECTRONIC-PROPERTIES; CARBON NANOTUBES; DURABILITY; CATALYSTS; CO; ALLOY;
D O I
10.1021/acscatal.5b02722
中图分类号
O64 [物理化学(理论化学)、化学物理学];
学科分类号
070304 ; 081704 ;
摘要
The enhancement of Pt nanoparticle anchoring strength and dispersion on carbon supports is highly desirable in polymer electrolyte membrane fuel cells (PEMFCs) as well as in other catalysis processes. Presented here is a comprehensive study of the interaction between catalyst nanoparticles and carbon supports in terms of the electronic structure change and its effects on the electrocatalytic performance of supported catalysts. Graphene was chosen as an ideal model support because the unique 2-D structure allows the direct investigation of the interaction with supported metal nanoparticles at their interface. We developed a facile strategy to covalently graft p-phenyl SO3H or p-phenyl NH2-groups onto the graphene surface. The functional groups were found to not only facilitate the homogeneous distribution of Pt nanoparticles on the surface of graphene supports and reduce the Pt average particle size but also strengthen the interaction of the Pt atoms with the functional groups and, consequently, minimize the migration/coalescence of the Pt nanoparticles in the course of accelerated durability tests. The experimental results from both X-ray photoelectron spectroscopy (XPS) and X-ray absorption spectroscopy (XAS) demonstrate the electron density shift from Pt to graphene supports with the strength of the Pt graphene interaction following the trend of Pt/p-phenyl NH2-graphene > Pt/p-phenyl SO3H-graphene > Pt/graphene. This study will shed light on strategies to improve not only the durability but also the activity of the metal nanoparticles via the functionalization of the catalyst supports in the catalysis field.
引用
收藏
页码:2642 / 2653
页数:12
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