Three-Dimensional Tracking and Visualization of Hundreds of Pt-Co Fuel Cell Nanocatalysts During Electrochemical Aging

被引:151
作者
Yu, Yingchao [3 ]
Xin, Huolin L. [4 ]
Hovden, Robert [1 ,2 ]
Wang, Deli [3 ]
Rus, Eric D. [3 ]
Mundy, Julia A. [1 ]
Muller, David A. [1 ,2 ]
Abruna, Hector D. [3 ]
机构
[1] Cornell Univ, Sch Appl & Engn Phys, Ithaca, NY 14853 USA
[2] Cornell Univ, Kavli Inst, Ithaca, NY 14853 USA
[3] Cornell Univ, Dept Chem & Chem Biol, Ithaca, NY 14853 USA
[4] Cornell Univ, Dept Phys, Ithaca, NY 14853 USA
基金
美国国家科学基金会;
关键词
Tomography; electrocatalysis; STEM; fuel cell; ORR; EELS; TRANSMISSION ELECTRON-MICROSCOPY; CARBON-SUPPORTED PLATINUM; OXYGEN REDUCTION; CATALYST DEGRADATION; CORROSION; NANOPARTICLES; ELECTROCATALYSTS; DISSOLUTION; STABILITY;
D O I
10.1021/nl203920s
中图分类号
O6 [化学];
学科分类号
0703 ;
摘要
We present an electron tomography method that allows for the identification of hundreds of electrocatalyst nanoparticles with one-to-one correspondence before and after electrochemical aging. This method allows us to track, in three-dimensions, the trajectories and morphologies of each Pt-Co nanocatalyst on a fuel cell carbon support. In conjunction with the use of atomic-scale electron energy loss spectroscopic imaging, our experiment enables the correlation of performance degradation of the catalyst with changes in particle/interparticle morphologies, particle-support interactions, and the near-surface chemical composition. We found that aging of the catalysts under normal fuel cell operating conditions (potential scans from +0.6 to +1.0 V for 30 000 cycles) gives rise to coarsening of the nanoparticles, mainly through coalescence, which in turn leads to the loss of performance. The observed coalescence events were found to be the result of nanoparticle migration on the carbon support during potential cycling. This method provides detailed insights into how nanocatalyst degradation occurs in proton exchange membrane fuel cells (PEMFCs) and suggests that minimization of particle movement can potentially slow down the coarsening of the particles and the corresponding performance degradation.
引用
收藏
页码:4417 / 4423
页数:7
相关论文
共 38 条
[1]   An investigation into factors affecting the stability of carbons and carbon supported platinum and platinum/cobalt alloy catalysts during 1.2 V potentiostatic hold regimes at a range of temperatures [J].
Ball, S. C. ;
Hudson, S. L. ;
Thompsett, D. ;
Theobald, B. .
JOURNAL OF POWER SOURCES, 2007, 171 (01) :18-25
[2]   Surface science - The going rate for catalysts [J].
Bowker, M .
NATURE MATERIALS, 2002, 1 (04) :205-206
[3]   The effect of size-dependent nanoparticle energetics on catalyst sintering [J].
Campbell, CT ;
Parker, SC ;
Starr, DE .
SCIENCE, 2002, 298 (5594) :811-814
[4]   VOLTAMMETRIC COMPARISON BETWEEN PLATINUM WITH PREFERRED ORIENTATION AND PLATINUM SINGLE-CRYSTAL ELECTRODES [J].
CERVINO, RM ;
TRIACA, WE ;
ARVIA, AJ .
ELECTROCHIMICA ACTA, 1985, 30 (10) :1323-1327
[5]   Platinum-Alloy Cathode Catalyst Degradation in Proton Exchange Membrane Fuel Cells: Nanometer-Scale Compositional and Morphological Changes [J].
Chen, Shuo ;
Gasteiger, Hubert A. ;
Hayakawa, Katsuichiro ;
Tada, Tomoyuki ;
Shao-Horn, Yang .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 2010, 157 (01) :A82-A97
[6]   Kinetic model of platinum dissolution in PEMFCs [J].
Darling, RM ;
Meyers, JP .
JOURNAL OF THE ELECTROCHEMICAL SOCIETY, 2003, 150 (11) :A1523-A1527
[7]   PARTICLE-SIZE EFFECT OF CARBON-SUPPORTED PLATINUM CATALYSTS FOR THE ELECTROOXIDATION OF METHANOL [J].
FRELINK, T ;
VISSCHER, W ;
VANVEEN, JAR .
JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 1995, 382 (1-2) :65-72
[8]  
Greeley J, 2009, NAT CHEM, V1, P552, DOI [10.1038/nchem.367, 10.1038/NCHEM.367]
[9]   Highly Stable Pt/Ordered Graphitic Mesoporous Carbon Electrocatalysts for Oxygen Reduction [J].
Gupta, Gaurav ;
Slanac, Daniel A. ;
Kumar, Pavan ;
Wiggins-Camacho, Jaclyn D. ;
Kim, Jeongnam ;
Ryoo, Ryong ;
Stevenson, Keith J. ;
Johnston, Keith P. .
JOURNAL OF PHYSICAL CHEMISTRY C, 2010, 114 (24) :10796-10805
[10]   IL-TEM investigations on the degradation mechanism of Pt/C electrocatalysts with different carbon supports [J].
Hartl, Katrin ;
Hanzlik, Marianne ;
Arenz, Matthias .
ENERGY & ENVIRONMENTAL SCIENCE, 2011, 4 (01) :234-238