CO-assisted ex-situ chemical activation of Pt-Cu/C oxygen reduction reaction electrocatalyst

被引:40
作者
Gatalo, Matija [1 ,2 ]
Moriau, Leonard [3 ]
Petek, Ursa [1 ,2 ]
Ruiz-Zepeda, Francisco [1 ,4 ]
Sala, Martin [5 ]
Grom, Matic [3 ]
Galun, Timotej [2 ]
Jovanovic, Primoz [3 ]
Pavlisic, Andraz [3 ]
Bele, Marjan [1 ]
Hodnik, Nejc [3 ]
Gaberscek, Miran [1 ,2 ]
机构
[1] Natl Inst Chem, Dept Mat Chem, Hajdrihova 19, Ljubljana 1000, Slovenia
[2] Univ Ljubljana, Fac Chem & Chem Technol, Vecna Pot 113, Ljubljana 1000, Slovenia
[3] Natl Inst Chem, Dept Catalysis & Chem React Engn, Hajdrihova 19, Ljubljana 1000, Slovenia
[4] Inst Met & Technol, Dept Phys & Chem Mat, Lepi Pot 11, Ljubljana 1000, Slovenia
[5] Natl Inst Chem, Dept Analyt Chem, Hajdrihova 19, Ljubljana 1000, Slovenia
关键词
Oxygen reduction reaction (ORR); Proton exchange membrane fuel cell (PEMFC); Platinum copper; Chemical activation; Carbon monoxide (CO); NANOPARTICLE ELECTROCATALYSTS; UNDERPOTENTIAL DEPOSITION; PLATINUM DISSOLUTION; MODEL SURFACES; PTCU3; STABILITY; ALLOY; SHELL; AU; CATALYSTS;
D O I
10.1016/j.electacta.2019.03.153
中图分类号
O646 [电化学、电解、磁化学];
学科分类号
081704 ;
摘要
In the future, low-temperature proton exchange membrane fuel cells (PEMFC), together with batteries, are expected to compete and eventually replace conventional combustion engines in the automotive industry. Currently, the most promising strategy towards cost-effective and highly-active oxygen reduction reaction (ORR) electrocatalysts seems to be alloying of Pt with less expensive and less noble 3d transition metals (Cu, Co and Ni,...). A crucial issue to be resolved in the near future is, however, to bridge the gap between the remarkable activities measured on the laboratory scale with thin film rotating disk electrode (TF-RDE) and the industrial membrane electrode assembly (MEA). In the case of Pt-Cu alloy, one of the major reasons for this difficulty is inadequate removal of unstable Cu or in other words, improper 'activation'. Inadequately removed Cu can act as an impurity by poisoning the Pt surface via the well-known underpotential deposition (UPD) interaction, resulting in the inhibition of ORR performance. Due to highly favourable experimental conditions, in-situ electrochemical activation (in-situ EA) in TF-RDE setup masks many of the issues one experiences when trying to do the same ex-situ. Thus, matching the ORR performance obtained after in-situ EA with ex-situ CA in the case of Pt-Cu system has not been properly addressed so far. Based on a deeper understanding of in-situ EA of our in-house designed Pt-Cu/C electrocatalyst we here demonstrate development of carbon monoxide (CO) assisted ex-situ CA method. By using this gram scale ex-situ CA method, we for the first time show that a Pt-Cu system can achieve very high ORR performances in TF-RDE setup without any need for the use of in-situ EA. (c) 2019 Elsevier Ltd. All rights reserved.
引用
收藏
页码:377 / 386
页数:10
相关论文
共 62 条
[1]   Electrochemical and Chemical Treatment Methods for Enhancement of Oxygen Reduction Reaction Activity of Pt Shell-Pd Core Structured Catalyst [J].
Aoki, Naoya ;
Inoue, Hideo ;
Shirai, Akira ;
Higuchi, Shunya ;
Matsui, Yuki ;
Daimon, Hideo ;
Doi, Takayuki ;
Inaba, Minoru .
ELECTROCHIMICA ACTA, 2017, 244 :146-153
[2]   Activation of carbon-supported catalysts by ozonized acidic solutions for the direct implementation in (electro-)chemical reactors [J].
Baldizzone, C. ;
Mezzavilla, S. ;
Hodnik, N. ;
Zeradjanin, A. R. ;
Kostka, A. ;
Schueth, F. ;
Mayrhofer, K. J. J. .
CHEMICAL COMMUNICATIONS, 2015, 51 (07) :1226-1229
[3]  
Bard A.J., 1980, ELECTROCHEMICAL METH
[4]   A highly active PtCu3 intermetallic core-shell, multilayered Pt-skin, carbon embedded electrocatalyst produced by a scale-up sol-gel synthesis [J].
Bele, M. ;
Jovanovic, P. ;
Pavlisic, A. ;
Jozinovic, B. ;
Zorko, M. ;
Recnik, A. ;
Chernyshova, E. ;
Hocevar, S. ;
Hodnik, N. ;
Gaberscek, M. .
CHEMICAL COMMUNICATIONS, 2014, 50 (86) :13124-13126
[5]  
Bele M., 2014, Electrocatalytic Composite(s), Associated Composition(s), and Associated Process(es), Patent No. [EP2735044 (A2), 2735044]
[6]  
Bele M., 2013, Electrocatalytic Composite(s), Associated Composition(s), and Associated Process(es), Patent No. [WO2013012398 (A2), 2013012398]
[7]  
Bele M., 2015, Patent No. [US9147885 (B2), 9147885]
[8]  
Bele M., 2016, Electrocatalytic Composite(s), Associated Composition(s), and Associated Process(es), Patent No. [JP6028027 (B2), 6028027]
[9]   INHIBITION OF HYDROGEN ADSORPTION BY SUBMONOLAYER DEPOSITION OF METALS ON PLATINUM [J].
CADLE, SH ;
BRUCKENS.S .
ANALYTICAL CHEMISTRY, 1971, 43 (13) :1858-&
[10]   Highly Crystalline Multimetallic Nanoframes with Three-Dimensional Electrocatalytic Surfaces [J].
Chen, Chen ;
Kang, Yijin ;
Huo, Ziyang ;
Zhu, Zhongwei ;
Huang, Wenyu ;
Xin, Huolin L. ;
Snyder, Joshua D. ;
Li, Dongguo ;
Herron, Jeffrey A. ;
Mavrikakis, Manos ;
Chi, Miaofang ;
More, Karren L. ;
Li, Yadong ;
Markovic, Nenad M. ;
Somorjai, Gabor A. ;
Yang, Peidong ;
Stamenkovic, Vojislav R. .
SCIENCE, 2014, 343 (6177) :1339-1343