We describe the development and test of an elevated pressure and temperature rotating disk electrode (RDE) system that allows measurements under well-defined mass transport conditions. As demonstrated for the oxygen reduction reaction on polycrystalline platinum (Pt) in 0.5M H2SO4, the setup can easily be operated in a pressure range of 1–101 bar oxygen, and temperature of 140 °C. Under such conditions, diffusion limited current densities increase by almost two orders of magnitude as compared to conventional RDE setups allowing, for example, fuel cell catalyst studies under more realistic conditions. Levich plots demonstrate that the mass transport is indeed well-defined, i.e., at low electrode potentials, the measured current densities are fully diffusion controlled, while at higher potentials, a mixed kinetic-diffusion controlled regime is observed. Therefore, the setup opens up a new field for RDE investigations under temperature and current density conditions relevant for low and high temperature proton exchange membrane fuel cells.

1.
T. J.
Schmidt
,
H. A.
Gasteiger
,
G. D.
Stab
,
P. M.
Urban
,
D. M.
Kolb
, and
R. J.
Behm
,
J. Electrochem. Soc.
145
,
2354
(
1998
).
2.
C. M.
Zalitis
,
D.
Kramer
, and
A. R.
Kucernak
,
Phys. Chem. Chem. Phys.
15
,
4329
(
2013
).
3.
S. S.
Kocha
,
J. D.
Yang
, and
J. S.
Yi
,
AIChE J.
52
,
1916
(
2006
).
4.
A.
Heinzel
and
V. M.
Barragán
,
J. Power Sources
84
,
70
(
1999
).
5.
Z.
Liu
,
J. S.
Wainright
,
M. H.
Litt
, and
R. F.
Savinell
,
Electrochim. Acta
51
,
3914
(
2006
).
6.
L.
Qingfeng
,
X.
Gang
,
H. A.
Hjuler
,
R. W.
Berg
, and
N. J.
Bjerrum
,
J. Electrochem. Soc.
141
,
3114
(
1994
).
7.
J. M.
Bisang
,
K.
Jüttner
, and
G.
Kreysa
,
Electrochim. Acta
39
,
1297
(
1994
).
8.
G. K. H.
Wiberg
,
M. J.
Fleige
, and
M.
Arenz
,
Rev. Sci. Instrum.
85
,
085105
(
2014
).
9.
J.
Fuhrmann
,
H.
Zhao
,
E.
Holzbecher
,
H.
Langmach
,
M.
Chojak
,
R.
Halseid
,
Z.
Jusys
, and
J.
Behm
,
Phys. Chem. Chem. Phys.
10
,
3784
(
2008
).
10.
S. J.
Ashton
,
Design, Construction and Research Application of a Differential Electrochemical Mass Spectrometer (DEMS)
(
Springer
,
Berlin
,
2012
).
11.
M.
Nesselberger
,
S. J.
Ashton
,
G. K. H.
Wiberg
, and
M.
Arenz
,
Rev. Sci. Instrum.
84
,
074103
(
2013
).
12.
S.
Hamada
,
M.
Itoh
,
H.
Matsuda
, and
J.
Yamada
,
J. Electroanal. Chem. Interfacial Electrochem.
44
(
2
),
189
(
1973
).
13.
T. J.
Schmidt
,
U. A.
Paulus
,
H. A.
Gasteiger
, and
R. J.
Behm
,
J. Electroanal. Chem.
508
,
41
(
2001
).
14.
T.
Rettich
,
J. Chem. Thermodyn.
32
,
1145
(
2000
).
15.
Q.
Li
,
R.
He
,
J. O.
Jensen
, and
N. J.
Bjerrum
,
Fuel Cells
4
,
147
(
2004
).
16.
B. R.
Scharifker
,
J. Electrochem. Soc.
134
,
2714
(
1987
).
17.
18.
R. T.
Ferrell
and
D. M.
Himmelblau
,
J. Chem. Eng. Data
12
,
111
(
1967
).
19.
P.
Han
and
D. M.
Bartels
,
J. Phys. Chem.
100
,
5597
(
1996
).
20.
K. E.
Gubbins
,
M. K.
Tham
, and
R. D.
Walker
,
J. Phys. Chem.
74
,
1747
(
1970
).
21.
A.
Bard
and
L.
Faulkner
, in
Electrochemical Methods: Fundamentals and Applications
(
Wiley
,
New York
,
2002
), Vol.
2001
.
22.
F.
Gloaguen
,
F.
Andolfatto
,
R.
Durand
, and
P.
Ozil
,
J. Appl. Electrochem.
24
,
863
(
1994
).
23.
U. A.
Paulus
,
T. J.
Schmidt
,
H. A.
Gasteiger
, and
R. J.
Behm
,
J. Electroanal. Chem.
495
,
134
(
2001
).
24.
A.
Wexler
,
J. Res. Natl. Bur. Stand., Sect. A
80A
,
775
(
1976
).
25.
J.
McBreen
,
W. E.
O’Grady
, and
R.
Richter
,
J. Electrochem. Soc.
131
(
5
),
1215
1216
(
1984
).
26.
Teflon PTFE 7A®: Properties Handbook (Dupont, 1996).
27.
V ictrex® PEEK 450G: Material Properties (Victrex, 2014).
28.
See supplementary material at http://dx.doi.org/10.1063/1.4922382 for determination of the temperature coefficient of potential of RHE vs Ag qRE, and for cyclic voltammetry of Pt poly in Argon saturated electrolyte.
29.
B. E.
Conway
and
J. C.
Currie
,
J. Chem. Soc., Faraday Trans. 1
74
,
1390
(
1978
).
30.
M.
Nesselberger
,
S.
Ashton
,
J. C.
Meier
,
I.
Katsounaros
,
K. J. J.
Mayrhofer
, and
M.
Arenz
,
J. Am. Chem. Soc.
133
,
17428
(
2011
).
31.
K. J. J.
Mayrhofer
,
D.
Strmcnik
,
B. B.
Blizanac
,
V.
Stamenkovic
,
M.
Arenz
, and
N. M.
Markovic
,
Electrochim. Acta
53
,
3181
(
2008
).
32.
H. A.
Gasteiger
,
S. S.
Kocha
,
B.
Sompalli
, and
F. T.
Wagner
,
Appl. Catal., B
56
,
9
(
2005
).

Supplementary Material

You do not currently have access to this content.