This work aims at studying protonic transport of mixed proton–electron-conducting Nd5.5WO11.25-δ oxide synthesized by a citrate method as material for hydrogen separation membranes. Structure of samples was characterized by X-ray diffraction (XRD), and protonic mobility was studied using temperature-programmed desorption of H2O and isotope heteroexchange of the bulk protons with D2O as well as mass relaxation after an abrupt change of H2O partial pressure. The temperature range of Nd5.5WO11.25-δ efficient operation is 300–400 °C, where H+ tracer diffusion and chemical diffusion coefficients are ∼1 × 10−11 and ∼2 × 10−5 cm2/s, respectively, being comparable to or even better than those for similar systems. Hence, Nd5.5WO11.25-δ is a promising material for the design of hydrogen separation membranes.

References

1.
Tao
,
Z.
,
Yan
,
L.
,
Qiao
,
J.
,
Wang
,
B.
,
Zhang
,
L.
, and
Zhang
,
J.
,
2015
, “
A Review of Advanced Proton-Conducting Materials for Hydrogen Separation
,”
Prog. Mater. Sci.
,
74
, pp.
1
50
.
2.
Ma
,
Y. H.
,
2008
, “
Hydrogen Separation Membranes
,”
Advanced Membrane Technology and Applications
,
N. N.
Li
,
A. G.
Fane
,
W. S. W.
Ho
, and
T.
Matsuura
, eds.,
Wiley
,
Hoboken, NJ
, pp.
671
684
.
3.
Ockwig
,
N. W.
, and
Nenoff
,
T. M.
,
2007
, “
Membranes for Hydrogen Separation
,”
Chem. Rev. Am. Chem. Soc.
,
107
(
10
), pp.
4078
4110
.
4.
Hancke
,
R.
,
Magrasó
,
A.
,
Norby
,
T.
, and
Haugsrud
,
R.
,
2013
, “
Hydration of Lanthanum Tungstate (La/W=5.6 and 5.3) Studied by TG and Simultaneous TG–DSC
,”
Solid State Ionics
,
231
, pp.
25
29
.
5.
Solís
,
C.
,
Escolastico
,
S.
,
Haugsrud
,
R.
, and
Serra
,
J. M.
,
2011
, “
La5.5WO12-δ Characterization of Transport Properties Under Oxidizing Conditions: A Conductivity Relaxation Study
,”
J. Phys. Chem. C.
,
115
(
22
), pp.
11124
11131
.
6.
Haugsrud
,
R.
,
2007
, “
Defects and Transport Properties in Ln6WO12 (Ln = La, Nd, Gd, Er)
,”
Solid State Ionics
,
178
(
7–10
), pp.
555
560
.
7.
Roitsch
,
S.
,
Barthel
,
J.
, and
Mayer
,
J.
,
2012
, “
Structural Investigations on Gas-Separation Membrane Materials by Transmission Electron Microscopy
,”
15th European Microscopy Congress (EMC)
,
Manchester, UK
, Sept. 16–21, Paper No. 492.
8.
Escolástico
,
S.
,
Solís
,
C.
,
Scherb
,
T.
,
Schumacher
,
G.
, and
Serra
,
J. M.
,
2013
, “
Hydrogen Separation in La5.5WO11.25-δ Membranes
,”
J. Membr. Sci.
,
444
, pp.
276
284
.
9.
Partin
,
G. S.
,
Korona
,
D. V.
,
Neiman
,
A. Y.
, and
Belova
,
K. G.
,
2015
, “
Conductivity and Hydration of Fluorite-Type La6-xWO12-1.5x Phases (x = 0.4; 0.6; 0.8; 1)
,”
Russ. J. Electrochem.
,
51
(
5
), pp.
381
390
.
10.
Magrasó
,
A.
, and
Haugsrud
,
R.
,
2014
, “
Effects of The La/W Ratio and Doping on the Structure, Defect Structure, Stability and Functional Properties of Proton-Conducting Lanthanum Tungstate La28-xW4+xO54+δ—A Review
,”
J. Mater. Chem. A
,
2
(
32
), pp.
12630
12641
.
11.
Escolástico
,
S.
,
Somacescu
,
S.
, and
Serra
,
J. M.
,
2014
, “
Solid State Transport and Hydrogen Permeation in the System Nd5.5W1-xRexO11.25-δ
,”
Chem. Mater.
,
26
(
2
), pp.
982
992
.
12.
McCarthy
,
G. J.
,
Fischer
,
R. D.
,
Johnson
,
G. G. J.
, and
Gooden
,
C. E.
,
1972
, “
Crystal Chemistry and Compound Formation in the Systems Rare Earth Sesquioxide—WO3
,”
Nat. Bur. Stand. (U. S.)
,
4
(
15
), pp.
397
411
.
13.
Trunov
,
V.
,
Tuushevskaya
,
G.
, and
Afonskii
,
N.
,
1968
, “
Investigation of the Double Oxides Formed in the Reaction of Nd2O3, Sm2O3, and Er2O3 With Tungsten (VI) Oxide
,”
Russ. J. Inorg. Chem.
,
13
(
4
), pp.
491
493
.
14.
Scherb
,
T.
,
2011
, “
Strukturelle Charakterisierung von Wasserstoff Trennenden Gasseparationsmembranen auf Lanthanoid-Wolframat-Basis
,” Ph.D. dissertation, Technische Universität Berlin, Berlin.
15.
Escolástico
,
S.
,
Solís
,
C.
,
Haugsrud
,
R.
,
Magrasó
,
A.
, and
Serra
,
J. M.
,
2017
, “
On the Ionic Character of H2 Separation Through Mixed Conducting Nd5.5W0.5Mo0.5O11.25-δ Membrane
,”
Int. J. Hydrogen Energy
,
42
(
16
), pp.
11392
11399
.
16.
Escolástico
,
S.
, and
Serra
,
J. M.
,
2015
, “
Nd5.5W1-xUxO11.25-δ System: Electrochemical Characterization and Hydrogen Permeation Study
,”
J. Membr. Sci.
,
489
, pp.
112
118
.
17.
Ryu
,
J. H.
,
Yoon
,
J.-W.
,
Lim
,
C. S.
,
Oh
,
W.-C.
, and
Shim
,
K. B.
,
2005
, “
Microwave-Assisted Synthesis of Nanocrystalline MWO4 (M: Ca, Ni) Via Water-Based Citrate Complex Precursor
,”
Ceram. Int.
,
31
(
6
), pp.
883
888
.
18.
Sadykov
,
V.
,
Sadovskaya
,
E.
,
Bobin
,
A.
,
Kharlamova
,
T.
,
Uvarov
,
N.
,
Ulikhin
,
A.
,
Argirusis
,
C.
,
Sourkouni
,
G.
, and
Stathopoulos
,
V.
,
2015
, “
Temperature-Programmed C18O2 SSITKA for Powders of Fast Oxide-Ion Conductors: Estimation of Oxygen Self-Diffusion Coefficients
,”
Solid State Ionics
,
271
, pp.
69
72
.
19.
Sadykov
,
V.
,
Sadovskaya
,
E.
, and
Uvarov
,
N.
,
2015
, “
Methods of Isotopic Relaxations for Estimation of Oxygen Diffusion Coefficients in Solid Electrolytes and Materials With Mixed Ionic-Electronic Conductivity
,”
Russ. J. Electrochem.
,
51
(
5
), pp.
458
467
.
20.
Den Otter
,
M.
,
2000
, “
Numerical Evaluation of Eigenvalues of the Sheet Diffusion Problem in the Surface/Diffusion Mixed Regime
,”
Solid State Ionics
,
134
(
3
4
), pp.
259
264
.
21.
Den Otter
,
M. W.
,
Bouwmeester
,
H. J. M.
,
Boukamp
,
B. A.
, and
Verweij
,
H.
,
2001
, “
Reactor Flush Time Correction in Relaxation Experiments
,”
J. Electrochem. Soc.
,
148
(
2
), pp.
J1
J6
.
22.
Poetzsch
,
D.
,
Merkle
,
R.
, and
Maier
,
J.
,
2014
, “
Proton Conductivity in Mixed-Conducting BSFZ Perovskite From Thermogravimetric Relaxation
,”
Phys. Chem. Chem. Phys.
,
16
(
31
), pp.
16446
16453
.
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