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Electronic Supplementary Material (ESI) for Physical Chemistry Chemical Physics.

This journal is the Owner Societies 2014

Carrier dynamics of a visible-light-responsive Ta3N5


photoanode for water oxidation
Ahmed Ziani,a Ela Nurlaela,a Dattatray S. Dhawale,a Diego Alves Silva,a
Erkki Alarousu,b Omar F. Mohammed,b and Kazuhiro Takanabea*
a

Division of Physical Sciences and Engineering,


KAUST Catalysis Center (KCC),
b
Solar and Photovoltaic Engineering Research Center (SPERC)
King Abdullah University of Science and Technology (KAUST)
Thuwal, 23955-6900 (Saudi Arabia)
*
E-mail: kazuhiro.takanabe@kaust.edu.sa
http://catec.kaust.edu.sa

Fig. S1. Cyclic voltammogram of a) 160 nm, b) 370 nm, c) 470 nm, and d) 6 x 160 nm Ta3N5
films at different scan rates. The experiments were conducted under bubbling Ar using a 0.5 M
NaOH solution (pH 13.5) as the electrolyte, a Pt wire as the counter electrode, and Ag/AgCl as
the reference electrode.

Fig. S2. Plot showing the linear relationship between the capacitive current and the scan rate for
all of the films.

Table S1. Relative electrochemical active surface areas of Ta3N5 films (using 160 nm film as the
baseline)
Film thickness (nm)

Capacitance (F cm-2)

160

10.3

320

8.6

470

18.3

6 160

94.6

Fig. S3. Mott-Schottky plots at different frequencies taken at two different potential range
for a) 160, b) 320, c) 470, and d) 6 160 nm Ta3N5 film. The experiments were conducted
under bubbling Ar using a 0.5 M NaOH solution (pH 13.5) as the electrolyte, a Pt wire as
the counter electrode, and Ag/AgCl as the reference electrode.

Table S2. Potentials at x-intercept and donor density for Ta3N5 films with different
thickness calculated from Mott-Schottky plots.

160

Intercept
potential from
potential
range of 1.21.0 V vs. RHE
(V vs. RHE)
0.9

4 1020

Intercept
potential from
potential range
of 0.6-0.1 V vs.
RHE
(V vs. RHE)
0.1

320

0.9

5 1020

0.05

6 1021

470

0.85

4 1020

0.1

4 1022

6 160

1.1

2 1021

0.15

2 1024

Film
thickness
(nm)

Donor density
(cm3)

Donor density
(cm3)
5 1021

Fig. S4. Nyquist plots of a) 160 nm and c) 370 nm and Bode plots of b) 160 nm and d) 370
nm Ta3N5 films obtained from staircase potential electrochemical impedance spectra
used to calculate the Mott-Schottky plots of the samples. The amplitude of the perturbation
signal was 5 mV (0.5 M NaOH, pH 13.5).

Fig. S5. Nyquist plots of a) 470 nm and c) 6 160 nm and Bode plots of b) 470 nm and d)
6 160 nm Ta3N5 films obtained from staircase potential electrochemical impedance
spectra used to calculate the Mott-Schottky plots of the samples. The amplitude of the
perturbation signal was 5 mV (0.5 M NaOH, pH 13.5).

Fig. S6. Linear sweep voltammogram (anodic direction) of 160 nm Ta3N5 film with and without
Co cocatalyst under AM 1.5 G solar light irradiation in a 0.1 M Na2SO4 electrolyte solution (pH
13 adjusted by adding NaOH) at 10 mV sec1.

Fig. S7. Linear sweep voltammogram of 160 nm Ta3N5 film on a Pt (200 nm) grown on silicon
(100) substrate under AM 1.5 solar light irradiation in a 0.1 M Na2SO4 electrolyte solution.