abstract - 國立臺灣大學rsliu/poster/2013/syuanhong-ms... · 2014-06-23 · 0.30 0.45 0.60...

1
0.30 0.45 0.60 0.75 0.90 1.05 1.20 -5 -4 -3 -2 -1 0 Current density (mA cm -2 ) Potential (V vs. RHE) 20 w.t. % Pt/C FePtN/C-700 o C-acid FePtN/C-650 o C-acid FePtN/C-600 o C-acid 10 20 30 40 50 60 70 80 Normalized intensity (a.u.) FePtN-2hr-500 o C FePtN-2hr-550 o C FePtN-2hr-600 o C FePtN-2hr-650 o C (111) FePtN-2hr-700 o C (110) (001) (002) (011) (002) (110) (011) Fe 3 PtN-ICSD-44864 Fe 2 N-ICSD-20390 (020) (002) (111) (001) 2Theta (degree) FePt-ICSD-659004 Nitrogen containing FePt Catalyst in Oxygen Reduction Reaction for Fuel Cells Syuan -Hong Chen (陳宣宏) and Ru-Shi Liu * (劉如熹) Department of Chemistry, National Taiwan University, Taipei 106, Taiwan Abstract To promote the commercial of fuel cell, designing a High activity, high stability and low cost catalyst was a critical issue. Recently, the catalyst which iron nitride nanoparticle deposited on the zero dimensional and three dimensional carbon support was synthesized under the ammonia atmosphere and demonstrated a well performance in activity, electron transfer and yield of hydrogen peroxide in oxygen reduction reaction. However, its activity was still lower than commercial Platinum catalyst. The electronic structure was an important factor to enhance the activity and inhabit the side reaction of catalyst. In present study, we established method to improve the activity by importing an electron donor, platinum for example, into the iron nitride catalyst enhance the back donation of active site. In the present study, the characteristics of catalyst were identified by following technology. Crystal structure identified X-ray powder diffraction. X- ray absorption spectroscopy by using synchrotron radiation was applied for oxidation number of iron and platinum. The oxygen reduction performance was identified by cyclic voltammery. Confirm the introduction of platinum into iron nitride catalyst would enhance the catalytic activity. Results Approaching Method Provide a low d-band vacancy element to promote backdonation of oxygen reduction reaction: enhance the activity of reaction X-ray Absorption Spectroscopy for Electronic structure Characterization Transmission Electron Microscopy Introduction XRD Pattern of Different Synthesis Method Conclusions Oxygen Reduction Reaction Performance :Pt :Fe :N Fe 2 N, trigonal Fe 3 PtN, cubic Pt 4+ NH 3 (g) 0.0 0.2 0.4 0.6 0.8 1.0 1.2 -6 -5 -4 -3 -2 -1 0 Current density (mA cm -2 ) Potential (V vs. RHE) 20 wt. % Pt/C FeN/C 10 20 30 40 50 60 70 80 Normalized intensity (a.u.) FePtN/C-600 o C-acid FePtN/C-650 o C-acid FePtN/C-700 o C-acid Fe 3 PtN-ICSD-44864 (002) (110) (011) (111) (001) (002) (011) 2Theta (degree) Fe 2 N-ICSD-20390 7050 7100 7150 7200 7250 7300 Energy (eV) Normalized Intensity Fe foil FeAc 2 FeN/C FePtN/C 11550 11560 11570 11580 11590 11600 Normalized Intensity Energy (eV) Pt foil PtO 2 Fe 3 PtN/C-acid 7112 7116 7120 7124 7128 Normalized Intensity (001) (111) 0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0 1.1 1.2 -5 -4 -3 -2 -1 0 Current density (mA cm -2 ) Potential (V vs. RHE) 20 w.t.% Pt/C FePtN/C FeN/C 0.0 0.2 0.4 0.6 0.8 2 3 4 0 25 50 75 100 Potential (V vs. RHE) 20 w.t. % Pt FePtN/C-700 o C FePtN/C-650 o C FePtN/C-600 o C H 2 O 2 yield (%) Electron number Electron transfer and H 2 O 2 yeild The activity of iron nitride catalyst improved by importing platinum as an electron donor. The oxidation states from XANES conform the electron transfer between iron and platinum. Ref: J. Electrochem. Soc. 1999, 146, 3750. Ref: Adv. Catal. 2000, 45, 71.

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Page 1: Abstract - 國立臺灣大學rsliu/poster/2013/SyuanHong-MS... · 2014-06-23 · 0.30 0.45 0.60 0.75 0.90 1.05 1.20-5-4-3-2-1 0 m-2) Potential (V vs. RHE) 20 w.t. % Pt/C FePtN/C-700oC-acid

0.30 0.45 0.60 0.75 0.90 1.05 1.20-5

-4

-3

-2

-1

0

Cu

rren

t d

ensi

ty (

mA

cm

-2)

Potential (V vs. RHE)

20 w.t. % Pt/C

FePtN/C-700oC-acid

FePtN/C-650oC-acid

FePtN/C-600oC-acid

10 20 30 40 50 60 70 80

No

rm

ali

zed

in

ten

sity

(a

.u.)

FePtN-2hr-500oC

FePtN-2hr-550oC

FePtN-2hr-600oC

FePtN-2hr-650oC

(111)

FePtN-2hr-700oC

(110)

(001)

(002)

(011)

(002)

(110)

(011)

Fe3PtN-ICSD-44864

Fe2N-ICSD-20390

(020)

(002)

(111)

(001)

2Theta (degree)

FePt-ICSD-659004

Nitrogen containing FePt Catalyst in Oxygen

Reduction Reaction for Fuel Cells

Syuan-Hong Chen (陳宣宏) and Ru-Shi Liu* (劉如熹)

Department of Chemistry, National Taiwan University, Taipei 106, Taiwan

Abstract

To promote the commercial of fuel cell, designing a High activity, high stability and low cost catalyst was a critical issue. Recently, the catalyst which

iron nitride nanoparticle deposited on the zero dimensional and three dimensional carbon support was synthesized under the ammonia atmosphere and

demonstrated a well performance in activity, electron transfer and yield of hydrogen peroxide in oxygen reduction reaction. However, its activity was still

lower than commercial Platinum catalyst.

The electronic structure was an important factor to enhance the activity and inhabit the side reaction of catalyst. In present study, we established

method to improve the activity by importing an electron donor, platinum for example, into the iron nitride catalyst enhance the back donation of active site.

In the present study, the characteristics of catalyst were identified by following technology. Crystal structure identified X-ray powder diffraction. X-

ray absorption spectroscopy by using synchrotron radiation was applied for oxidation number of iron and platinum. The oxygen reduction performance

was identified by cyclic voltammery. Confirm the introduction of platinum into iron nitride catalyst would enhance the catalytic activity.

Results

Approaching Method

Provide a low d-band vacancy element to promote backdonation of oxygen reduction reaction: enhance the activity of reaction

X-ray Absorption Spectroscopy for

Electronic structure Characterization

Transmission Electron Microscopy

Introduction

XRD Pattern of Different Synthesis Method

Conclusions

Oxygen Reduction Reaction Performance

:Pt :Fe :N

Fe2N, trigonal Fe3PtN, cubic

Pt4+

NH3(g)

0.0 0.2 0.4 0.6 0.8 1.0 1.2-6

-5

-4

-3

-2

-1

0

Cu

rren

t d

en

sity

(m

A c

m-2

)

Potential (V vs. RHE)

20 wt. % Pt/C

FeN/C

10 20 30 40 50 60 70 80

No

rm

ali

zed

in

ten

sity

(a

.u.)

FePtN/C-600oC-acid

FePtN/C-650oC-acid

FePtN/C-700oC-acid

Fe3PtN-ICSD-44864

(002)

(110)

(011)

(111)

(001)

(002)

(011)

2Theta (degree)

Fe2N-ICSD-20390

7050 7100 7150 7200 7250 7300

Energy (eV)

Norm

ali

zed

In

ten

sity

Fe foil

FeAc2

FeN/C

FePtN/C

11550 11560 11570 11580 11590 11600

Norm

ali

zed

In

ten

sity

Energy (eV)

Pt foil

PtO2

Fe3PtN/C-acid

7112 7116 7120 7124 7128

Norm

ali

zed

In

ten

sity

(001)

(111)

0.3 0.4 0.5 0.6 0.7 0.8 0.9 1.0 1.1 1.2-5

-4

-3

-2

-1

0

Cu

rren

t d

ensi

ty (

mA

cm

-2)

Potential (V vs. RHE)

20 w.t.% Pt/C

FePtN/C

FeN/C

0.0 0.2 0.4 0.6 0.82

3

4

0

25

50

75

100

Potential (V vs. RHE)

20 w.t. % Pt

FePtN/C-700oC

FePtN/C-650oC

FePtN/C-600oC

H2O

2 y

ield

(%

)

Ele

ctr

on

nu

mb

er

Electron transfer and H2O2 yeild

The activity of iron nitride catalyst improved by importing

platinum as an electron donor. The oxidation states from XANES

conform the electron transfer between iron and platinum.

Ref: J. Electrochem. Soc. 1999, 146, 3750. Ref: Adv. Catal. 2000, 45, 71.