Pd-Co carbon-nitride electrocatalysts for polymer electrolyte fuel cells

被引：62

作者：

Di Noto, Vito ^{[1
,3
]}

Negro, Enrico ^{[1
]}

Lavina, Sandra ^{[1
]}

Gross, Silvia ^{[3
]}

Pace, Giuseppe ^{[2
]}

机构：

[1] Univ Padua, Dipartimento Sci Chim, I-35131 Padua, Italy

[2] CNR, ISTM, Dipartimento Proc Chim Ingn, I-35131 Padua, Italy

[3] CNR, ISTM, Dipartimento Sci Chim, I-35131 Padua, Italy

来源：

ELECTROCHIMICA ACTA | 2007年 / 53卷 / 04期

关键词：

PEM fuel cells; pd-co carbon-nitride electrocatalysts; vibrational spectroscopy; XPS; CV-TF-RDE method;

D O I：

10.1016/j.electacta.2007.05.028

中图分类号：

O646 [电化学、电解、磁化学];

学科分类号：

081704 ;

摘要：

in this paper is described the preparation of new platinum-free Pd-Co carbon-nitride electrocatalysts (Pd-Co-CNs) for application in low-temperature fuel cells. Two groups of materials with formula K-n[PdxCoyCzNlHm] were synthesized, which are grouped in two ensembles: the first is characterized by a molar ratio y/x > 1(I), and the second by y/x < 1 (II). K-n[PdxCoyCzNlHm] materials were prepared through a two-step synthesis protocol. The effect of the Pd/Co molar ratio and of the temperature of the thermal treatments on the structure and properties of the products were studied extensively by thermogravimetry, scanning electron microscopy, and vibrational (FT-IR and micro-Raman) and XPS spectroscopy. Vibrational studies revealed that I and II systems consist of two polymorphs of alpha- and graphitic-like carbon-nitride nanomaterials. The electrochemical activity towards the oxygen reduction reaction (ORR) and the hydrogen oxidation reaction (HOR) was measured by cyclic voltarnmetry measurements with thin-film rotating disk electrode (CV-TF-RDE). The electrochemical performance of Pd-Co-CNs of group I obtained at t(f) >= 700 degrees C resulted higher than that measured for a platinum-based commercial electrocatalyst in terms of both the activity towards the ORR and the HOR and of the resistance towards the poisoning effect of methanol towards the ORR. (c) 2007 Elsevier Ltd. All rights reserved.

引用

页码：1604 / 1617

页数：14

共 43 条

[31] Carbon supported Pt-Co alloys electrocatalysts for as methanol-resistant oxygen-reduction direct methanol fuel cells [J].

Salgado, JRC ;

Antolini, E ;

Gonzalez, ER .

APPLIED CATALYSIS B-ENVIRONMENTAL, 2005, 57 (04) :283-290

[32]

SATO MH, 2006, J AM CHEM SOC, V128, P3526

[33]

SCHMIDT TJ, 2003, HDB FUEL CELLS FUNDA, V2, pCH22

[34] HIGH-RESOLUTION X-RAY PHOTOEMISSION SPECTRUM OF VALENCE BANDS OF GOLD [J].

SHIRLEY, DA .

PHYSICAL REVIEW B, 1972, 5 (12) :4709-&

[35] RAMAN AND IR STUDIES OF GRAPHITE INTERCALATES [J].

SOLIN, SA .

PHYSICA B & C, 1980, 99 (1-4) :443-452

[36] Structure-relationships in electrocatalysis: oxygen reduction and hydrogen oxidation reactions on Pt(111) and Pt(100) in solutions containing chloride ions [J].

Stamenkovic, V ;

Markovic, NM ;

Ross, PN .

JOURNAL OF ELECTROANALYTICAL CHEMISTRY, 2001, 500 (1-2) :44-51

[37] RAMAN SPECTRUM OF GRAPHITE [J].

TUINSTRA, F ;

KOENIG, JL .

JOURNAL OF CHEMICAL PHYSICS, 1970, 53 (03) :1126-&

[38]

VIELSTICH W, 2003, HDB FUEL CELLS FUNDA, V1, pCH4

[39] Research on carbon nitrides [J].

Wang, EG .

PROGRESS IN MATERIALS SCIENCE, 1997, 41 (05) :241-298

[40] Micro-Raman spectroscopy investigation of C3N4 crystals deposited on nickel substrates [J].

Werninghaus, T ;

Zahn, DRT ;

Wang, EG ;

Chen, Y .

← 1 2 3 4 5 →