Process for producing fuel cell electrode catalyst, process for producing transition metal oxycarbonitride, fuel cell electrode catalyst and uses thereof

Abstract

Provided is a process for producing a fuel cell electrode catalyst having high catalytic activity which uses a transition metal, e.g., titanium, which process comprises thermal treatment at relatively low temperature, i.e., not including thermal treatment at high temperature (calcining) step. The process for producing a fuel cell electrode catalyst comprises a step (1) of mixing at least a transition metal-containing compound, a nitrogen-containing organic compound and a solvent to provide a catalyst precursor solution; a step (2) of removing the solvent from the catalyst precursor solution; and a step (3) of thermally treating a solid residue obtained in the step (2) at a temperature of 500 to 1100° C. to provide an electrode catalyst; wherein the transition metal-containing compound is partly or wholly a compound comprising at least one transition metal element (M1) selected from the group 4 and 5 elements of the periodic table as a transition metal element.

Description

CROSS REFERENCE TO RELATED APPLICATIONS[0001]This application is a National Stage of International Application No. PCT / JP2011 / 052689 filed Feb. 9, 2011, claiming priority based on Japanese Patent Application Nos. 2010-028025 filed Feb. 10, 2010, JP 2010-251890 filed Nov. 10, 2010 and JP 2011-006192 filed Jan. 14, 2011, the contents of all of which are incorporated herein by reference in their entirety.TECHNICAL FIELD[0002]The present invention relates to a process for producing a fuel cell electrode catalyst; a process for producing a transition metal oxycarbonitride; and a fuel cell electrode catalyst; and uses thereof.BACKGROUND ART[0003]A polymer electrolyte fuel cell has a solid polymer electrolyte sandwiched between an anode and a cathode. A fuel is fed to the anode, and oxygen or air is fed to the cathode, whereby oxygen is reduced at the cathode to produce electricity. The fuel is primarily hydrogen, methanol or the like.[0004]To increase the reaction rate in the fuel cell an...

AI Technical Summary

Benefits of technology

[0064]According to the process for producing a fuel cell electrode catalyst of the present invention, a fuel cell electrode catalyst having high catalytic activity which uses a transition metal, e.g., titanium, can be produced through thermal treatment at relatively low temperature, i.e., without performing thermal treatment at high temperature (calcining) step.

[0065]According to the process for producing a transition metal oxycarbonitride of the present invention, a transition metal oxycarbonitride can be produced at lower temperature as compared with conventional techniques, and thus production cost can be reduced and production process safety can be increased.

Problems solved by technology

However, since these noble metals are expensive and limited in resource amount, alternative catalysts have been desired.

Further, the noble metals used on the cathode surface are sometimes dissolved in an acidic atmosphere and are not suited in applications requiring long-term durability.

However, catalysts containing base metal materials described in Patent Literature 1 and Patent Literature 2 have a problem in terms of their failure to provide oxygen reducing activity that is sufficient on a practical basis.

Catalysts described in Patent Literature 3 and Patent Literature 4, although showing high oxygen reducing catalytic activity, have a problem in terms of their extremely low stability under fuel cell operation conditions.

Performing such high-temperature heating treatment is not impossible on an industrial basis, but involves difficulty and invites increase in equipment cost and difficulty in operation control, leading to the increase in the production cost.

However, according to the production process described in Patent Literature 7, the production of the carbon-containing titanium oxynitride requires two-stage synthesis: the preparation of a titanium oxynitride by reacting a nitrogen-containing organic compound with a titanium precursor, and the preparation of a carbon-containing titanium oxynitride by reacting a phenol resin with the titanium oxynitride precursor, and thus involves complicated steps.

In particular, the preparation of the titanium oxynitride precursor requires complicated steps including stirring, heating and refluxing at 80° C. as well as cooling and concentrating under reduced pressure, thus resulting in high cost.

In addition, since the phenol resin is a thermosetting resin having a three-dimensional network structure, it is difficult to homogenously mix and react the phenol resin with a metal oxide.

The production process, however, cannot provide an electrode catalyst having sufficient catalytic performance.

This catalyst, however, has problems in terms of highly toxicity of the raw material, high cost and insufficient catalytic activity.

The production process, however, does not use a nitrogen-containing organic substance and thus cannot provide an electrode catalyst having sufficient catalytic performance.