Preparation of Single-atom Palladium Catalyst and Its Application in Direct Formic Acid Fuel Cell

Abstract

The invention relates to a fuel cell technology, and aims to provide preparation of a monatomic palladium catalyst and application of the monatomic palladium catalyst in a direct formic acid fuel cell. The preparation method comprises the following steps of: preparing an o-phenylenediamine cyclodextrin inclusion compound from o-phenylenediamine and [beta]-cyclodextrin, adding the o-phenylenediamine cyclodextrin inclusion compound into a chloropalladic acid solution, and performing stirring to obtain a palladium coordinated o-phenylenediamine cyclodextrin inclusion compound solution; adding sodium chloride, carrying out liquid nitrogen flash freezing, and performing drying to obtain a precursor; carbonizing the precursor under the protection of nitrogen atmosphere, performing cooling, washing and drying to obtain the monatomic palladium catalyst. The technical route is simple, universality is achieved, and generation of impure phases can be avoided. The monatomic palladium catalyst hashigher electrocatalytic activity, and the cost can be effectively reduced. The co-catalytic application of the monatomic palladium catalyst and the cocatalyst (VO)SO4 provides a new thought for the design and performance improvement of the direct formic acid fuel cell, and is beneficial to the commercial development of the fuel cell.

Description

technical field

[0001] The present invention relates to a kind of fuel cell technology, more specifically, relate to a kind of homogeneous / heterogeneous co-catalyzed direct formic acid fuel cell and its monoatomic palladium catalyst as heterogeneous catalyst, vanadium oxide sulfate as homogeneous catalyst Process for the preparation of atomic palladium catalysts. Background technique

[0002] Direct formic acid fuel cell uses formic acid liquid as fuel, and its electromotive force is 1.48V, which is higher than that of hydrogen-oxygen fuel cell, and it is easy to store and transport fuel, and has high energy density. It is a very potential liquid fuel cell. However, the electrochemical oxidation reaction activity of the formic acid anode is low and the catalyst is easily poisoned, resulting in low performance of the battery. Similar to the electrochemical oxidation of methanol, the electrochemical oxidation of formic acid (HCOOH) over palladium catalysts consists of multipl...

Examples

Embodiment 1

[0065] Embodiment one: o-phenylenediamine solution preparation

[0066] At 90° C., 5 g of o-phenylenediamine was dissolved in 95 mL of deionized water, and dispersed by ultrasonic vibration (ultrasonic frequency 40 kHz) for 5 minutes to obtain a solution of o-phenylenediamine with a concentration of 5 wt%.

Embodiment 2

[0067] Example 2: Preparation of β-cyclodextrin inclusion compound of o-phenylenediamine

[0068] At 90°C, dissolve 7g of o-phenylenediamine in 93mL of deionized water, and disperse for 5 minutes with ultrasonic vibration (ultrasonic frequency 40kHz) to obtain a solution of o-phenylenediamine with a concentration of 7wt%. Take 100mL of deionized water and dissolve 10g of β- Add o-phenylenediamine solution after the cyclodextrin, and disperse for 30 minutes with ultrasonic vibration (ultrasonic frequency 40kHz), the o-phenylenediamine enters the cyclodextrin cavity to form a cyclodextrin inclusion complex of o-phenylenediamine, and after vacuum drying, the obtained o-Phenylenediamine Cyclodextrin Inclusion Compound.

Embodiment 3

[0069] Example 3: Palladium-Coordinated Ortho-Phenylenediamine Cyclodextrin Inclusion Compound Solution

[0070] At 90°C, dissolve 10 g of o-phenylenediamine in 90 mL of deionized water, and disperse for 5 minutes with ultrasonic vibration (ultrasonic frequency 40 kHz) to obtain a solution of o-phenylenediamine with a concentration of 10 wt %. Take 100 mL of deionized water and dissolve 25 g of β- Add o-phenylenediamine solution after the cyclodextrin, and disperse for 30 minutes with ultrasonic vibration (ultrasonic frequency 40kHz), the o-phenylenediamine enters the cyclodextrin cavity to form a cyclodextrin inclusion complex of o-phenylenediamine, and after vacuum drying, the obtained o-Phenylenediamine Cyclodextrin Inclusion Compound.

[0071] Dissolve 0.01 g of chloropalladium acid in 200 mL of deionized water to obtain a chloropalladium acid solution, take 10 g of the above-mentioned o-phenylenediamine cyclodextrin inclusion compound, add it to the chloropalladium acid s...

technical field

[0001] The present invention relates to a kind of fuel cell technology, more specifically, relate to a kind of homogeneous / heterogeneous co-catalyzed direct formic acid fuel cell and its monoatomic palladium catalyst as heterogeneous catalyst, vanadium oxide sulfate as homogeneous catalyst Process for the preparation of atomic palladium catalysts. Background technique

[0002] Direct formic acid fuel cell uses formic acid liquid as fuel, and its electromotive force is 1.48V, which is higher than that of hydrogen-oxygen fuel cell, and it is easy to store and transport fuel, and has high energy density. It is a very potential liquid fuel cell. However, the electrochemical oxidation reaction activity of the formic acid anode is low and the catalyst is easily poisoned, resulting in low performance of the battery. Similar to the electrochemical oxidation of methanol, the electrochemical oxidation of formic acid (HCOOH) over palladium catalysts consists of multipl...

Examples

Embodiment 1

[0065] Embodiment one: o-phenylenediamine solution preparation

[0066] At 90° C., 5 g of o-phenylenediamine was dissolved in 95 mL of deionized water, and dispersed by ultrasonic vibration (ultrasonic frequency 40 kHz) for 5 minutes to obtain a solution of o-phenylenediamine with a concentration of 5 wt%.

Embodiment 2

[0067] Example 2: Preparation of β-cyclodextrin inclusion compound of o-phenylenediamine

[0068] At 90°C, dissolve 7g of o-phenylenediamine in 93mL of deionized water, and disperse for 5 minutes with ultrasonic vibration (ultrasonic frequency 40kHz) to obtain a solution of o-phenylenediamine with a concentration of 7wt%. Take 100mL of deionized water and dissolve 10g of β- Add o-phenylenediamine solution after the cyclodextrin, and disperse for 30 minutes with ultrasonic vibration (ultrasonic frequency 40kHz), the o-phenylenediamine enters the cyclodextrin cavity to form a cyclodextrin inclusion complex of o-phenylenediamine, and after vacuum drying, the obtained o-Phenylenediamine Cyclodextrin Inclusion Compound.

Embodiment 3

[0069] Example 3: Palladium-Coordinated Ortho-Phenylenediamine Cyclodextrin Inclusion Compound Solution

[0070] At 90°C, dissolve 10 g of o-phenylenediamine in 90 mL of deionized water, and disperse for 5 minutes with ultrasonic vibration (ultrasonic frequency 40 kHz) to obtain a solution of o-phenylenediamine with a concentration of 10 wt %. Take 100 mL of deionized water and dissolve 25 g of β- Add o-phenylenediamine solution after the cyclodextrin, and disperse for 30 minutes with ultrasonic vibration (ultrasonic frequency 40kHz), the o-phenylenediamine enters the cyclodextrin cavity to form a cyclodextrin inclusion complex of o-phenylenediamine, and after vacuum drying, the obtained o-Phenylenediamine Cyclodextrin Inclusion Compound.

[0071] Dissolve 0.01 g of chloropalladium acid in 200 mL of deionized water to obtain a chloropalladium acid solution, take 10 g of the above-mentioned o-phenylenediamine cyclodextrin inclusion compound, add it to the chloropalladium acid s...

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