Metal alloy-carbon nanotube network macroscopic body composite material, preparation method and application thereof

A technology of carbon nanotubes and metal alloys, which is applied in the field of energy and cleanliness, can solve the problems of inability to ensure high utilization of nanocatalysts and high combination of carbon supports, reduced catalytic performance and anti-poisoning performance, and easy agglomeration and migration. Achieve excellent anti-methanol poisoning performance, strong binding force and low cost

Active Publication Date: 2020-10-16
SUZHOU INST OF NANO TECH & NANO BIONICS CHINESE ACEDEMY OF SCI
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Problems solved by technology

In addition, there are also many research efforts devoted to the development of other binary or multi-component metal alloy nanocatalysts, such as Pb-Fe (Nano Energy 2018,50,70.Atomic rearrangement from disordered toordered Pd-Fe nanocatalysts with trace amount of Pt decoration for efficient electrocatalysis ), Pt-Fe-Cu (Chemistry of Materials, 2018, 30, 5987. Copper-Induced Formation of Structurally Ordered Pt–Fe–Cu Ternary Intermetallic Electrocatalysts with Tunable Phase Structure and Improved Stability), IrM (M=Fe / Co / Ni / Cu) (Nano Energy 2016,29,261-267.Tuning electrocatalytic activity ofPt monolayer shell by bimetallic Ir-M(M=Fe,Co,Ni or Cu)cores for the oxygenreduction reaction.) However, the alloy catalysts currently studied are basically zero One-dimensional nanoparticles or one-dimensional nanowires, when used in fuel cells or metal-air batteries, usually need to be supported on carbon supports with high specific surface area. The high surface energy of metal alloys at the nanoscale is prone to agglomeration and migration, thereby reducing the Catalytic performance and anti-poisoning performance
Moreover, the preparation process of the currently developed alloy catalysts is complex and time-consuming. In addition, when applied to practical devices, the catalysts are mostly powder materials that need to be dispersed on carbon supports and further loaded in porous electrodes to make oxygen electrodes, which cannot ensure High utilization of nanocatalysts and high binding of carbon supports

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[0031] One aspect of the embodiments of the present invention provides a method for preparing a metal alloy-carbon nanotube network macroscopic body composite material, which includes:

[0032] (1) providing a carbon nanotube network macroscopic body, the carbon nanotube network macroscopic body contains iron as a trace impurity;

[0033] (2) Activating the carbon nanotube network macroscopic body;

[0034] (3) Contacting the activated carbon nanotube network macroscopic body with the metal precursor solution, causing the iron element to undergo a displacement reaction with the metal precursor to generate an elemental metal combined with the elemental iron, the elemental metal It has oxygen reduction catalytic activity, followed by drying treatment;

[0035] (4) Transient electric heating is performed on the carbon nanotube network macroscopic body treated in step (3) to obtain a metal alloy-carbon nanotube network macroscopic body composite material.

[0036] In some typical ...

Embodiment 1

[0080] The preparation process of a metal alloy-carbon nanotube network macroscopic body composite material provided by this embodiment is as follows: figure 1 As shown, it includes the following steps:

[0081] Step 1. Provide the carbon nanotube network macrobody prepared by floating chemical vapor deposition method, its preparation process is: the FCCVD tubular furnace device is heated to 1300 ℃, injects with syringe pump containing 2wt.% ferrocene and 0.4wt.% Thiophene solution in absolute ethanol at an injection rate of 20 mL h -1 , the carrier gas is Ar / H 2 Mixed gas, Ar flow rate 2200sccm, H 2 The flow rate is 2000sccm, the original CNT airgel is collected by the roller after floating out from the tail, sprayed with ethanol and infiltrated, and further compressed by the roller shaft to obtain a carbon nanotube network macroscopic body containing 5% iron impurity, and then electrochemically Activation treatment, including: using the carbon nanotube network macroscopic...

Embodiment 2

[0087] Step 1. Provide the carbon nanotube network macrobody prepared by floating chemical vapor deposition method, its preparation process is: the FCCVD tubular furnace device is heated to 1300 ℃, injects with syringe pump containing 2wt.% ferrocene and 0.4wt.% Thiophene solution in absolute ethanol at an injection rate of 20 mL h -1 , the carrier gas is Ar / H 2 Mixed gas, Ar flow rate 2200sccm, H 2 The flow rate is 2000 sccm, the original CNT airgel is collected by the roller after floating out from the tail, sprayed with ethanol and infiltrated, and further compressed with a roller to obtain a carbon nanotube network macroscopic body containing 1wt.% iron impurity, and then electrochemically activate it The treatment includes: using the carbon nanotube network macroscopic body as an anode, using a platinum sheet of the same area as a counter electrode, using a solution of 0.2g sodium hydroxide dissolved in 1mL water and 20mL ethanol as an electrolyte, and using a direct cur...

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Abstract

The invention discloses a metal alloy-carbon nanotube network macroscopic body composite material, a preparation method and application thereof. The preparation method comprises the following steps providing a carbon nanotube network macroscopic body, wherein the carbon nanotube network macroscopic body contains elemental iron serving as a trace impurity; carrying out activation treatment on the carbon nanotube network macroscopic body; making the activated carbon nanotube network macroscopic body contact a metal precursor solution to enable the elemental iron and the metal precursor to be subjected to a replacement reaction to generate an elemental metal combined with the elemental iron, wherein the elemental metal has oxygen reduction catalytic activity, and then drying treatment is conducted; and finally carrying out transient electric heating to obtain the composite material. According to the invention, the preparation method is low in cost, simple and easy to implement and short in consumed time, the binding force between the carbon nanotube network macroscopic body and the metal alloy nanoparticles in the obtained composite material is high, the catalytic performance is excellent, the stability is high, the methanol poisoning resistance is excellent, and the carbon nanotube network macroscopic body can be directly used as an oxygen electrode for a metal-air battery.

Description

technical field [0001] The invention relates to an oxygen-functional electrocatalytic electrode, in particular to a metal alloy-carbon nanotube network macroscopic body composite material and a preparation method thereof, as well as the application of the composite material in preparing an oxygen electrode, belonging to the field of energy and clean technology. Background technique [0002] Metal-air batteries have attracted extensive attention from researchers due to their high specific energy density, reproducibility, and safety. One of the challenges in the development of metal-air batteries is to explore high-performance oxygen-functional catalysts. The current commercialized 20wt% platinum carbon oxygen reduction catalyst is a carbon material with a high specific surface area supported by platinum nanoparticles. Due to the weak interaction between platinum nanoparticles and carbon and the problem of oxidative corrosion of carbon supports, it cannot be used for a long tim...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): H01M4/90H01M12/06
CPCH01M4/9041H01M4/9083H01M12/06
Inventor 邸江涛曾沙吕波朱铖锋李清文
Owner SUZHOU INST OF NANO TECH & NANO BIONICS CHINESE ACEDEMY OF SCI
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