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Metal-N4 doped carbon catalyst with high oxygen reduction performance and preparation method thereof

A carbon catalyst and metal technology, which is applied in the field of high-performance carbon catalysts and the preparation of metal-N4 active site growth induced by synergistic effect, can solve the problems of poor catalytic ORR ability, loss of active sites, restricting catalytic performance, etc. The effect of aggregation, ease of operation, and excellent catalytic activity for oxygen reduction reaction

Pending Publication Date: 2022-04-12
SHANGHAI UNIV
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  • Summary
  • Abstract
  • Description
  • Claims
  • Application Information

AI Technical Summary

Problems solved by technology

[0004] However, the preparation of Me-N by high-temperature pyrolysis x In the process of -C catalyst, there are two main problems restricting the improvement of its catalytic performance
On the one hand, metal atoms are usually transformed into various metal-based nanoparticles, such as metal elements, oxides, carbides, nitrides, etc., which have poor or completely useless ability to catalyze ORR.
On the other hand, Me-N 4 The active site will be lost in large quantities

Method used

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  • Metal-N4 doped carbon catalyst with high oxygen reduction performance and preparation method thereof
  • Metal-N4 doped carbon catalyst with high oxygen reduction performance and preparation method thereof
  • Metal-N4 doped carbon catalyst with high oxygen reduction performance and preparation method thereof

Examples

Experimental program
Comparison scheme
Effect test

Embodiment 1

[0035] In this example, a Fe-N x -C carbon catalyst.

[0036] In this example, iron phthalocyanine was used to prepare Fe-N x The method of -C carbon catalyst, comprises the steps:

[0037] 200 mg iron phthalocyanine (FePc, purchased from AlfaAesar), 200 mg phthalocyanine (Pc, purchased from aladdin) and 400 mg zinc chloride (ZnCl 2 , purchased from aladdin), ultrasonically dispersed into 20mL of absolute ethanol, ultrasonically mixed until uniform, and continued to heat ultrasonically to completely evaporate the liquid solvent, after drying, it was pyrolyzed at 950°C for 1h under the protection of high-purity argon to prepare iron-nitrogen doped heterogeneous carbon catalysts (Fe-N x -C).

[0038] Experimental test analysis:

[0039] 1) For the present embodiment Fe-N x The morphology of -C carbon catalyst was observed microscopically, and its morphology and structure were as follows figure 1 SEM shown. It can be seen from the topography that the carbon catalyst has a...

Embodiment 2

[0050] This embodiment is basically the same as Embodiment 1, and the special features are:

[0051] In this example, Fe-N was prepared by pyrolysis for 0.5 hours x -C carbon catalyst, comprising the steps of:

[0052] 200 mg iron phthalocyanine (FePc, purchased from AlfaAesar), 200 mg phthalocyanine (Pc, purchased from aladdin) and 400 mg zinc chloride (ZnCl 2 , purchased from aladdin), ultrasonically dispersed into 20mL of absolute ethanol, ultrasonically mixed until uniform, and continued to heat ultrasonically to completely evaporate the liquid solvent, after drying, it was pyrolyzed at 950°C for 0.5h under the protection of high-purity argon to prepare iron nitrogen Doped carbon catalysts (Fe-N x -C).

[0053] Experimental test analysis:

[0054] 1) Test the oxygen reduction activity of the carbon catalyst of this embodiment:

[0055] Fe-N x -C carbon catalyst loading is 600μg / cm 2 , 20wt% Pt / C catalyst loading is 75μg / cm 2 They were coated on the surface of glass...

Embodiment 3

[0059] This embodiment is basically the same as the previous embodiment, and the special features are:

[0060] In this example, Fe-N was prepared by pyrolysis for 1.5 hours x -C carbon catalyst, comprising the steps of:

[0061] 200 mg iron phthalocyanine (FePc, purchased from AlfaAesar), 200 mg phthalocyanine (Pc, purchased from aladdin) and 400 mg zinc chloride (ZnCl 2 , purchased from aladdin), ultrasonically dispersed into 20mL of absolute ethanol, ultrasonically mixed until uniform, and continued to heat ultrasonically to completely volatilize the liquid solvent, after drying, it was pyrolyzed at 950°C for 1.5h under the protection of high-purity argon to prepare iron nitrogen Doped carbon catalysts (Fe-N x -C).

[0062] Experimental test analysis:

[0063] 1) test the present embodiment Fe-N x Oxygen reduction activity of -C carbon catalysts:

[0064] Fe-N x -C carbon catalyst loading is 600μg / cm 2 , 20wt% Pt / C catalyst loading is 75μg / cm 2 They were coated on ...

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Abstract

The invention discloses a metal-N4-doped carbon catalyst with high oxygen reduction performance and a preparation method thereof, the metal-N4-doped carbon catalyst is a transition metal and nitrogen element-doped two-dimensional carbon nanosheet, the carbon catalyst has a porous lamellar nanostructure, all metal species in the carbon catalyst are an Me-N4 structure composed of atomic transition metal and N4, and Me-N4 is an active site. Wherein Me is at least one metal of Fe, Co, Ni, Cu, Zn and Mn. The method comprises the following steps: adding three compound precursors of metal phthalocyanine, phthalocyanine and zinc salt into a liquid solvent according to a set mass ratio, uniformly mixing, continuously heating until the liquid solvent is completely volatilized, and preparing the metal-N4 doped non-noble metal carbon catalyst by adopting a one-step high-temperature pyrolysis method. The catalyst disclosed by the invention has high oxygen reduction reaction (ORR) catalytic activity, excellent CH3OH / CO tolerance and good stability; the preparation process is simple and easy to control, the used raw materials are commercially available products, and batch production can be realized.

Description

technical field [0001] The invention belongs to the technical field of new energy, and relates to a high-performance carbon catalyst for oxygen reduction reaction and synergistic effect induced metal-N 4 Preparation method for active site growth. Background technique [0002] With the rapid consumption of fossil fuels and increasing environmental concerns, electrochemical energy storage and conversion technologies have emerged as promising avenues for the development of clean energy devices. Electrochemical oxygen reduction reaction (ORR) in metal-air batteries and H 2 -O 2 It plays a vital role in next-generation energy storage and conversion systems such as fuel cells. So far, platinum-based catalysts remain the benchmark electrocatalysts for ORR. Unfortunately, platinum's high cost, scarcity, and poor durability severely hinder its widespread application in practical energy systems. Therefore, it is crucial to design highly efficient, durable, and low-cost non-noble ...

Claims

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Application Information

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Patent Type & Authority Applications(China)
IPC IPC(8): H01M4/96B82Y40/00B82Y30/00
CPCY02E60/50
Inventor 张世明陈梦慧容忠言张久俊
Owner SHANGHAI UNIV
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