Nitrogenous Carbon Catalyst Synthesis via Sol-Gel Pyrolysis

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Solution Overview

Problem

Current methods for synthesizing porous carbonaceous materials with metal dopants for oxygen reduction in proton exchange membrane fuel cells are complex and costly, requiring multiple steps and the use of sacrificial pore-forming materials.

Innovation Solution

A process involving sol-gel polymerization in a solvent medium with aldehydes, hydroxybenzene derivatives, and metal precursors, followed by pyrolysis in a non-oxidizing atmosphere, to produce nitrogenous carbonaceous materials with metal dopants integrated throughout the structure, eliminating the need for separate doping steps and sacrificial materials.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Reliability

If conventional multi-step methods are used to synthesize porous carbonaceous materials with metal dopants, then the material can be obtained with desired properties, but the synthesis process becomes complex and costly

Engineering Contradiction:
Improvematerial qualityVSAvoidsynthesis process complexity
Core Design Contradiction:
ReliabilityVSDevice complexity

Solution Approach 1:

The invention merges multiple synthesis steps into a single sol-gel process. Metal precursors, nitrogen sources, and carbon precursors are combined in one reaction mixture that undergoes sol-gel polymerization followed by pyrolysis, simultaneously forming the porous carbon structure and incorporating metal dopants without requiring separate doping steps or sacrificial pore-forming materials

Inventive Principle:
Principle #5Merging (Combining)

Solution Approach 2:

The sol-gel process serves multiple functions simultaneously: it forms the porous carbonaceous matrix, incorporates metal dopants through precursor decomposition, introduces nitrogen atoms from the hydrocarbon compound, and creates the desired pore structure without requiring additional materials or steps for each function

Inventive Principle:
Principle #6Universality (Multi-functionality)

2Reliability

If conventional methods with separate doping steps are used, then metal dopants can be incorporated, but the manufacturing cost and process time increase

Engineering Contradiction:
Improvemetal dopant incorporationVSAvoidsynthesis efficiency
Core Design Contradiction:
ReliabilityVSProductivity

Solution Approach 1:

Metal precursors are incorporated into the sol-gel reaction mixture before polymerization occurs. The precursors are uniformly distributed throughout the forming gel matrix, ensuring complete incorporation into the final carbonaceous material without requiring subsequent doping steps

Inventive Principle:
Principle #10Preliminary action

Solution Approach 2:

The metal doping step is merged with the carbonization step. Both processes occur simultaneously during pyrolysis of the hydrogel, eliminating the need for separate doping operations and reducing overall process time and cost

Inventive Principle:
Principle #5Merging (Combining)

3Stability of the object's composition

If sacrificial pore-forming materials are used to create porous structure, then desired porosity can be achieved, but the process becomes more complex and costly

Engineering Contradiction:
ImproveporosityVSAvoidprocess complexity
Core Design Contradiction:
Stability of the object's compositionVSDevice complexity

Solution Approach 1:

The sol-gel process itself generates the porous structure through its inherent polymerization and drying mechanisms. The formation of the gel network and subsequent removal of volatile components creates porosity without requiring external pore-forming agents or sacrificial materials

Inventive Principle:
Principle #25Self-service

Solution Approach 2:

The invention directly produces a porous carbonaceous material through controlled sol-gel polymerization and pyrolysis. The pore structure is formed intrinsically during the gelation and drying processes, eliminating the need for separate pore-forming material incorporation and removal steps

Inventive Principle:
Principle #31Porous materials

Applied Scientific Principles

This section explains which scientific principles are used to turn an abstract innovation direction into a practical engineering solution.

Function Achieved in This Case

This method simplifies the synthesis, reduces costs, and enhances electrochemical performance by distributing catalytic sites throughout the material, increasing efficiency in oxygen reduction reactions.

Implementation Method 1

activating a sol polymerization -gel at the level of said solvent medium of step (a) to form a nitrogenous carbon hydrogel

Methodology Applied
Scientific EffectSol-gel polymerization: Photopolymerisation

Implementation Method 2

pyrolyzing said dry form of hydrogel in a non-oxidizing atmosphere, to form said porous, nitrogenous and charged carbonaceous material

Methodology Applied
Scientific EffectPyrolysis: Pyrolysis

Data Source

PatentEP3780197A1Method for preparing a porous carbonaceous and nitrogenous material with metallic dopant, in particular useful as a catalyst for oxygen reduction reaction (ORR)
Publication Date: 2021.02.17 COMMISSARIAT A LENERGIE ATOMIQUE ET AUX ENERGIES ALTERNATIVES
  • EP3780197A1 patent drawingFigure 1
  • EP3780197A1 patent drawingFigure 2
  • EP3780197A1 patent drawing

AI summary

The present invention relates to a process for preparing a nitrogen-containing porous carbon material filled throughout with at least one metallic dopant, comprising at least the steps of (a) having a solvent medium containing, in solution, at least one aldehyde, one hydroxybenzene derivative, and one nitrogen-source hydrocarbon compound, and furthermore at least one precursor of said metallic dopant, (b) activating a sol-gel polymerization in said solvent medium from step (a) to form a nitrogen-containing carbon hydrogel containing at least one metallic precursor throughout, (c) having a dry form of said nitrogen-containing carbon hydrogel formed in step (b), and (d) pyrolyzing said dry form in an inert atmosphere to form and recover a nitrogen-containing porous carbon material filled at least throughout with at least one metallic dopant.