CeO2-Supported Single Atom Catalysts for Direct Methane Conversion

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Solution Overview

Problem

Conventional methods for methane conversion to olefins and aromatics face challenges such as low carbon efficiency, high capital costs, and carbon coking due to the presence of metal ensembles in catalysts, limiting their stability and selectivity.

Innovation Solution

The synthesis of single atom noble metal catalysts supported on CeO2, specifically Pt, Pd, Rh, Ru, Ag, Au, and Ir, which are characterized by atomic dispersion and absence of clusters, allowing for efficient non-oxidative methane conversion to light olefins and aromatics with reduced coke selectivity.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Reliability

If conventional catalysts with metal ensembles are used for methane conversion, then catalytic activity is achieved, but carbon coking occurs and stability is limited

Engineering Contradiction:
Improvecatalyst stabilityVSAvoidcarbon coking
Core Design Contradiction:
ReliabilityVSObject-generated harmful factors

Solution Approach 1:

The catalyst structure is segmented to the atomic level, with individual noble metal atoms dispersed on CeO2 support. This atomic-level segmentation eliminates metal ensembles and prevents carbon coking while maintaining catalytic activity for methane conversion to olefins and aromatics

Inventive Principle:
Principle #1Segmentation

Solution Approach 2:

The invention creates localized atomic dispersion of noble metal atoms on specific CeO2 support sites. This local quality control ensures that catalytic sites are isolated at the atomic level, preventing carbon deposition while maintaining high activity for C-C coupling reactions

Inventive Principle:
Principle #3Local quality

2Manufacturing precision

If single atom catalysts are synthesized, then atomic dispersion and absence of clusters are achieved, but synthesis complexity increases

Engineering Contradiction:
Improveatomic dispersionVSAvoidsynthesis complexity
Core Design Contradiction:
Manufacturing precisionVSDevice complexity

Solution Approach 1:

CeO2 nanoparticles serve as an intermediary support that facilitates the formation and stabilization of single atom noble metal catalysts. The CeO2 support provides specific sites for atomic dispersion and prevents cluster formation during synthesis and reaction, simplifying the overall synthesis process while achieving atomic-level precision

Inventive Principle:
Principle #24Intermediary (Mediator)

Solution Approach 2:

The invention employs controlled synthesis parameters including temperature, atmosphere, and precursor ratios to achieve atomic dispersion. By optimizing these parameters, the synthesis process achieves precise atomic-level control without requiring excessively complex procedures

Inventive Principle:
Principle #35Parameter changes

3Productivity

If conventional multistage syngas processes are used, then methane conversion is achieved, but carbon efficiency is low and capital cost is high

Engineering Contradiction:
Improvemethane conversion efficiencyVSAvoidcarbon efficiency
Core Design Contradiction:
ProductivityVSLoss of energy

Solution Approach 1:

The invention extracts and eliminates the intermediate syngas step from the conventional methane conversion process. By using single atom catalysts, the process directly converts methane to olefins and aromatics in one step, improving carbon efficiency and reducing energy losses associated with multiple conversion stages

Inventive Principle:
Principle #2Taking out (Extraction)

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

The CeO2-supported single atom catalysts demonstrate superior catalytic performance and stability, achieving high methane conversion and selectivity towards C2 productivity with minimal coke formation, making them suitable for practical applications.

Implementation Method 1

Single atom catalysts (SACs) represent a new frontier of heterogeneous catalysis and have been demonstrated to exhibit enhanced catalytic activity and selectivity in many reactions, including CO oxidation, water-gas shift, methane steam reforming, selective hydrogenation of alkynes and dienes and so on

Methodology Applied
Scientific EffectCatalysis: Catalysis

Implementation Method 2

The superior catalytic performance can be attributed to the atomic dispersion of metal atoms with low coordination number, quantum confinement and/or strong metal-support (mostly metal oxides) interactions

Methodology Applied
Scientific EffectStrong metal-support interactions: Adsorption

Implementation Method 3

The superior catalytic performance can be attributed to the atomic dispersion of metal atoms with low coordination number, quantum confinement and/or strong metal-support (mostly metal oxides) interactions

Methodology Applied
Scientific EffectQuantum confinement:

Data Source

PatentUS11518722B2Method for preparation of nanoceria supported atomic noble metal catalysts and the application of platinum single atom catalysts for direct methane conversion
Publication Date: 2022.12.06 JOHNS HOPKINS UNIVERSITY
  • US11518722B2 patent drawing
  • US11518722B2 patent drawing
  • US11518722B2 patent drawing

AI summary

Described are methods for converting methane to olefins, aromatics, or a combination thereof using a single atom catalyst comprising CeO2 nanoparticles impregnated with individual atoms of noble metals including Pt, Pd, Rh, Ru, Ag, Au, Ir, or a combination thereof. These single atom catalysts of the present invention are heated with methane to form olefins and aromatics.