Tunable Mesoporous BEA Zeolite Synthesis via Dual Organosilane Templates

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Solution Overview

Problem

Existing methods for producing mesoporous zeolites are limited by the need for specific organosilane templates to achieve desired pore width distributions, restricting the range of mesopore sizes that can be achieved and limiting catalytic activity.

Innovation Solution

A method involving a combination of two or more distinct organosilane mesopore templates, with varying ratios, to produce mesoporous zeolites with tunable pore widths, allowing for a continuous range of mesopore sizes and enhanced catalytic activity.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Ease of manufacture

If a single organosilane template is used to functionalize the growing seed crystal, then the zeolite structure is simplified and easier to manufacture, but the range of achievable pore width distributions is limited to specific values corresponding to each template

Engineering Contradiction:
Improvesimplicity of zeolite structureVSAvoidrange of pore width distributions
Core Design Contradiction:
Ease of manufactureVSAdaptability or versatility

Solution Approach 1:

The patent combines multiple distinct organosilane templates (specifically Template A and Template B) in the zeolite precursor solution to achieve a continuous range of pore width distributions. By merging the functions of different templates, the invention overcomes the limitation of single templates that can only produce discrete pore sizes, enabling tunable mesopore structures with center of pore width distribution ranging from 24 Å to 48 Å.

Inventive Principle:
Principle #5Merging (Combining)

Solution Approach 2:

The invention changes the parameter of template composition by using varying ratios of different organosilane templates. By adjusting the molar ratio of Template A to Template B (from 100:0 to 0:100 and intermediate ratios), the center of pore width distribution can be continuously tuned across a wide range, transforming the discrete pore size limitation into a continuous可调 parameter.

Inventive Principle:
Principle #35Parameter changes

2Adaptability or versatility

If multiple distinct organosilane templates are combined in varying ratios, then the range of achievable mesopore sizes expands to a continuous spectrum, but the complexity of the synthesis process increases

Engineering Contradiction:
Improverange of mesopore sizesVSAvoidcomplexity of synthesis process
Core Design Contradiction:
Adaptability or versatilityVSDevice complexity

Solution Approach 1:

The patent employs two distinct organosilane templates (Template A and Template B) that serve multiple functions: Template A produces mesopores with center of pore width distribution of 24 Å, Template B produces 48 Å mesopores, and their combinations continuously tune the pore size. This multi-functionality allows a single synthesis system to achieve a continuous range of pore sizes without requiring separate synthesis protocols for each pore size.

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

Solution Approach 2:

The invention simplifies the management of multiple templates by systematically varying their molar ratios as a controlled parameter. The synthesis process manages complexity by establishing clear relationships between template ratios and resulting pore sizes, making the tunable system predictable and controllable despite using multiple templates.

Inventive Principle:
Principle #35Parameter changes

3Adaptability or versatility

If a single organosilane template is used, then the catalytic activity is limited to specific hydrocarbon feeds or desired products, but the catalyst design and selection process is simpler

Engineering Contradiction:
Improvecatalytic activity for different hydrocarbonsVSAvoidcatalyst selection complexity
Core Design Contradiction:
Adaptability or versatilityVSDevice complexity

Solution Approach 1:

The patent establishes a direct relationship between template composition parameters and catalytic performance by enabling continuous tuning of pore width distribution. This allows catalysts to be optimized for different hydrocarbon cracking applications by adjusting the Template A:Template B ratio, creating a systematic approach to catalyst design that balances versatility with manageable complexity.

Inventive Principle:
Principle #35Parameter changes

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 approach enables the production of mesoporous zeolites with a center of pore width distribution that can be tailored to any value within a continuous spectrum, optimizing catalytic activity and expanding the range of achievable mesopore sizes without the need for multiple templates.

Implementation Method 1

mixing a silicon-containing material, an aluminum-containing material, and at least a quaternary amine to produce a zeolite precursor solution, wherein the quaternary amine comprises tetraethylammonium hydroxide

Methodology Applied
Scientific EffectIon exchange: Ion Exchange

Implementation Method 2

pre-crystallizing the zeolite precursor solution at a pre-crystallization temperature of greater than 125 °C and autogenous pressure to form a pre-crystallized zeolite precursor solution

Methodology Applied
Scientific EffectCrystallization: Crystallisation

Implementation Method 3

combining two or more distinct organosilane mesopore templates with the pre-crystallized zeolite precursor solution to produce a zeolite precursor gel

Methodology Applied
Scientific EffectSelf-assembly: Self-Assembly

Implementation Method 4

crystallizing the zeolite precursor gel to produce a crystalline zeolite intermediate

Methodology Applied
Scientific EffectCrystallization: Crystallisation

Implementation Method 5

calcining the crystalline zeolite intermediate to produce the mesoporous zeolite

Methodology Applied
Scientific EffectPyrolysis: Pyrolysis

Data Source

PatentEP3790844B1Methods for the synthesis of tunable mesoporous BEA zeolites
Publication Date: 2022.05.11 SAUDI ARABIAN OIL CO
  • EP3790844B1 patent drawingFigure 1~2B
  • EP3790844B1 patent drawingFigure 3~4
  • EP3790844B1 patent drawingFigure 5A~5C

AI summary

Methods of forming mesoporous zeolites with tunable pore widths are provided. In some embodiments, the method includes mixing a silicon-containing material, an aluminum-containing material, and at least a quaternary amine to produce a zeolite precursor solution. The zeolite precursor solution is pre-crystallized at a pre-crystallization temperature of greater than 125°C and autogenous pressure to form a pre-crystallized zeolite precursor solution and combined with two or more distinct organosilane mesopore templates to produce a zeolite precursor gel. The zeolite precursor gel is crystallized to produce a crystalline zeolite intermediate and the crystalline zeolite intermediate is calcined to produce the mesoporous zeolite.