Hierarchical Magnetic Nanoparticle-Enzyme Assemblies for Substrate Inhibition

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Solution Overview

Problem

Peroxidases are highly sensitive to substrate inhibition, particularly by hydrogen peroxide, which limits their activity and use in various processes due to complex kinetics, restricting their application in bioprocesses.

Innovation Solution

The development of bionanocatalysts (BNCs) composed of horseradish peroxidase self-assembled with magnetic nanoparticles, which form mesoporous clusters that enhance enzymatic activity, reduce inhibition, and are incorporated into macroporous scaffolds for improved catalytic performance.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Productivity

If peroxidases are used as free enzymes, then they can catalyze oxidation reactions, but their activity is restricted by substrate inhibition and complex kinetics

Engineering Contradiction:
Improveenzymatic activityVSAvoidtolerance to substrate inhibition
Core Design Contradiction:
ProductivityVSReliability

Solution Approach 1:

The patent utilizes mesoporous silica structures with controlled pore sizes (2-50 nm) to immobilize peroxidase enzymes. The porous architecture provides high surface area for enzyme attachment while allowing substrate diffusion, creating a confined environment that modifies enzyme-substrate interactions and reduces substrate inhibition effects.

Inventive Principle:
Principle #31Porous materials

Solution Approach 2:

The invention creates composite materials combining peroxidase enzymes with magnetic nanoparticles and mesoporous silica supports. This composite structure integrates the catalytic function of the enzyme with the structural benefits of the nanoparticle-support system, enhancing both activity and stability under various process conditions.

Inventive Principle:
Principle #40Composite materials

2Ease of repair

If peroxidases are immobilized on surface-modified particles using complex biochemistries, then they can be reused, but enzymatic activities and reaction efficiencies are reduced

Engineering Contradiction:
Improveenzyme reuse capabilityVSAvoidenzymatic activity
Core Design Contradiction:
Ease of repairVSProductivity

Solution Approach 1:

The patent extracts the enzyme from complex biochemical conjugation processes and immobilizes it directly onto mesoporous silica surfaces through simpler adsorption or entrapment mechanisms. This eliminates the need for complex surface modification chemistry while preserving enzymatic activity and enabling easy recovery through magnetic separation.

Inventive Principle:
Principle #2Taking out (Extraction)

Solution Approach 2:

The mesoporous silica structure acts as an intermediary between the enzyme and the magnetic nanoparticles, providing a protective matrix that maintains enzyme activity while facilitating magnetic separation for reuse. This intermediary structure prevents direct contact between the enzyme and potentially deactivating surfaces.

Inventive Principle:
Principle #24Intermediary (Mediator)

3Productivity

If magnetic nanoparticles are used to enhance enzyme activity, then turnover rates increase, but the system complexity increases

Engineering Contradiction:
Improveturnover rateVSAvoidsystem structure
Core Design Contradiction:
ProductivityVSDevice complexity

Solution Approach 1:

The patent merges multiple functions into a single integrated system: magnetic nanoparticles provide both the magnetic separation capability and structural support for the mesoporous silica, while the silica support provides enzyme immobilization and catalytic activity. This consolidation reduces overall system complexity compared to separate components.

Inventive Principle:
Principle #5Merging (Combining)

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 BNCs exhibit significantly higher activity and resilience under various conditions, enabling their use in applications where free enzymes are not effective, with enhanced turnover rates and reduced substrate inhibition, allowing for efficient catalysis and easy reuse.

Implementation Method 1

bionanocatalysts (BNCs) consisting of an enzyme, particularly a free-radical-producing (FRP) enzyme, such as horseradish peroxidase (I IRP), self-assembled with magnetic nanoparticles (MNPs)

Methodology Applied
Scientific EffectSelf-assembly: Self-Assembly

Implementation Method 2

The liquid-phase chemical reaction containing magnetic particles therein is subjected to a plurality of magnetic fields of selected magnetic strength, relative position in the liquid-phase chemical reaction, and relative motion to spatially confine the magnetic particles

Methodology Applied
Scientific EffectMagnetic field: Magnetic Field

Implementation Method 3

Peroxidases (EC 1.11.1) are widely found in biological systems and form a subset of oxidoreductases that reduce hydrogen peroxide (H2O2) to water in order to oxidize a large variety of aromatic compounds

Methodology Applied
Scientific EffectEnzyme catalysis: Enzyme

Implementation Method 4

oxidize a large variety of aromatic compounds ranging from phenol to aromatic amines

Methodology Applied
Scientific EffectOxidation: Oxidation

Data Source

PatentUS12084649B2Hierarchical magnetic nanoparticle-enzyme mesoporous assemblies embedded in macroporous scaffolds
Publication Date: 2024.09.10 CORNELL UNIVERSITY
  • US12084649B2 patent drawing
  • US12084649B2 patent drawing
  • US12084649B2 patent drawing

AI summary

A hierarchical catalyst composition comprising a continuous or particulate macroporous scaffold in which is incorporated mesoporous aggregates of magnetic nanoparticles, wherein an enzyme is embedded in mesopores of the mesoporous aggregates of magnetic nanoparticles. Methods for synthesizing the hierarchical catalyst composition are also described. Also described are processes that use the recoverable hierarchical catalyst composition for depolymerizing lignin, remediation of water contaminated with aromatic substances, polymerizing monomers by a free-radical mechanism, epoxidation of alkenes, halogenation of phenols, inhibiting growth and function of microorganisms in a solution, and carbon dioxide conversion to methanol. Further described are methods for increasing the space time yield and/or total turnover number of a liquid-phase chemical reaction that includes magnetic particles to facilitate the chemical reaction, the method comprising subjecting the chemical reaction to a plurality of magnetic fields of selected magnetic strength, relative position in the chemical reaction, and relative motion.