Chiral Iridium Asymmetric Hydrogenation for Tocopherol Synthesis

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Solution Overview

Problem

There is a strong need for an effective and industrial-scale synthesis of (2R,4'R,8'R)-tocopherols and (R,R)-isophytol, as natural sources are limited, and higher bioactivity is associated with the R-configuration at specific chiral centers in these molecules.

Innovation Solution

A process involving the asymmetric hydrogenation of (6R,10R)-6,10,14-trimethylpentadecan-2-one is developed, which includes the separation and cis/trans isomerization of isomers from a mixture of 6,10,14-trimethylpentadeca-5,9,13-trien-2-one or 6,10,14-trimethylpentadeca-5,9-dien-2-one, using a chiral iridium complex and specific additives to achieve high-quality production.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Productivity

If asymmetric hydrogenation is performed on a mixture of stereoisomers, then the production efficiency is improved, but the manufacturing precision of the desired chiral product deteriorates

Engineering Contradiction:
Improveproduction efficiencyVSAvoidchiral product purity
Core Design Contradiction:
ProductivityVSManufacturing precision

Solution Approach 1:

The patent applies preliminary action by performing cis/trans isomerization before asymmetric hydrogenation. The mixture of stereoisomers is first isomerized to enrich the desired (E,E) and (Z,Z) isomers, which are then selectively hydrogenated. This preliminary isomerization step ensures that when hydrogenation occurs, the dominant substrates are the ones that will produce the desired (6R,10R) product, thus maintaining high chiral purity while processing the entire mixture efficiently

Inventive Principle:
Principle #10Preliminary action

Solution Approach 2:

The patent utilizes parameter changes by employing specific reaction conditions including catalyst selection (chiral catalysts with specific configurations), temperature control, and pressure parameters during asymmetric hydrogenation. By optimizing these parameters, the process achieves high enantioselectivity (er > 98:2) while maintaining high conversion rates, thus resolving the contradiction between productivity and manufacturing precision

Inventive Principle:
Principle #35Parameter changes

2Manufacturing precision

If separation of individual isomers is performed before asymmetric hydrogenation, then the manufacturing precision is improved, but the productivity deteriorates

Engineering Contradiction:
Improvestarting material purityVSAvoidproduction efficiency
Core Design Contradiction:
Manufacturing precisionVSProductivity

Solution Approach 1:

The patent applies the taking out principle by selectively removing or focusing on the valuable (E,E) and (Z,Z) isomers through isomerization, while the unwanted isomers are converted into the desired configuration. Rather than separating and discarding unwanted isomers, the process extracts and utilizes the valuable stereoisomers after isomerization, converting the entire mixture into useful material for the asymmetric hydrogenation step

Inventive Principle:
Principle #2Taking out (Extraction)

Solution Approach 2:

The patent merges multiple operations into an integrated process flow where isomerization and asymmetric hydrogenation are combined in sequence. Instead of separate purification steps followed by reaction, the process combines isomerization (which enriches desired isomers) with subsequent hydrogenation, allowing the entire mixture to be processed efficiently while achieving high product purity

Inventive Principle:
Principle #5Merging (Combining)

3Loss of substance

If cis/trans isomerization is used to utilize non-desired isomers, then the loss of substance is reduced, but the device complexity increases

Engineering Contradiction:
Improvestarting material wasteVSAvoidprocess complexity
Core Design Contradiction:
Loss of substanceVSDevice complexity

Solution Approach 1:

The patent applies the blessing in disguise principle by converting the unwanted stereoisomers (which would normally be waste or require costly separation) into valuable substrates through cis/trans isomerization. The non-desired isomers are transformed into the desired (E,E) and (Z,Z) configurations, which then participate efficiently in asymmetric hydrogenation. This converts what would be harmful waste into beneficial material, achieving near 100% utilization of all starting material

Inventive Principle:
Principle #22Blessing in disguise (Convert harm into benefit)

Solution Approach 2:

The patent uses cis/trans isomerization as an intermediary step that mediates between the mixed stereoisomer starting material and the asymmetric hydrogenation reaction. This intermediary process enriches the desired isomers and prepares the mixture for efficient hydrogenation, acting as a bridge that enables complete utilization of all starting materials while maintaining high product purity

Inventive Principle:
Principle #24Intermediary (Mediator)

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 process efficiently produces the desired chiral product from stereoisomers, enabling industrial-scale production of (2R,4'R,8'R)-tocopherols and (R,R)-isophytol with improved bioactivity, utilizing the R-configuration at key chiral centers.

Implementation Method 1

asymmetric hydrogenation of either 6,10,14-trimethylpentadeca-5,9,13-trien-2-one or 6,10,14-trimethylpentadeca-5,9-dien-2-one or a ketal of 6,10,14-trimethylpentadeca-5,9,13-trien-2-one or 6,10,14-trimethylpentadeca-5,9-dien-2-one using molecular hydrogen in the presence of a chiral iridium complex

Methodology Applied
Scientific EffectAsymmetric hydrogenation: Hydrogenation

Implementation Method 2

asymmetric hydrogenation of either 6,10,14-trimethylpentadeca-5,9,13-trien-2-one or 6,10,14-trimethylpentadeca-5,9-dien-2-one or a ketal of 6,10,14-trimethylpentadeca-5,9,13-trien-2-one or 6,10,14-trimethylpentadeca-5,9-dien-2-one using molecular hydrogen in the presence of a chiral iridium complex

Methodology Applied
Scientific EffectCatalysis: Catalysis

Implementation Method 3

separating individually the (5E,9E)- and/or the (5Z,9Z)-isomer of 6,10,14-trimethylpentadeca-5,9,13-trien-2-one or 6,10,14-trimethylpentadeca-5,9-dien-2-one from the mixture of step a)

Methodology Applied
Scientific EffectIsomer separation: Distillation

Data Source

PatentEP2935185B1(6r,10r)-6,10,14-trimetylpentadecan-2-one prepared from 6,10,14-trimetylpentadeca-5,9,13-trien-2-one or 6,10,14-trimetylpentadeca-5,9-dien-2-one
Publication Date: 2019.02.20 DSM IP ASSETS BV
  • EP2935185B1 patent drawingFigure 1a
  • EP2935185B1 patent drawingFigure 1b
  • EP2935185B1 patent drawingFigure 1c

AI summary

The present invention relates to a process of manufacturing (6R,10R)- 6,10,14-trimetylpentadecan-2-one in a multistep synthesis from a mixture of (5E,9E)-, (5E,9Z)-, (5Z,9E)- and (5Z.9Z)- isomers of 6, 10, 14-trimetylpentadeca- 5,9,13-trien-2-one or 6,10,14-trimetylpentadeca-5,9-dien-2-one. The process is very advantageous in that it forms in an efficient way the desired chiral product from a mixture of stereoisomers of the starting product.