Diastereomerically Pure DL/LD-Methionylmethionine via Epimerization

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Solution Overview

Problem

The existing process for preparing DL/LD-methionylmethionine from DD/LL-methionine results in a product with an unfavorable ratio of diastereomers, leading to differing physical properties such as solubility, flowability, and flammability, which are not suitable for aquaculture applications.

Innovation Solution

A process involving cyclization and epimerization of DD/LL-methionylmethionine to produce DL/LD-2,6-bis(methionyl)-1,4-diketopiperazine, followed by hydrolysis, to achieve a higher proportion of the less soluble DL/LD diastereomer, improving handling and safety properties by converting the more soluble DDLL-Met-Met back into its precursor DKP and epimerizing it to DLLD-Met-Met.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Reliability

If the existing process is used to prepare DL/LD-methionylmethionine from DD/LL-methionine, then the product is obtained, but the ratio of diastereomers is unfavorable (60/40 DLLD/DDLL) leading to high water solubility (21.0 g/l for DDLL) which causes losses through leaching from feed pellets

Engineering Contradiction:
Improveproduct stability in aquaculture feedVSAvoidlosses through leaching
Core Design Contradiction:
ReliabilityVSLoss of substance

Solution Approach 1:

The invention changes the diastereomeric composition parameter of the product by introducing an epimerization step that converts DDLL-DKP to DLLD-DKP. This parameter change results in a product with ≥90 mol% DLLD diastereomer, which has low water solubility (0.4 g/l), thereby preventing leaching losses from feed pellets while maintaining animal nutritional requirements

Inventive Principle:
Principle #35Parameter changes

Solution Approach 2:

Instead of directly converting DDLL-Met-Met to DLLD-Met-Met, the invention inverts the approach by first converting both diastereomers to their DKP precursors, then epimerizing the DDLL-DKP to DLLD-DKP before final hydrolysis. This indirect route through the cyclic DKP intermediate enables effective diastereomeric enrichment

Inventive Principle:
Principle #13The other way round (Inversion)

2Manufacturing precision

If DDLL-Met-Met crystallizes out in the form of needles, then it can be separated, but it has high water solubility (21.0 g/l) which is unfavorable for aquaculture use

Engineering Contradiction:
Improvediastereomeric purityVSAvoidleaching from feed
Core Design Contradiction:
Manufacturing precisionVSLoss of substance

Solution Approach 1:

The invention changes the diastereomeric composition parameter by epimerizing DDLL-DKP to DLLD-DKP during the cyclization process. The resulting product contains ≥90 mol% DLLD diastereomer, which has low water solubility (0.4 g/l), preventing leaching losses while maintaining manufacturability through controlled crystallization

Inventive Principle:
Principle #35Parameter changes

Solution Approach 2:

The invention converts the harmful high solubility of DDLL-Met-Met into a benefit by epimerizing it to DLLD-Met-Met during processing. The low solubility of the DLLD form (0.4 g/l) is then advantageous as it prevents leaching from feed pellets, transforming a previously problematic property into a desirable one

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

3Loss of substance

If a higher proportion of DLLD-Met-Met is produced, then water solubility decreases (0.4 g/l), but the process requires additional epimerization steps

Engineering Contradiction:
Improvereduced leachingVSAvoidprocess steps
Core Design Contradiction:
Loss of substanceVSDevice complexity

Solution Approach 1:

The invention merges the cyclization reaction with the epimerization process into a single integrated step. By conducting the cyclization of Met-Met to DKP under conditions that promote epimerization (pH 4-7, elevated temperature), the process simultaneously achieves both objectives without requiring separate epimerization equipment or steps

Inventive Principle:
Principle #5Merging (Combining)

Solution Approach 2:

The invention maintains continuous useful action by performing epimerization during the cyclization reaction itself rather than as a separate step. The reaction conditions (pH 4-7, temperature) are optimized to continuously promote both cyclization and epimerization, eliminating idle time and additional processing stages

Inventive Principle:
Principle #20Continuity of useful action

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 achieves a higher yield of diastereomerically pure DL/LD-methionylmethionine with improved bulk density, flow characteristics, and reduced flammability, making it more suitable for use in aquaculture as an animal feed additive.

Implementation Method 1

a process for the diastereomerically pure preparation of DL/LD-methionylmethionine from DD/LL-methionylmethionine by means of cyclization and epimerization

Methodology Applied
Scientific EffectCyclization:

Implementation Method 2

the undesired DDLL-Met-Met is back-converted into the direct precursor DKP again and in the process is simultaneously epimerized

Methodology Applied
Scientific EffectEpimerization:

Implementation Method 3

subsequent hydrolysis

Methodology Applied
Scientific EffectHydrolysis: Hydrolysis

Data Source

PatentEP4271666B1Process for the diastereomerically pure preparation of DL/LD-methionylmethionine
Publication Date: 2024.12.18 EVONIK OPERATIONS GMBH
  • EP4271666B1 patent drawingFigure 1
  • EP4271666B1 patent drawingFigure 2
  • EP4271666B1 patent drawing

AI summary

The invention relates in particular to a process for the preparation of DL/LD-methionine diketopiperazine (I) characterized in that a DD/LL-methionylmethionine-containing aqueous solution or suspension, which has a pH of 3 to 7, measured using a pH electrode at 20°C, is reacted at a temperature of 150 to 220°C, preferably at 170 to 210°C, until an aqueous solution or suspension has formed containing at least a proportion of 30 mol%, preferably 50 mol%, especially 60 mol% of DL/LD-methionine diketopiperazine, based on the total content of DL/LD- and DD/LL-methionine diketopiperazine in the reaction mixture. This process forms part of an overall process for the preparation of DL/LD-methionylmethionine, which is obtained by hydrolysis from the DL/LD-methionine diketopiperazine (I) produced initially.