Quinazoline Synthesis via Selective Demethylation and Merging

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Solution Overview

Problem

The existing process for preparing N-(3-ethynylphenyl)-7-methoxy-6-(3-morpholinopropoxy) quinazolin-4-amine dihydrochloride is not commercially viable due to the use of expensive reactants like Isovanillin, low overall yield, requirement of pyrophoric catalysts, and cumbersome work-up procedures.

Innovation Solution

A new process using 6,7-dimethoxyquinazoline-4(3H)-one as a starting material, avoiding expensive reactants and pyrophoric catalysts, and simplifying the work-up procedures by eliminating the need for intermediate isolation, with steps including selective demethylation, acetylation, chlorination, and subsequent reactions to achieve high yields and purity.

Engineering Contradictions & Design Principles

VSEngineering Contradiction Analysis

1Ease of manufacture

If the existing process using Isovanillin is employed, then the compound can be prepared, but the process is not commercially viable due to expensive reactants and low overall yield

Engineering Contradiction:
Improvecommercial viabilityVSAvoidoverall yield
Core Design Contradiction:
Ease of manufactureVSProductivity

Solution Approach 1:

The patent replaces expensive Isovanillin with cheap and readily available 6,7-dimethoxyquinazoline-4(3H)-one as the starting material. This substitution of costly reactants with inexpensive alternatives directly addresses the commercial viability issue while maintaining the ability to produce the target compound

Inventive Principle:
Principle #27Cheap short-living objects (Disposable)

Solution Approach 2:

The synthesis is divided into multiple discrete steps (demethylation, acetylation, chlorination, condensation) allowing for better process control and intermediate management. This segmentation enables optimization of each individual step's yield while avoiding the cumulative losses of a single-step process

Inventive Principle:
Principle #1Segmentation

2Ease of manufacture

If the existing process is used, then the compound can be prepared, but it requires pyrophoric catalysts like Raney Nickel and high pressure reactions

Engineering Contradiction:
Improveprocess safetyVSAvoidhazardous reagents
Core Design Contradiction:
Ease of manufactureVSObject-affected harmful factors

Solution Approach 1:

The patent eliminates pyrophoric Raney Nickel catalyst and high-pressure equipment by using conventional reagents and ambient pressure conditions. This substitution of hazardous materials with safer alternatives directly improves process safety while removing the need for specialized handling equipment

Inventive Principle:
Principle #27Cheap short-living objects (Disposable)

Solution Approach 2:

The patent converts potentially harmful reactions into safer alternatives by replacing pyrophoric catalysts with conventional base-catalyzed condensations and high-pressure hydrogenations with ambient pressure reactions using safer reagents like thionyl chloride and morpholinopropyl chloride

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

3Ease of operation

If the existing process is followed, then the compound can be prepared, but it involves cumbersome work-up procedures and isolation of intermediates

Engineering Contradiction:
Improvework-up simplicityVSAvoidprocess timeline
Core Design Contradiction:
Ease of operationVSLoss of time

Solution Approach 1:

The patent combines multiple operations into streamlined sequences: demethylation followed by acetylation without full isolation, and chlorination followed by condensation in sequence. This merging of steps reduces the number of isolation and purification operations, simplifying work-up procedures and reducing overall process time

Inventive Principle:
Principle #5Merging (Combining)

Solution Approach 2:

The patent performs acetylation as a preliminary protective step before chlorination, and conducts chlorination and condensation in sequence without isolating the intermediate. This preliminary action approach allows for smoother process flow and eliminates time-consuming isolation steps

Inventive Principle:
Principle #10Preliminary 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

The new process achieves high yields and purity (>99.9% HPLC) of the compound, making it commercially viable, cost-effective, and scalable, while avoiding the use of expensive reagents and hazardous catalysts, thus improving process timelines and reducing environmental impact.

Implementation Method 1

selective demethylation of 6,7-dimethoxyquinazoline-4(3H)-one using DL-Methionine-sulfuric acid medium to get 6-hydroxy-7-methoxy quinazoline-4(3H)-one

Methodology Applied
Scientific EffectSelective demethylation: Chemical Bonding

Implementation Method 2

acetylation of 6-hydroxy-7-methoxyquinazoline-4(3H)-one in acetic anhydride medium to get 6-acetoxy-7-methoxyquinazoline-4(3H)-one

Methodology Applied
Scientific EffectAcetylation: Chemical Bonding

Implementation Method 3

reacting 6-acetoxy-7-methoxy-quinazoline-4(3H)-one with thionyl chloride in the presence of DMF in chloroform to get 6-acetoxy-4-chloro-7-methoxyquinazoline hydrochloride

Methodology Applied
Scientific EffectChlorination: Chemical Bonding

Implementation Method 4

reacting 6-acetoxy-4-chloro-7-methoxyquinazoline hydrochloride in-situ with 3-ethynylaniline of formula-III in isopropanol medium to get 6-acetoxy-4-(3-ethynylanilino)-7-methoxyquinazoline hydrochloride

Methodology Applied
Scientific EffectNucleophilic substitution: Chemical Bonding

Implementation Method 5

treating 6-acetoxy-4-(3-ethynylanilino)-7-methoxyquinazoline hydrochloride salt of formula-XVII in-situ with aqueous ammonia in methanol medium to get 4-(3-ethynylanilino)-6-hydroxy-7-methoxyquinazoline

Methodology Applied
Scientific EffectHydrolysis: Chemical Bonding

Implementation Method 6

reacting 4-(3-ethynylanilino)-6-hydroxy-7-methoxyquinazoline of formula-XVIII with 3-morpholinopropyl chloride of compound of formula-VI in presence of base in DMF to get N-(3-ethynylphenyl)-7-methoxy-6-(3-morpholinopropoxy) quinazolin-4-amine

Methodology Applied
Scientific EffectEther formation: Chemical Bonding

Data Source

PatentEP3609875B1An improved process for the preparation of n-(3-ethynylphenyl)-7-methoxy-6-(3-morpholinopropoxy) quinazolin -4-amine dihydrochloride
Publication Date: 2021.10.20 NATCO PHARMA LTD
  • EP3609875B1 patent drawingFigure 1
  • EP3609875B1 patent drawingFigure 2
  • EP3609875B1 patent drawing

AI summary

Present invention relates to an improved process for the preparation of N-(3- ethynylphenyl)-7-methoxy-6-(3-morpholinopropoxy) quinazolin-4-amine dihydrochloride of formula-I.