Preparation and Application of TMPZnCl·LiCl: The Influence of Magnesium Chloride on Regioselectivity

TMPZnCl·LiCl is a novel, mild, and efficient base used for the metallation of aromatic rings, resulting in anions that await electrophilic attack.

The University of Munich published an article in the OPRD journal discussing how the presence or absence of magnesium chloride affects regioselectivity when using TMPZnCl·LiCl as a base. Let’s take a look at the reaction.

Reaction Process

  • Compound 1 via pathway a, without magnesium chloride, yields compound 5.

  • Compound 1 via pathway b, with magnesium chloride, yields compound 6.

Preparation and Application of TMPZnCl·LiCl: The Influence of Magnesium Chloride on Regioselectivity

Iodination Case

Preparation and Application of TMPZnCl·LiCl: The Influence of Magnesium Chloride on Regioselectivity

Preparation of TMPZn·LiCl

A dry and argon-flushed 1.0 L Schlenk flask, equipped with a magnetic stirring bar and a rubber septum, was charged with 2,2,6,6-tetramethylpiperidine (59.5 mL, 350 mmol) freshly dissolved in THF (350 mL). This solution was cooled to −40 °C, and n-BuLi (2.3 M in hexane, 152.2 mL, 350 mmol) was added dropwise. After the addition was complete, the reaction mixture was allowed to warm up slowly to −10 °C for 1 h. ZnCl2 (1.0 M in THF, 368 mL, 368 mmol, 1.05 equiv) was added dropwise, and the resulting solution was stirred for 30 min at −10 °C and then for 30 min at 25 °C. The solvents were then removed under vacuum, affording a yellowish solid. Freshly distilled THF was then slowly added under vigorous stirring until the salts were completely dissolved. The freshly prepared TMPZnCl·LiCl (2) solution was titrated prior to use at 25 °C with benzoic acid using 4-(phenylazo)diphenylamine as an indicator. A concentration of 1.35 M in THF was obtained.

Preparation of C(3) Zincated Chromone 3.
A dry and argon flushed flask, equipped with a magnetic stirring bar and a rubber septum, was charged with chromone (1, 7.3 g, 50 mmol) in dry THF (50 mL). The base TMPZnCl·LiCl (2, 1.2M in THF, 50 mL, 1.2 equiv) was added dropwise at 0 °C over 30 min, through an additional funnel. The reaction mixture was warmed to 25 °C and stirred for an additional 7 h. The completion of the metalation was checked by GC analysis of reaction aliquots quenched with iodine indicating a regioselectivity of C(2):C(3) = 98:2 and 98% conversion.
Preparation of C(2) Zincated Chromone 4.
A dry and argon flushed flask, equipped with a magnetic stirring bar and a rubber septum, was charged with chromone (1, 7.31 g, 50 mmol) and dry MgCl2 (0.4 M in THF, 250 mL) at 0 °C. The base TMPZnCl·LiCl (2, 1.2 M in THF, 50 mL, 1.2 equiv) was added dropwise at −5 °C over 30 min, through an addition funnel. The reaction mixture was warmed to 0 °C and stirred for an additional 2 h. The completion of the metalation was checked by GC analysis of reaction aliquots quenched with iodine indicating a regioselectivity of C(2):C(3) = 92:8 and full conversion.

References

Org. Process Res. Dev. 2017, 21, 660−663

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