Abstract

An amine transaminase was engineered for the efficient production of a chiral precursor to sacubitril, (2R,4S)-5-([1,1′-biphenyl]-4-yl)-4-amino-2-methylpentanoic acid, a key component in the blockbuster heart failure drug Entresto. Starting from an enzyme with trace activity and preference for the undesired diastereoisomer, 11 rounds of enzyme evolution were performed. The resultant variant, CDX-043, showed high productivity giving 90% conversion at 75 g/L substrate concentration with 1% enzyme loading with respect to the substrate in 24 h and without the use of an organic cosolvent. The product diastereomeric purity toward the desired (2R,4S)-stereoisomer was >99.9:0.1 d.r. This variant also exhibited high process robustness and could tolerate reaction temperatures up to 65 °C, isopropylamine concentrations of at least 2 M, and reaction times of at least 5 days. A structural analysis of the enzyme variants gave insight into how the mutations affected activity and selectivity. This enzyme variant allows for the efficient and cost-effective production of sacubitril at large scale.

Highlights

  • The pharmaceutical drug Entresto, used for the treatment of heart failure, combines sacubitril and valsartan as active pharmaceutical ingredients (APIs) in a 1:1 molar ratio in a crystalline supramolecular complex (Figure 1)

  • Entresto combines two modes of action, with sacubitril acting as a neprilysin inhibitor and valsartan as an angiotensin receptor blocker

  • In the PARADIGM-HF clinical trial, this drug was found to be more effective than standard treatment options in patients with heart failure with reduced ejection fraction.[1]

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Summary

INTRODUCTION

The pharmaceutical drug Entresto, used for the treatment of heart failure, combines sacubitril and valsartan as active pharmaceutical ingredients (APIs) in a 1:1 molar ratio in a crystalline supramolecular complex (Figure 1). This biocatalytic transformation forms the strategic centerpiece of the alternative route, which could not be pursued using established chemical transformations and as such fully relies on the successful diastereoselective transamination of ketone 1 to amine 2.3e,4.

RESULTS AND DISCUSSION
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