Development of a quantification method for arginase inhibitors by LC-MS/MS with benzoyl chloride derivatization

J Pharm Biomed Anal. 2024 Aug 15:246:116210. doi: 10.1016/j.jpba.2024.116210. Epub 2024 May 8.

Abstract

Arginase is an enzyme responsible for converting arginine, a semi-essential amino acid, to ornithine and urea. Arginine depletion suppresses immunity via multiple mechanisms including inhibition of T-cell and NK cell proliferation and activity. Arginase inhibition is therefore an attractive mechanism to potentially reverse immune suppression and thus has been explored as a therapy for oncology and respiratory indications. Small molecules targeting arginase present significant bioanalytical challenges for in vitro and in vivo characterization as inhibitors of arginase are typically hydrophilic in nature. The resulting low or negative LogD characteristics are incompatible with common analytical methods such as RP-ESI-MS/MS. Accordingly, a sensitive, high-throughput bioanalytical method was developed by incorporating benzoyl chloride derivatization to increase the hydrophobic characteristics of these polar analytes. Samples were separated by reversed phase chromatography on a Waters XBridge BEH C18 3.5 μm, 30 × 3 mm column using gradient elution. The mass spec was operated in positive mode using electrospray ionization. The m/z 434.1→176.1, 439.4→181.2, 334.9→150.0 and 339.9→150.0 for AZD0011, AZD0011 IS, AZD0011-PL and AZD0011-PL IS respectively were used for quantitation. The linear calibration range of the assay was 1.00-10,000 ng/mL with QC values of 5, 50 and 500 ng/mL. The qualified method presented herein exhibits a novel, robust analytical performance and was successfully applied to evaluate the in vivo ADME properties of boronic acid-based arginase inhibitor prodrug AZD0011 and its active payload AZD0011-PL.

Keywords: Arginase; Benzoyl chloride; Chromatography; Derivatization; LC-MS/MS; Mass spectrometry.

MeSH terms

  • Animals
  • Arginase* / antagonists & inhibitors
  • Chromatography, High Pressure Liquid / methods
  • Chromatography, Liquid / methods
  • Chromatography, Reverse-Phase / methods
  • Enzyme Inhibitors / analysis
  • Enzyme Inhibitors / chemistry
  • Enzyme Inhibitors / pharmacology
  • Humans
  • Hydrophobic and Hydrophilic Interactions
  • Liquid Chromatography-Mass Spectrometry
  • Reproducibility of Results
  • Spectrometry, Mass, Electrospray Ionization / methods
  • Tandem Mass Spectrometry* / methods

Substances

  • Arginase
  • Enzyme Inhibitors