Contents

Retention–Fragmentation Biosynthetic Fingerprinting of Engineered Kdo\(_2\)-Monophosphoryl Lipid A Variants

Author(s): Michael P. Doyle1, Sayan Pratab1
1Department of Chemistry, The University of Texas at San Antonio, San Antonio, TX 78249, United States
Michael P. Doyle
Department of Chemistry, The University of Texas at San Antonio, San Antonio, TX 78249, United States
Sayan Pratab
Department of Chemistry, The University of Texas at San Antonio, San Antonio, TX 78249, United States

Abstract

Kdo2-lipid A and Kdo2-monophosphoryl lipid A (Kdo2-MPLA) connect Gram-negative outer-membrane biochemistry with the analytical design of lipopolysaccharide-derived vaccine-adjuvant candidates. Their characterization is demanding because acyl-chain number, acyl-chain position, phosphate state, Kdo substitution, and ion adduction jointly shape reversed-phase retention and tandem mass-spectrometric fragmentation. This study establishes a retention–fragmentation biosynthetic fingerprint for eight structurally assigned Kdo2-lipid A derivatives from engineered Escherichia coli analyzed by triethylamine-assisted reversed-phase LC–MS/MS. Each species was encoded by acylation class, phosphate number, total acyl carbon count, secondary-acyl-chain identity, primary-chain length, precursor-adduct state, and diagnostic MS/MS evidence. A constrained two-parameter retention rule based on total acyl carbon number and phosphate count explained the observed retention ladder with high internal consistency (R2 = 0.992; root-mean-square error = 0.158 min; leave-one-out mean absolute error = 0.19 min). Matched structural contrasts showed that diphosphorylation advanced elution by 0.15–0.16 min within tetra- and hexa-acylated scaffolds, whereas replacement of C13:0(3-OH) by C14:0(3-OH) delayed elution by 0.24 min in the penta-L series. Diagnostic MS/MS evidence from Kdo/Kdo2 ions, 0, 4A2 cross-ring fragments, phosphate loss, acyl-chain loss, and adduct-dependent suppression of glycosidic cleavage separated MPLA-like, diphosphoryl lipid A (DPLA)-like, and adduct-dominated spectra. The fingerprint distinguishes target MPLA products, residual diphosphorylated species, and primary-chain microheterogeneity, giving a chemically constrained quality-control readout for Kdo2-MPLA engineering.

Keywords: Kdo2-lipid A; monophosphoryl lipid A; LC–MS/MS; triethylamine; lipidomics; biosynthetic fingerprinting; adduct-aware annotation; vaccine adjuvant
Copyright © 2026 Michael P. Doyle, Sayan Pratab. This is an open access article distributed under the Creative Commons Attribution License, which permits unrestricted use, distribution, and reproduction in any medium, provided the original work is properly cited.