The paper introduces PAP-SL (parallel (immuno)affinity purification coupled to shotgun lipidomics), enabling simultaneous isolation and stoichiometric lipid quantification of six compartmentsβplasma membrane (PM), endoplasmic reticulum (ER), cis-Golgi, trans-Golgi network (TGN), mitochondria, and lysosomesβfrom matched post-nuclear fractions of HeLa cells. Validation by Western blotting confirmed compartment specificity with only minor cross-contamination (mitochondrial lipids in TGN) .
The dataset comprises 331 lipid species across 24 classes (cholesterol, 7 sphingolipid classes, 16 glycerophospholipid classes including diacyl, ether, and lyso subcategories) from 5 independent PAP rounds with 4β5 replicates. Absolute quantification used internal standards on a Q Exactive Orbitrap with LipidXplorer identification and LipidQ normalization .
Pearson correlation networks (|r|>0.7) and hierarchical clustering converged on six modules (IβVI) covering 261 species: PM (Cluster I), PMβlysosome bridge (II), lysosome (III), ERβlysosome bridge (IV), ER (V), and mitochondria (VI). Intra-class correlations were strong (median r = 0.52) versus weak inter-class correlations (r = β0.057), indicating that biosynthetic origin constrains co-distribution .
The cholesterol gradient (7.8 mol% in ER β 50 mol% at PM) and parallel PS enrichment (0.31 β 3.0 mol%) mirror known ORP-mediated transport . Ceramide showed a flat distribution while SM expanded from 0.79 mol% (ER) to 12.6 mol% (PM), consistent with CERT-mediated ERβGolgi transfer followed by SM synthesis at the Golgi .
A key novel finding is that the sn-1 ether linkage redirects ER-synthesized GPLs toward lysosomes. PC O- reached 11.7 mol% in lysosomes (PC O-:PC ratio ~0.5 vs ~0.15 in ER), while PE O- peaked at both PM (3.0 mol%) and lysosomes (4.2 mol%). In KRAS-knockout HKh-2 cells, lysosomal PC O- collapsed from 17 mol% (HCT116) to 1.8 mol%, correlating with enhanced CDP-ethanolamine flux; ethanolamine supplementation reproduced this collapse (5.8 β 1.6 mol%) . The authors propose selective persistence (ether bonds resist lysosomal phospholipases) as the mechanism, supported by chemical hydrolysis resistance of ether linkages .
Mean double bonds per molecule declined from 1.8 (ER) to 1.1 (PM) for PC while saturated PC species rose from 9 mol% (ER) to 31 mol% of class at PM. The authors identify two complementary strategies: (1) whole-class recruitment of intrinsically saturated PS and SM, and (2) species-level enrichment of saturated GPLs within otherwise unsaturated classes . This is consistent with the concept that saturated acyl chains pack favorably with cholesterol and SM .
This work transforms fragmented compartment lipidomics into a cell-wide atlas with organizing principles. The etherGPL lysosomal territory finding is genuinely novel and has implications for lysosomal membrane stability, cancer metabolism (KRAS-driven ethanolamine demand), and ether lipid biology .
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