Dynamic and temporal assessment of human dried blood spot MS/MSALLshotgun lipidomics analysis.
BACKGROUND
Real-time and dynamic assessment of an individual's lipid homeostatic state in blood is complicated due to the need to collect samples in a clinical environment. In the context of precision medicine and population health, tools that facilitate sample collection and empower the individual to participate in the process are necessary to complement advanced bioanalytical analysis. The dried blood spot (DBS) methodology via finger prick or heel prick is a minimally invasive sample collection method that allows the relative ease and low cost of sample collection as well as transport. However, it has yet to be integrated into broad scale personalized lipidomic analysis. Therefore, in this study we report the development of a novel DBS high resolution MS/MSALLlipidomics workflow.


METHODS
In this report we compared lipidomic analysis of four types of blood sample collection methods (DBS, venous whole blood, serum, and plasma) across several parameters, which include lipidomics coverage of each matrix and the effects of temperature and time on the coverage and stability of different lipid classes and molecular species. The novel DBS-MS/MSALLlipidomics platform developed in this report was then applied to examine postprandial effects on the blood lipidome and further to explore the temporal fluctuation of the lipidome across hours and days.


RESULTS
More than 1,200 lipid molecular species from a single DBS sample were identified and quantified. The lipidomics profile of the DBS samples is comparable to whole blood matrix. DBS-MS/MSALLlipidomic analysis in postprandial experiments revealed significant alterations in triacylglyceride species. Temporal analysis of the lipidome at various times in the day and across days identified several lipid species that fluctuate as a function of time, and a subset of lipid species were identified to be significantly altered across hours within a day and within successive days of the week.


CONCLUSIONS
A novel DBS-MS/MSALLlipidomics method has been established for human blood. The feasibility and application of this method demonstrate the potential utility for lipidomics analysis in both healthy and diverse diseases states. This DBS MS-based lipidomics analysis represents a formidable approach for empowering patients and individuals in the era of precision medicine to uncover novel biomarkers and to monitor lipid homeostasis.
BERG, LLC, 500 Old Connecticut Path, Bldg B, 3rd Floor, Framingham, MA 01701 USA.
Fei
F
Gao
BERG, LLC, 500 Old Connecticut Path, Bldg B, 3rd Floor, Framingham, MA 01701 USA.
Justice
J
McDaniel
BERG, LLC, 500 Old Connecticut Path, Bldg B, 3rd Floor, Framingham, MA 01701 USA.
Emily Y
EY
Chen
BERG, LLC, 500 Old Connecticut Path, Bldg B, 3rd Floor, Framingham, MA 01701 USA.
Hannah E
HE
Rockwell
BERG, LLC, 500 Old Connecticut Path, Bldg B, 3rd Floor, Framingham, MA 01701 USA.
Jeremy
J
Drolet
BERG, LLC, 500 Old Connecticut Path, Bldg B, 3rd Floor, Framingham, MA 01701 USA.
Vivek K
VK
Vishnudas
BERG, LLC, 500 Old Connecticut Path, Bldg B, 3rd Floor, Framingham, MA 01701 USA.
Vladimir
V
Tolstikov
BERG, LLC, 500 Old Connecticut Path, Bldg B, 3rd Floor, Framingham, MA 01701 USA.
Rangaprasad
R
Sarangarajan
BERG, LLC, 500 Old Connecticut Path, Bldg B, 3rd Floor, Framingham, MA 01701 USA.
Niven R
NR
Narain
BERG, LLC, 500 Old Connecticut Path, Bldg B, 3rd Floor, Framingham, MA 01701 USA.
Michael A
MA
Kiebish
Dried blood spot; Human; Mass spectrometry; Shotgun lipidomics