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Fig 1.

Biochemical pathway of propionate metabolism (simplified).

3OHPA: 3-hydroxypropionic acid; MMA: methylmalonic acid; MCA: methylcitric acid; Cbl: cobalamin. Drawn using Inkscape 0.91pre4 (Open Source Software licensed under the GNU General Public License).

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Table 1.

Optimized MS/MS settings in the second-tier LC-MS/MS assay (negative electrospray ion mode).

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Table 2.

Assay validation in calibrator dried blood spots (n = 10).

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Fig 2.

LC-MS/MS chromatogram of DBS from a healthy newborn.

Peak 1: 3-hydroxypropionic acid (3OHPA); peak 2: lactic acid; peak 3: succinic acid; peak 4: methylmalonic acid (MMA); peaks 5a and 5b: methylcitric acid (MCA); peak 0: interfering peak; DBS: dried blood spot. Numbered black peaks: unlabelled analytes; numbered unfilled peaks: deuterated internal standards. All intensities (Y-axes) have been normalized to 4*105 cps for better comparability (not on the inserted zoom-in figures) and have been plotted against retention time (X-axes). Chromatograms were generated by MassLynx 4.1 (Waters, Milford, MA, USA) and modified using Inkscape 0.91pre4 (Open Source Software licensed under the GNU General Public License).

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Fig 3.

LC-MS/MS chromatogram of DBS from a PA patient.

Peak 1: 3-hydroxypropionic acid (3OHPA); peak 2: lactic acid; peak 3: succinic acid; peak 4: methylmalonic acid (MMA); peaks 5a and 5b: methylcitric acid (MCA); peak 0: interfering peak; DBS: dried blood spot; PA: propionic acidemia. Numbered black peaks: unlabelled analytes; numbered unfilled peaks: deuterated internal standards. All intensities (Y-axes) have been normalized to 4*105 cps for better comparability (not on the inserted zoom-in figures) and have been plotted against retention time (X-axes). Chromatograms were generated by MassLynx 4.1 (Waters, Milford, MA, USA) and modified using Inkscape 0.91pre4 (Open Source Software licensed under the GNU General Public License).

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Fig 3 Expand

Fig 4.

LC-MS/MS chromatogram of DBS from a MMAmut(0) patient.

Peak 1: 3-hydroxypropionic acid (3OHPA); peak 2: lactic acid; peak 3: succinic acid; peak 4: methylmalonic acid (MMA); peaks 5a and 5b: methylcitric acid (MCA); peak 0: interfering peak; DBS: dried blood spot; MMAmut(0): methylmalonyl-CoA mutase deficiency (complete). Numbered black peaks: unlabelled analytes; numbered unfilled peaks: deuterated internal standards. All intensities (Y-axes) have been normalized to 4*105 cps for better comparability (not on the inserted zoom-in figures) and have been plotted against retention time (X-axes). Chromatograms were generated by MassLynx 4.1 (Waters, Milford, MA, USA) and modified using Inkscape 0.91pre4 (Open Source Software licensed under the GNU General Public License).

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Fig 4 Expand

Table 3.

Assay validation in dried blood spots using quality control samples at three concentrations (n = 10).

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Table 3 Expand

Table 4.

Results of dried blood spot samples from patients with known diagnosis: Retrospective analysis of NBS specimens (untreated) and samples during therapy.

Data are provided as medians (ranges).

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Table 5.

Results of External Quality Assurance dried blood spot samples (n = 7).

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