Fast and Effective Ion Mobility-Mass Spectrometry Separation of d-Amino-Acid-Containing Peptides.

Fast and Effective Ion Mobility-Mass Spectrometry Separation of d-Amino-Acid-Containing Peptides.
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DOI:
10.1021/acs.analchem.7b03401
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发表时间:
2017-11-07
影响因子:
7.4
通讯作者:
Fernandez-Lima F
Fernandez-Lima F
中科院分区:
化学1区
文献类型:
--
作者:
Jeanne Dit Fouque K;Garabedian A;Porter J;Baird M;Pang X;Williams TD;Li L;Shvartsburg A;Fernandez-Lima F

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Despite often minute concentrations in vivo, D-amino acid containing peptides (DAACPs) are crucial to many life processes. Standard proteomics protocols fail to detect them as D/L substitutions do not affect the peptide parent and fragment masses. The differences in fragment yields are often limited, obstructing the investigations of important but low abundance epimers in isomeric mixtures. Separation of D/L-peptides using ion mobility spectrometry (IMS) was impeded by small collision cross section differences (commonly ~1%). Here, broad baseline separation of DAACPs with up to ~30 residues employing trapped IMS with resolving power up to ~340, followed by time-of-flight mass spectrometry is demonstrated. The D/L-pairs co-eluting in one charge state were resolved in another, and epimers merged as protonated species were resolved upon metalation, effectively turning the charge state and cationization mode into extra separation dimensions. Linear quantification down to 0.25% proved the utility of high resolution IMS-MS for real samples with large inter-isomeric dynamic range. Very close relative mobilities found for DAACP pairs using traveling-wave IMS (TWIMS) with different ion sources and faster IMS separations showed the transferability of results across IMS platforms. Fragmentation of epimers can enhance their identification and further improve detection and quantification limits, and we demonstrate the advantages of online mobility separated collision-induced dissociation (CID) followed by high resolution mass spectrometry (TIMS-CID-MS) for epimer analysis.
DOI: 10.1039/c4ay01655f
发表时间: 2014-12-07
期刊: Analytical methods : advancing methods and applications
影响因子: --
作者:
Castellanos A;Benigni P;Hernandez DR;DeBord JD;Ridgeway ME;Park MA;Fernandez-Lima F
通讯作者: Fernandez-Lima F
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影响因子: 7.4
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发表时间: 2011-06-15
影响因子: 2
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发表时间: 2005-07-15
影响因子: 7.4
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