International Journal of Mass Spectrometry最新文献

{"title":"Nonlinear frequency modulation for Fourier transform ion mobility mass spectrometry improves experimental efficiency","authors":"Elvin R. Cabrera ,&nbsp;Robert L. Schrader ,&nbsp;Thomas E. Walker ,&nbsp;Arthur Laganowsky ,&nbsp;David H. Russell ,&nbsp;Brian H. Clowers","doi":"10.1016/j.ijms.2024.117197","DOIUrl":"10.1016/j.ijms.2024.117197","url":null,"abstract":"<div><p><span><span>Through optimization of terminal frequencies and effective sampling rates, we have developed nonlinear sawtooth-shaped frequency sweeps for efficient Fourier transform ion mobility </span>mass spectrometry (FT-IM-MS) experiments. This is in contrast to conventional FT-IM-MS experiments where ion gates are modulated according to a linear frequency sweep. Linear frequency sweeps are effective but can be hindered by the amount of useful signal obtained using a single sweep over a large frequency range imposed by ion gating inefficiencies, particularly small ion packets, and gate depletion. These negative factors are direct consequences of the inherently low gate pulse widths of high-frequency ion gating events, placing an upper bound on FT-IM-MS performance. Here, we report alternative ion modulation strategies. Sawtooth frequency sweeps may be constructed for the purpose of either extending high-SNR transients or conducting efficient signal-averaging experiments for low-SNR transients. The data obtained using this approach show high-SNR signals for a set of low-mass tetraalkylammonium salts (&lt;1000 </span><em>m</em>/<em>z</em><span>) where resolving powers in excess of 500 are achieved. Data for low-SNR obtained for multimeric protein complexes streptavidin (53 kDa) and GroEL (800 kDa) also reveal large increases in the signal-to-noise ratio for reconstructed arrival time distributions.</span></p></div>","PeriodicalId":338,"journal":{"name":"International Journal of Mass Spectrometry","volume":"497 ","pages":"Article 117197"},"PeriodicalIF":1.8,"publicationDate":"2024-01-09","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139410965","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"A remembrance of John B. Fenn on the 20th anniversary of his 2002 Nobel Prize in Chemistry","authors":"M. Labowsky ,&nbsp;P.J. Gale","doi":"10.1016/j.ijms.2023.117187","DOIUrl":"10.1016/j.ijms.2023.117187","url":null,"abstract":"","PeriodicalId":338,"journal":{"name":"International Journal of Mass Spectrometry","volume":"497 ","pages":"Article 117187"},"PeriodicalIF":1.8,"publicationDate":"2024-01-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139083466","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Development of a portable gas chromatography linear ion trap mass spectrometer (GC-LIT-MS) for VOCs analysis in water","authors":"Qiu Junwei,&nbsp;Xu Kai,&nbsp;Zhang Tao,&nbsp;Zhu Huijun,&nbsp;Zhang Shuo,&nbsp;Lu Xinxin,&nbsp;Li Xiaoxu","doi":"10.1016/j.ijms.2023.117189","DOIUrl":"10.1016/j.ijms.2023.117189","url":null,"abstract":"<div><p><span><span><span>The detection of volatile organic compounds (VOCs) in water faces challenges due to the presence of complex matrix interferences and low concentration. This paper presented a portable </span>gas chromatography linear </span>ion trap<span> mass spectrometer (GC-LIT-MS) coupled with dynamic headspace sampling (DHS) system for sensitive and rapid on-site analysis of VOCs in water. The instrument weighs 18 kg and has compact dimensions of 43 cm × 35 cm x 20 cm, offering portability and convenience. A low thermal mass (LTM) chromatographic column, utilizing resistive heating, enables rapid heating and cooling within the runtime of GC. The linear ion trap, for the first time, has been integrated as a mass analyser in portable gas chromatography-mass spectrometer (GC-MS). Its ability to store a greater number of ions within the trap expands the dynamic range of the instrument. The influence of dynamic headspace injection conditions on the purging efficiency of VOCs was investigated and the equilibrium temperature was optimized. The GC-LIT-MS method was demonstrated to be capable to identify and separate 55 VOCs in water within 4 min, with most of them exhibiting detection limits of less than 1 μg L</span></span>⁻¹. The calibration of 4 VOCs with concentrations ranged from 2 parts per million (ppm) to 200 ppm showed excellent linearity (R² &gt; 0.99) and dynamic range more than five orders of magnitude. Resolution superior to unit mass was achieved within the range of 15 AMU to 550 AMU.</p></div>","PeriodicalId":338,"journal":{"name":"International Journal of Mass Spectrometry","volume":"497 ","pages":"Article 117189"},"PeriodicalIF":1.8,"publicationDate":"2023-12-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139064861","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Gas-phase Ni(II) affinities of alternative metal binding peptides from competitive threshold collision-induced dissociation","authors":"Perfect Asare,&nbsp;Kwabena N. Senyah,&nbsp;Jonathan D. Wilcox,&nbsp;Jovany Morales,&nbsp;Laurence A. Angel","doi":"10.1016/j.ijms.2023.117188","DOIUrl":"10.1016/j.ijms.2023.117188","url":null,"abstract":"<div><p><span>The Ni(II) affinity<span> of the polyhistidine tag<span> is used in the purification of recombinant proteins by immobilized metal affinity chromatography. Here we measured the relative gas-phase Ni(II) affinities of four alternative metal binding (amb) peptides and the 7xHis tag using the competitive threshold collision-induced dissociation (TCID) technique. The general primary structure of the four amb peptides was acetyl-Aa</span></span></span>₁-Aa₂-Gly₃-Pro₄-Aa₅-Gly₆-Cys₇, designed to test whether the His₁-Cys₂ or Asp₁-His₂ would exhibit the higher Ni(II) affinity and whether the Tyr₅<span> with its ability of forming long-range π-nickel interaction and hydrogen bonding would contribute to the Ni(II) affinity. The Cys</span>₇<span><span> is retained in all the amb sequences because previous research has shown that both the thiolate side group and </span>carboxylate<span> terminus simultaneously coordinate the metal ion. The Ni(II) affinity was measured using the dissociation of the [amb + Ni(II) + NTA]</span></span>⁻<span> complex, where NTA = nitrilotriacetic acid, which is a commonly used ligand for Ni(II) inside the IMAC column. The dissociation of [amb + Ni(II) + NTA]</span>⁻ produced two main product channels; [amb + Ni(II)]⁻ + NTA and [NTA + Ni(II)]⁻<span> + amb, whose competition was modeled by TCID to extract the relative gas-phase Ni(II) affinities. Extensive molecular modeling using PM6 located the low-energy structures whose molecular parameters were used in the TCID analyses if their collision cross sections agreed with those measured by traveling-wave ion mobility mass spectrometry and they were compatible with a concerted reaction. We compare the final results by conducting the TCID analyses using alternative PM6 parameters and by making the ternary complexes in acidic and basic solutions.</span></p></div>","PeriodicalId":338,"journal":{"name":"International Journal of Mass Spectrometry","volume":"497 ","pages":"Article 117188"},"PeriodicalIF":1.8,"publicationDate":"2023-12-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"139064686","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Detection of emerging disinfection by-products by reversed-phase ion-pair chromatography electrospray-ionization mass spectrometry in drinking water","authors":"Bhekumuzi P. Gumbi ,&nbsp;Leon J. Khoza ,&nbsp;Nokwanda Hendricks ,&nbsp;Gbadebo C. Adeyinka ,&nbsp;Pinkie Ntola ,&nbsp;Siyabonga S. Ndlela ,&nbsp;Patrick G. Ndungu","doi":"10.1016/j.ijms.2023.117186","DOIUrl":"10.1016/j.ijms.2023.117186","url":null,"abstract":"<div><p><span>A sensitive and specific methodology that allows unequivocal identification of polydiallyldimethylammonium chloride (PDADMAC) disinfection by-product it monomer<span><span> diallyldimethylammonium chloride (DADMAC) in drinking water samples based on reversed-phase ion-pair chromatography–electrospray ionization – </span>mass spectrometry<span> was optimized. Ion-pair reagent heptafluorobutyric (HFBA) was found to play a crucial role in the optimization of chromatographic parameters. The chromatographic retention time was optimized by varying concentrations of ion-pair reagent, flow rate<span>, and column temperature to enable good chromatographic retention and sensitivity of disinfection by-product of interest DADMAC in positive electrospray ionization and using selected ion monitoring (SIM) mode. The method was validated and showed good linear regression of 0.99 and a detection limit of 0.008 mg L</span></span></span></span>⁻¹<span>. The developed method was applied in a drinking water treatment plant operated by Mgeni Water in Durban, South Africa, to detect trace levels of the disinfection by-product of interest (DADMAC) at various points of the treatment process. The concentration of DADMAC in the water treatment plant ranged from not detected up to 0.65 mg L</span>⁻¹<span><span>. In addition, this work through mass spectrometry provides the first evidence of ion-pairing (465 m/z peak) between DADMAC and the reagent, which is a confirmation of online derivatization<span>. Also, the use of ion-pair prevented dimerization of DADMAC (286 m/z peak) inside the </span></span>ionization chamber leading to high sensitivity.</span></p></div>","PeriodicalId":338,"journal":{"name":"International Journal of Mass Spectrometry","volume":"496 ","pages":"Article 117186"},"PeriodicalIF":1.8,"publicationDate":"2023-12-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138680143","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Determining protonation site in fentanyl protomers using ion mobility-aligned MS/MS fragmentation","authors":"Ralph Aderorho,&nbsp;Christopher D. Chouinard","doi":"10.1016/j.ijms.2023.117185","DOIUrl":"10.1016/j.ijms.2023.117185","url":null,"abstract":"<div><p><span><span>Drug overdoses<span> in the United States totalled over 100,000 in 2022, with an estimated 68 % of those being attributed to illicitly manufactured fentanyls (IMFs). Their ease and low cost of synthesis have prompted a proliferation of new fentanyl<span> analogues in the illicit drug market, and further created demand for analytical tools capable of identifying these new substances. Ion mobility-mass spectrometry (IM-MS) has emerged as a strong candidate to lead this effort, but the presence of multiple mobility peaks for a single fentanyl compound has created ambiguity in analysis. Herein, we use a combination of IM and tandem </span></span></span>mass spectrometry (MS/MS) and determine that the multiple mobility peaks correspond to protonation site isomers, or ‘protomers’, where protonation can occur at either the N-piperidine ring and N-amide. Unique fragmentation spectra and energy-resolved CID revealed characteristic dissociation pathways for each protomer. Furthermore, this approach was applied to another analogue, despropionyl </span><em>ortho</em>-methylfentanyl, and was subsequently able to annotate its protomers as well. This approach holds tremendous promise for identification of future novel opioids including fentanyl analogues.</p></div>","PeriodicalId":338,"journal":{"name":"International Journal of Mass Spectrometry","volume":"496 ","pages":"Article 117185"},"PeriodicalIF":1.8,"publicationDate":"2023-12-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138630803","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Proteomic analysis of N-glycosylation of the human placenta between preeclampsia and normal pregnancies","authors":"Guangjin Qu ,&nbsp;Qiqi Luo ,&nbsp;Panpan Hu ,&nbsp;Kun Huang ,&nbsp;Feifei Hu ,&nbsp;Mingli Huang ,&nbsp;Shanshun Luo ,&nbsp;Yue Li","doi":"10.1016/j.ijms.2023.117184","DOIUrl":"10.1016/j.ijms.2023.117184","url":null,"abstract":"<div><p>Protein <em>N</em>-glycosylation plays critical roles in modulating placental function, but little is known about <em>N</em><span>-glycoproteins in the human placenta and modifications in preeclampsia (PE). Here, we show a large, site-specific </span><em>N</em>-glycoproteome profiling study of PE and normal placenta using quantitative <em>N</em><span>-glycoproteomics based on mass spectrometry. The study identified disease signatures of altered </span><em>N</em>-glycoproteins and <em>N</em>-glycosylation site occupancy in PE and provided a system-level view of human placental <em>N</em>-glycoproteins and <em>in vivo N</em><span>-glycosylation sites. The study led to the discovery of a roster of glycoproteins with aberrant </span><em>N</em>-glycosylation levels associated with PE, including CD34, ENPP1 (ectonucleotide pyrophosphatase/phosphodiesterase family member 1), insulin-like growth factor binding protein (IGFBP3), and HYOU1 (hypoxia up-regulated 1). An emerging phenomenon that <em>N</em><span>-glycosylation is involved in several PE pathways, including cell adhesion molecules, PI3K-Akt signaling, pyrimidine metabolism, and metabolic pathways was revealed by pathway analysis of PE-associated aberrant glycoproteins. After enzymolysis, the proteins in each group were enriched with </span><em>N</em><span>-glycosylated peptides by lectin, the glycochain was excised by peptide </span><em>N</em>-glycosidase F (PNGase F) in H₂18O, and the glycosylated sites were analyzed by LC-MS/MS to achieve large-scale qualitative and quantitative analysis of <em>N</em>-glycosylated proteins. Our findings highlight the role of <em>N</em>-glycosylation in the pathogenesis of PE and provide new molecular and system-level insights for understanding and treating this disease.</p></div>","PeriodicalId":338,"journal":{"name":"International Journal of Mass Spectrometry","volume":"496 ","pages":"Article 117184"},"PeriodicalIF":1.8,"publicationDate":"2023-12-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138573043","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Resolving metal binding properties within subunits of a multimeric enzyme Mnx by surface induced dissociation and native ion mobility mass spectrometry","authors":"Deseree J. Reid ,&nbsp;Stephanie M. Thibert ,&nbsp;Jesse W. Wilson ,&nbsp;Alexandra V. Soldatova ,&nbsp;Bradley M. Tebo ,&nbsp;Thomas G. Spiro ,&nbsp;Mowei Zhou","doi":"10.1016/j.ijms.2023.117172","DOIUrl":"https://doi.org/10.1016/j.ijms.2023.117172","url":null,"abstract":"<div><p><span><span>Multi-subunit enzymes function as coordinated assemblies. Yet most enzymatic assays measure the summed output of all populations in solution and cannot easily differentiate contributions of individual subunits. Native mass spectrometry detects intact protein complexes in the gas phase. Surface induced dissociation further releases subunits from protein complexes while retaining compact conformations and bound ligands. Combined with </span>ion mobility<span>, the released subunits can then be carefully monitored for more in-depth structural analysis. Mnx is a unique bacterial multicopper oxidase complex that oxidizes Mn(II) to form MnO</span></span>₂<span> minerals, and is composed of three subunits: MnxG, a multicopper oxidase containing the active site, and two accessory proteins, MnxE and MnxF which also bind copper ions<span>. Other known multicopper oxidases do not require accessory proteins, therefore the functions of MnxE and MnxF are not well understood. Here, we use native mass spectrometry with surface induced dissociation and ion mobility to characterize the metal binding properties of Mnx with two metals, catalytic Cu(II) and Mn(II) substrate. We demonstrate our assay can detect subtle structural changes within each subunit, which are presumably related to the allosteric mechanism. We also noticed that ionic strength<span> and solution composition can impact metal binding and must be carefully investigated for such experiments.</span></span></span></p></div>","PeriodicalId":338,"journal":{"name":"International Journal of Mass Spectrometry","volume":"496 ","pages":"Article 117172"},"PeriodicalIF":1.8,"publicationDate":"2023-11-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138472104","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Quality by design optimization and validation of a HPTLC-MS method for simultaneous estimation of paracetamol and prochlorperazine from bulk and formulation","authors":"Shubhangee S. Gaikwad ,&nbsp;Saurabh D. Kalkate ,&nbsp;Amruta A. Bankar ,&nbsp;Amol S. Bansode","doi":"10.1016/j.ijms.2023.117171","DOIUrl":"https://doi.org/10.1016/j.ijms.2023.117171","url":null,"abstract":"<div><p>Study reports that the, stability indicating high-performance thin layer chromatographic technique (HPTLC) was developed as well as validated for estimating Paracetamol and Prochlorperazine in bulk and dosage form. These drugs are largely used in migraine and first line treatment of schizophrenia. Selected drug combination employed for Quality by design based Box Behnken design by high performance thin layer chromatography method utilizing aluminium plates; pre-coated using silica gel 60F₂₅₄ as stationary phase by using acetone: toluene: methanol (4:4:2 v/v/v) as a mobile phase. Densitogram shows R_f values for Paracetamol at 0.74 and for Prochlorperazine at 0.32 evaluated by densitometry measurement bands at 248 nm. Paracetamol and Prochlorperazine marketed formulation of 700 mg by using various excipients prepared at lab scale and it was evaluated for various types of tablet tests, and it showed the accurate result with respect to standard guidelines. The approach has been validated in accordance with International Conference on Harmonization (ICH) requirements. The correlation coefficient was found to be 0.992 and 0.998 at a concentration range of 100–300 μg/band and 1000–3000 ng/band for Paracetamol and Prochlorperazine, respectively. The method had an accuracy of 100.51 % and 100.53 % for Paracetamol and Prochlorperazine, respectively. The degradation of Paracetamol and Prochlorperazine was carried out in an acid, alkaline, oxidative, thermal and photolytic environment. The stress degraded product was successfully separated using the HPTLC and using high resonance mass spectroscopy technique (HRMS-MS), the degradation product was discovered.</p></div>","PeriodicalId":338,"journal":{"name":"International Journal of Mass Spectrometry","volume":"495 ","pages":"Article 117171"},"PeriodicalIF":1.8,"publicationDate":"2023-11-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.sciencedirect.com/science/article/pii/S1387380623001628/pdfft?md5=b55cb2e55bba70eeb28efbc1fec92e6f&pid=1-s2.0-S1387380623001628-main.pdf","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138413382","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

{"title":"Surface-induced dissociation of protein complex ions in a modified electrostatic linear ion trap","authors":"Ian J. Carrick,&nbsp;Joshua T. Johnson,&nbsp;Scott A. McLuckey","doi":"10.1016/j.ijms.2023.117170","DOIUrl":"https://doi.org/10.1016/j.ijms.2023.117170","url":null,"abstract":"<div><p><span><span>The electrostatic linear </span>ion trap<span> (ELIT) is a device that can provide mass analysis via frequency measurement, followed by Fourier transformation<span> from the frequency domain to the time domain, or via time measurement in a multi-reflection time-of-flight measurement. ELIT devices have been demonstrated to be capable of relatively high mass measurement resolution as well as high-resolution ion isolation capabilities. We have been exploring the possibility of developing the ELIT geometry as a stand-alone high-performance tandem mass spectrometer for native </span></span></span>mass spectrometry (MS) studies. In this context, it is desirable to use an activation method capable of dissociating the high-mass complexes encountered in native MS. To this end, we describe the implementation of surface-induced dissociation (SID) in an ELIT and describe initial results for protein complexes generated under native conditions in which ion isolation, fragmentation, and product ion mass analysis all occur within the ELIT.</p></div>","PeriodicalId":338,"journal":{"name":"International Journal of Mass Spectrometry","volume":"496 ","pages":"Article 117170"},"PeriodicalIF":1.8,"publicationDate":"2023-11-19","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"138472103","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":3,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}