MALDI Matrices for Biomolecular Analysis Based on Functionalized Carbon Nanomaterials

Ugarov, M. V.; Egan, Thomas F.; Khabashesku, Dmitry V.; Schultz, J.; Peng, Haowei; Khabashesku, Valéry N.; Furutani, Hiroshi; Prather, Kimberly A.; Wang, H.-W. J.; Jackson, Shelley N.; Woods, Amina S.

doi:10.1021/ac049192x

Cited by 97 publications

(88 citation statements)

References 22 publications

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“…Taking into account the results from this research, we could conclude that the attempt of using fullerene as a possible matrix for MALDI screening of anthocyanins should be extended on testing the effect of derivatized and/or acidified fullerenes as possible matrices, since those matrices require lower laser power for ionization. Furthermore, the fullerene derivatives, as a new class of matrices, possesses high analyte ionization efficiency, small molar ratios (less than 1) of matrix/analyte and a broader optical absorption spectrum, which should obviate specific wavelength lasers for MALDI acquisitions (Ugarov et al 2004) and could be used for MALDI screening of anthocyanins. Thus, further investigations are necessary to be performed in order to allow proper identification of grape and wine anthocyanins (glycosides, acetyl, and pcoumaroyl derivatives) applying the new MALDI matrices.…”

Section: Resultsmentioning

confidence: 99%

Rapid MALDI-TOF-MS Detection of Anthocyanins in Wine and Grape Using Different Matrices

et al. 2010

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Matrix-assisted laser desorption/ionization timeof-flight mass spectrometry (MALDI-TOF-MS) as a new valuable technique has been used for qualitative screening of anthocyanins in wine and grape samples from Vranec and Merlot variety. For that purpose, different MALDI matrices have been tested, such as α-cyano-4-hydroxycinnamic acid, sinapic acid, 2,5-dihydroxybenzoic acid (2,5-DHB), and C 70 fullerene. It was observed that 2,5-DHB was superior with respect to all the matrices used in the study. Furthermore, fullerene was, for the first time, tested and used as a possible matrix for MALDI-TOF-MS identification of anthocyanins in wine and grape samples. The results obtained showed identification of aglycone forms of anthocyanins only, since the higher laser energy applied for ionization of the fullerene molecules led to great deal of fragmentation of the sugar moiety from glucosides, acetylglucoside, and p-coumaroylglucoside groups from the corresponding anthocyanin molecules. Additionally, liquid chromatography/electrospray ionization mass spectrometry has also been applied for anthocyanin characterization.

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Section: Resultsmentioning

confidence: 99%

Rapid MALDI-TOF-MS Detection of Anthocyanins in Wine and Grape Using Different Matrices

et al. 2010

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“…Although the Au NPs were selective and efficient nanomaterials for glutathione, they were not useful for the analysis of analytes having values of m/z greater than 1300. When using the Se NPs, TiO 2 NPs, and CdTe QDs for SALDI-MS analyses, the mass range reached as high as the mass of cytochrome c. The SALDI-MS approach allowed the detection of chymotrypsin by using the Pt NSPs and Fe 3 4 NPs and CdTe QDs in the analysis of insulin, we detected adducts of Fe and Cd, respectively. Presumably, the formation of metal-analyte adducts was due to strong interactions between the Fe 3ϩ /Cd 2ϩ ions and the proteins through metal-ligand (carboxylate and amino) coordination [9].…”

Section: Methodsmentioning

confidence: 95%

“…We detected multiply charged ions for cytochrome c, trypsinogen, and chymotrypsin when using the Fe 3 O 4 NPs for SALDI-MS analyses. In our experiments, NH 4 ϩ ions acted as the main proton donors during the desorption and ionization processes. Notably, we had prepared the Fe 3 O 4 NPs from an ammonia solution under basic conditions.…”

Section: Methodsmentioning

confidence: 97%

“…In our experiments, NH 4 ϩ ions acted as the main proton donors during the desorption and ionization processes. Notably, we had prepared the Fe 3 O 4 NPs from an ammonia solution under basic conditions. We observed similar results when analyzing cytochrome c using the TiO 2 NPs as the added nanomate- rial; notably, the TiO 2 NPs had been prepared under acidic conditions.…”

Section: Methodsmentioning

confidence: 97%

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Nanomaterial-based surface-assisted laser desorption/ionization mass spectrometry of peptides and proteins

Chiang

Lin

et al. 2010

J. Am. Soc. Mass Spectrom.

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We have investigated six nanomaterials for their applicability as surfaces for the analyses of peptides and proteins using surface-assisted laser desorption/ionization mass spectrometry (SALDI-MS). Gold nanoparticles (NPs) were useful nanomaterials for small analytes (e.g., glutathione); Pt nanosponges and Fe 3 O 4 NPs were efficient nanomaterials for proteins, with an upper detectable mass limit of ca. 25 kDa. Nanomaterials have several advantages over organic matrices, including lower limits of detection for small analytes and lower batch-to-batch variations (fewer problems associated with "sweet spots"), when used in laser desorption/ionization mass spectrometry. (J Am Soc Mass Spectrom 2010, 21, 1204 -1207) © 2010 American Society for Mass Spectrometry S urface-assisted laser desorption/ionization mass spectrometry (SALDI-MS) was developed recently using nanomaterials rather than organic compounds as matrices, for the determination of analytes of interest. For example, laser desorption/ionization (LDI) of intact proteins and protein aggregates in the presence of glycerol has been demonstrated using cobalt particles (ca. 30 nm) [1]. Similar to the role played by organic matrices, the particles absorb energy from the laser irradiation and transfer it efficiently to the analytes, thereby inducing desorption and ionization. Mixtures of graphite particles (2-150 m) and glycerol have been employed in the analysis of proteins and peptides [2,3]. Several other nanomaterials, including carbon nanotubes, nanodiamonds, and various nanoparticles (NPs, namely SiO 2 , ZnS, TiO 2 , Fe 3 O 4 , Fe 3 O 4 /TiO 2 , and Au) are also useful-without the addition of glycerol-for SALDI-MS [4 -12]. Because of their unique chemical and physical properties, NPs can also act as selective probes and/or efficient ionization nanomaterials. For example, Au and TiO 2 NPs are suitable for the concentration and ionization of aminothiols and catechins, respectively, in SALDI-MS [8,11]. One other advantage of using NPs is that fewer "sweet spots" are formed, thereby maximizing reproducibility. Although NPs have been used successfully for the determination of a range of analytes (from small analytes to proteins), a review of the literature reveals that the various NPs provide quite different results in terms of sensitivity, reproducibility, and mass range. Thus, our aim in this study was to evaluate the performance of several types of NPs for the analysis of peptides and proteins. ExperimentalSix nanomaterials-Au NPs, TiO 2 NPs, Se NPs, CdTe quantum dots (QDs), Fe 3 O 4 NPs, and Pt nanosponges (NSPs)-were tested for the SALDI-MS-based analyses of peptides and proteins; they were prepared in aqueous solutions and characterized according to procedures described in the literature [8,11,[13][14][15][16]. A twolayer preparation method was applied to deposit the nanomaterials and samples onto the metal plates used in SALDI-MS. First, one of the nanomaterial solutions (1 L) was deposited into one of the wells of the MS plate and dried under ambient cond...

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“…This desorption/ionization on porous silicon (DIOS) mass spectrometry [10] allows the analysis of various compounds, such as small organic molecules [11], amino acids [12], peptides [13], and fatty acids [14]. More recently, other research groups achieved direct desorption/ionization from carbon nanotubes [15], fullerenes [16], Au clusters [17], silicon nanopowder [18], and porous alumina [19]. These LDI methods, sometimes referred to as "matrix-free", produce mass spectra that exhibit less matrix ions in the low mass range compared with the chemical noise generated by the organic matrices used in matrix-assisted laser desorption/ionization (MALDI) mass spectrometry.…”

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confidence: 99%

Laser desorption/ionization mass spectrometry on porous silica and alumina for peptide mass fingerprinting

Shenar

Martinez

Enjalbal

2008

J. Am. Soc. Mass Spectrom.

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We investigated a variant of desorption/ionization on porous silicon (DIOS) mass spectrometry utilizing an aqueous suspension of either porous silica gel or porous alumina (pore size of 60 and 90 Å, respectively). Laser desorption/ionization (LDI) from samples directly deposited on a stainless steel surface without any inorganic substrates was also achieved. Synthetic peptides designed to cover large sequence diversity constituted our model compounds. Sample preparation, including material conditioning, peptide solubilization, and deposition protocol onto standard matrix-assisted laser desorption/ionization (MALDI) probe, as well as ionization source tuning were optimized to perform sensitive reproducible LDI analyses. The addition of either a cationizing agent or an alkali metal scavenger to the sample suspension allowed modification of the ionization output. Comparing hydrophilic silica gel to hydrophobic reversed-phase silica gel as well as increasing material pore size provided further insights into desorption/ionization processes. Furthermore, mixtures of peptides were analyzed to probe the spectral suppression phenomenon when no interfering organic matrix was present. The results gathered from synthetic peptide cocktails indicated that LDI mass spectrometry on silica gel or alumina constitutes a promising complementary method to MALDI in proteomics for peptide mass fingerprinting. [19]. These LDI methods, sometimes referred to as "matrix-free", produce mass spectra that exhibit less matrix ions in the low mass range compared with the chemical noise generated by the organic matrices used in matrix-assisted laser desorption/ionization (MALDI) mass spectrometry. Such chemical noise that usually pollutes the low mass range of MALDI mass spectra and that may complicate the detection of small molecules is less pronounced in the DIOS mass spectra.Nevertheless, the drawback of such an approach is in the preparation of the silicon material. To present adequate physical properties [20], silicon surfaces are conditioned via a galvanostatic etching procedure from Si wafer to produce pores with nanometer diameters. Commercially available ready-to-use DIOS-chips can also be mounted on modified MALDI plates [20]. Otherwise, silicon powders (5 to 50 nm particle size) were investigated as a substitute to DIOS chips to make the overall sample preparation simpler and safer [18]. Provided that the appropriate powder preparation was performed (including particle etching by HF, oxidation by HNO 3 , and derivatization of the generated SiOH groups), such silicon nanopowder method was found to exhibit the same characteristics as DIOS mass spectrometry.Porous silicon is a material that presents (1) a large active surface and (2) a strong absorbance in the UV range. Such a form of silicon was thus found particularly suitable for LDI mass spectrometry with irradiation at 337 nm, the pore size and the surface chemical nature being the most important parameters as stated by Siuzdak and coworkers in their early publications on DIOS [20...

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MALDI Matrices for Biomolecular Analysis Based on Functionalized Carbon Nanomaterials

Cited by 97 publications

References 22 publications

Rapid MALDI-TOF-MS Detection of Anthocyanins in Wine and Grape Using Different Matrices

Rapid MALDI-TOF-MS Detection of Anthocyanins in Wine and Grape Using Different Matrices

Nanomaterial-based surface-assisted laser desorption/ionization mass spectrometry of peptides and proteins

Laser desorption/ionization mass spectrometry on porous silica and alumina for peptide mass fingerprinting

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