“…Compared to the nSi‐based LDI‐TOF MS, the AuNPs‐nSi‐based LDI‐TOF MS exhibited less matrix‐related interference and higher signal to noise ratio, indicating that Au NPs plays an important role in enhancement of D/I efficiency. Gan et al reported a novel platform using optimized SiO 2 @Au core‐shell structure as matrix for highly efficient LDI‐TOF MS analysis of small biomolecules in both positive‐ and negative‐ion mode. Different from the positive ion mode, the negative ion mode affords exclusively deprotonated ions in the analysis of phenylalanine, mannitol, glutamic acid, and glycose with clean background and high sensitivity.…”
Section: Nanostructured Substrates For Negative Ion Ldi‐tof Msmentioning
Matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF MS) is an excellent analytical technique for rapid and sensitive analysis of macromolecules such as polymers and proteins. However, the main drawback of MALDI-TOF MS is its difficulty to detect small molecules with mass below 700 Da because of the intensive interference from MALDI matrix in the low mass region. In recent years there has been considerable interest in developing matrix-free laser desorption/ionization by using nanostructured substrates to substitute the conventional organic matrices, which is often referred as surface-assisted laser desorption/ionization time-of-flight mass spectrometry (SALDI-TOF MS). Despite these attractive features, most of the current SALDI-TOF MS for the analysis of small molecules employ positive ion mode, which is subjected to produce multiple alkali metal adducts, and thus increases the complexity of the analysis. Different from the complicated adducts produced in positive ion mode, mass spectra obtained in negative ion mode are featured by deprotonated ion peaks without matrix interference, which simplifies the interpretation of mass spectra and detection of unknown. In this review, we critically survey recent advances in nanostructured substrates for negative ion LDI-TOF MS analysis of small molecules in the last 5 years. Special emphasis is placed on the preparation of the nanostructured substrates and the results achieved in negative ion SALDI-MS. In addition, a variety of promising applications including environmental, biological, and clinical analysis are introduced. The ionization mechanism of negative ionization is briefly discussed.
“…Compared to the nSi‐based LDI‐TOF MS, the AuNPs‐nSi‐based LDI‐TOF MS exhibited less matrix‐related interference and higher signal to noise ratio, indicating that Au NPs plays an important role in enhancement of D/I efficiency. Gan et al reported a novel platform using optimized SiO 2 @Au core‐shell structure as matrix for highly efficient LDI‐TOF MS analysis of small biomolecules in both positive‐ and negative‐ion mode. Different from the positive ion mode, the negative ion mode affords exclusively deprotonated ions in the analysis of phenylalanine, mannitol, glutamic acid, and glycose with clean background and high sensitivity.…”
Section: Nanostructured Substrates For Negative Ion Ldi‐tof Msmentioning
Matrix-assisted laser desorption/ionization time-of-flight mass spectrometry (MALDI-TOF MS) is an excellent analytical technique for rapid and sensitive analysis of macromolecules such as polymers and proteins. However, the main drawback of MALDI-TOF MS is its difficulty to detect small molecules with mass below 700 Da because of the intensive interference from MALDI matrix in the low mass region. In recent years there has been considerable interest in developing matrix-free laser desorption/ionization by using nanostructured substrates to substitute the conventional organic matrices, which is often referred as surface-assisted laser desorption/ionization time-of-flight mass spectrometry (SALDI-TOF MS). Despite these attractive features, most of the current SALDI-TOF MS for the analysis of small molecules employ positive ion mode, which is subjected to produce multiple alkali metal adducts, and thus increases the complexity of the analysis. Different from the complicated adducts produced in positive ion mode, mass spectra obtained in negative ion mode are featured by deprotonated ion peaks without matrix interference, which simplifies the interpretation of mass spectra and detection of unknown. In this review, we critically survey recent advances in nanostructured substrates for negative ion LDI-TOF MS analysis of small molecules in the last 5 years. Special emphasis is placed on the preparation of the nanostructured substrates and the results achieved in negative ion SALDI-MS. In addition, a variety of promising applications including environmental, biological, and clinical analysis are introduced. The ionization mechanism of negative ionization is briefly discussed.
“…A subsequent 10 min reduction in an overnight-aged mixture of HAuCl 4 (3 mL, 1%) and K 2 CO 3 (100 mL, 3.6 mM) in the presence of formaldehyde (5 mL) resulted in a continuous Au shell on the silica surface. The nanoparticles were centrifuged after reaction and re-dispersed in water to form a stable suspension [18,43]. The averaged dimension of obtained Au nanoshells was a 100 nm core in diameter and a 33 nm Au shell in thickness (an outer diameter of 166 nm).…”
Section: Synthesis Of Npsmentioning
confidence: 99%
“…>108 mol À1 cm À1 at 518 nm for 14 nm Au NPs); (3) cost-friendly and facile preparation method for large scale application; (4) mature surface modification protocol based on the gold-thiol (AueS) interaction for capturing analytes [20]. Even though different types of metallic plasmonic particles have been developed with promising detection limits of analytes (~nmol-pmol) for LDI MS [18,21], their working mechanism is yet to be explored limiting their application with real case biological samples.…”
Section: Introductionmentioning
confidence: 99%
“…Nd:YAG laser at 355 nm) [20] while plasmon resonances of Au NPs typically locate in the visible-near infrared (NIR) range. Previously we have employed Au nanoshells for LDI MS detection of standard small molecules [18], but the enhancing mechanism has not been investigated regarding the surface plasmon resonance. In this work, we report the generation of hot carriers in plasmonic Au nanoshells for the enhanced LDI MS detection of amino acids in serum (Scheme 1).…”
“…Au@SiO 2 CSNPs with a smaller gold core (about 18 nm) and ultrathin silica shell (2~4 nm) exhibited the best efficiency including a better signal to noise ratio and signal intensity. SiO 2 @Au core-shell nanomaterials were applied for the analysis of small biomolecules including glucose, cellobiose, phenylalanine, glutamic acid, mannitol and adenosine [97]. By further surface modification with aptamers, Apt-SiO 2 @Au nanoshells allowed simultaneously targeted enrichment and detection of kanamycin with a detection limit at 200 pM.…”
Section: Nanomaterial-assisted Ldi For the Analysis Of Small Biolomentioning
Matrix-assisted laser desorption/ionization (MALDI), a soft ionization method, coupling with time-of-flight mass spectrometry (TOF MS) has become an indispensible tool for analyzing macromolecules, such as peptides, proteins, nucleic acids and polymers. However, the application of MALDI for the analysis of small molecules (<700 Da) has become the great challenge because of the interference from the conventional matrix in low mass region. To overcome this drawback, more attention has been paid to explore interference-free methods in the past decade. The technique of applying nanomaterials as matrix of laser desorption/ionization (LDI), also called nanomaterial-assisted laser desorption/ionization (nanomaterial-assisted LDI), has attracted considerable attention in the analysis of low-molecular weight compounds in TOF MS. This review mainly summarized the applications of different types of nanomaterials including carbon-based, metal-based and metal-organic frameworks as assisted matrices for LDI in the analysis of small biological molecules, environmental pollutants and other low-molecular weight compounds.
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