“…Figure S2 demonstrates the mass spectra of BSA and BSA-AuNCs with different incubation times; all of the characterizations were performed on an electrospray ionization mass spectrometry (ESI-MS). The background signals from precursors of BSA and HAuCl 4 as well as AuNCs composed of a few Au atoms gradually decreased along with prolonged incubation time and were eventually removed with the BSA-AuNCs, which were prepared with an incubation time of 24 h. These data provided convincing evidence that both Au(0) content and particle size of BSA-AuNCs increased with prolonged incubation time. − The phase structures of the BSA and BSA-AuNCs with different incubation times are characterized by X-ray diffraction (XRD) and Fourier transform infrared (FTIR) spectroscopy. According to Figure S3A, XRD patterns for BSA and the BSA-AuNCs with an incubation time of 6, 10, 12, and 24 h fail to exhibit obvious diffraction peaks related to normal AuNCs.…”
To determine the intrinsic effects of body elements on the electrochemiluminescence (ECL) of metal nanoclusters (NCs), herein, a valence-state engineering strategy is developed to adjust the NCs' ECL with bovine serum albumin (BSA)-stabilized AuNCs as a model, in which engineering the valence state of the Au body element, i.e., Au(0) and Au(I), is performed via successively reducing the precursor AuCl 4 − to Au(I) and Au(0) with BSA. The obtained BSA-AuNCs/N 2 H 4 system leads to three anodic ECL processes at 0.37 (ECL-1), 0.85 (ECL-2), and 1.45 V (ECL-3). ECL-1 is generated from the BSA-Au(0) section of BSA-AuNCs in a surface-defect-involved route and is much stronger and redshifted compared to ECL-2 and ECL-3, which are generated from the BSA-Au(I) section of BSA-AuNCs in the band-gapengineered route. Each of the anodic ECL processes can be selectively generated and/or suppressed via adjusting the Au(I)/ Au(0) ratio of BSA-AuNCs, tunable ECL generation route, and triggering potential, and the emission intensity and waveband of metal NCs are conveniently achieved in body-element-involved valence-state engineering.
“…Figure S2 demonstrates the mass spectra of BSA and BSA-AuNCs with different incubation times; all of the characterizations were performed on an electrospray ionization mass spectrometry (ESI-MS). The background signals from precursors of BSA and HAuCl 4 as well as AuNCs composed of a few Au atoms gradually decreased along with prolonged incubation time and were eventually removed with the BSA-AuNCs, which were prepared with an incubation time of 24 h. These data provided convincing evidence that both Au(0) content and particle size of BSA-AuNCs increased with prolonged incubation time. − The phase structures of the BSA and BSA-AuNCs with different incubation times are characterized by X-ray diffraction (XRD) and Fourier transform infrared (FTIR) spectroscopy. According to Figure S3A, XRD patterns for BSA and the BSA-AuNCs with an incubation time of 6, 10, 12, and 24 h fail to exhibit obvious diffraction peaks related to normal AuNCs.…”
To determine the intrinsic effects of body elements on the electrochemiluminescence (ECL) of metal nanoclusters (NCs), herein, a valence-state engineering strategy is developed to adjust the NCs' ECL with bovine serum albumin (BSA)-stabilized AuNCs as a model, in which engineering the valence state of the Au body element, i.e., Au(0) and Au(I), is performed via successively reducing the precursor AuCl 4 − to Au(I) and Au(0) with BSA. The obtained BSA-AuNCs/N 2 H 4 system leads to three anodic ECL processes at 0.37 (ECL-1), 0.85 (ECL-2), and 1.45 V (ECL-3). ECL-1 is generated from the BSA-Au(0) section of BSA-AuNCs in a surface-defect-involved route and is much stronger and redshifted compared to ECL-2 and ECL-3, which are generated from the BSA-Au(I) section of BSA-AuNCs in the band-gapengineered route. Each of the anodic ECL processes can be selectively generated and/or suppressed via adjusting the Au(I)/ Au(0) ratio of BSA-AuNCs, tunable ECL generation route, and triggering potential, and the emission intensity and waveband of metal NCs are conveniently achieved in body-element-involved valence-state engineering.
“…After the use of gel-based or gel-free methods to sufficiently reduce sample complexities, the peptides are mixed and analyzed using mass spectroscopy. In proteomic studies, the most used ionization methods are electrospray ionization (ESI) ( Chen et al, 2017 ) and matrix-assisted laser desorption/ionization (MALDI) ( Kailasa et al, 2020 ). However, electrospray ionization is employed more due to its high-throughput secondary spectra of peptides.…”
“…A commercial open ambient nanospray source (Thermo) and an enclosed electrospray source (CEESI, Haochuang, China) − were utilized in MS experiments, respectively. Electrospray voltage between the spray tip and the MS interface was 2.0 kV, the temperature of ion transfer capillary was 250 °C, the max inject time was 100 ms, microscans 1 and the MS1 resolution was 30 000 (at m / z = 400).…”
There are two challenges in oligonucleotide detection by liquid chromatography coupled with mass spectrometry (LC-MS), the serious ion suppression effects caused by ion-pair reagents and the low detection sensitivity in positive mode MS. In this study, highly concentrated alcohol vapors were introduced into an enclosed electrospray ionization chamber, and oligonucleotides could be well detected in negative mode MS even with 100 mM triethylammonium acetate (TEAA) as an ion-pair reagent. The MS signal intensity was improved 600-fold (for standard oligonucleotide dT15) by the isopropanol vapor assisted electrospray, and effective ion-pair LC separation was feasibly coupled with high-sensitive MS detection. Then, oligonucleotides were successfully detected in positive mode MS with few adducts by propanoic acid vapor assisted electrospray. The signal intensity was enhanced more than 10-fold on average compared with adding acids into the electrospray solution. Finally, oligonucleotides and peptides or histones were simultaneously detected in MS with little interference with each other. Our strategy provides a useful alternative for investigating the biological functions of oligonucleotides.
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