Ion Mobility Spectrometry Characterization of the Intermediate Hydrogen-Containing Gold Cluster Au7(PPh3)7H52+

Ligare, Marshall R.; Morrison, Kelsey A.; Hewitt, Michael A.; Reveles, J. Ulises; Govind, Niranjan; Hernández, Heriberto; Baker, Erin; Clowers, Brian H.; Laskin, Julia; Johnson, Grant E.

doi:10.1021/acs.jpclett.0c03664

Cited by 12 publications

(14 citation statements)

References 64 publications

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“…The proposed structure consists of three bridging Au–H–Au and two single‐bonded Au–H motifs. [ 291 ] The experimental CCS value (421) matches spectacularly well with the theoretically derived value (422). By comparing the CCS values, it is feasible to identify the presence of different isomers/structures and track the structural transformation within the IM‐MS experiment.…”

Section: Characterization Of Au Clusterssupporting

confidence: 76%

A Review of State of the Art in Phosphine Ligated Gold Clusters and Application in Catalysis

et al. 2022

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Atomically precise gold clusters are highly desirable due to their well-defined structure which allows the study of structure-property relationships. In addition, they have potential in technological applications such as nanoscale catalysis. The structural, chemical, electronic, and optical properties of ligated gold clusters are strongly defined by the metal-ligand interaction and type of ligands. This critical feature renders gold-phosphine clusters unique and distinct from other ligand-protected gold clusters. The use of multidentate phosphines enables preparation of varying core sizes and exotic structures beyond regular polyhedrons. Weak gold-phosphorous (Au-P) bonding is advantageous for ligand exchange and removal for specific applications, such as catalysis, without agglomeration. The aim of this review is to provide a unified view of gold-phosphine clusters and to present an in-depth discussion on recent advances and key developments for these clusters. This review features the unique chemistry, structural, electronic, and optical properties of gold-phosphine clusters. Advanced characterization techniques, including synchrotron-based spectroscopy, have unraveled substantial effects of Au-P interaction on the composition-, structure-, and size-dependent properties. State-of-the-art theoretical calculations that reveal insights into experimental findings are also discussed. Finally, a discussion of the application of gold-phosphine clusters in catalysis is presented.

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Section: Characterization Of Au Clusterssupporting

confidence: 76%

A Review of State of the Art in Phosphine Ligated Gold Clusters and Application in Catalysis

et al. 2022

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“…Cyclooctaglycine [46] and Au6 cluster [47] were used for cyclic peptide (CP) and gold nanoparticles (GN) modelling, respectively. The different configurations of small Au clusters with 3 to 20 atoms are well known due to numerous experimental and theoretical studies [48][49][50][51][52][53]. The interaction of gold nanoparticles -cyclic peptide (CPGN) with 5-fluorouracil (FU) was investigated from seven different directions.…”

Section: Resultsmentioning

confidence: 99%

Structural and energetic analysis of cyclic peptide-gold nano-drug delivery system: a DFT study

Khoshbayan¹,

Morsali²,

Bozorgmehr³

et al. 2021

Nanosystems: Phys. Chem. Math.

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“…After the MS inlet, the ions were focused by the high-pressure ion funnel and accumulated into the lower-pressure trapping ion funnel. 92 The ions were then pulsed into the N 2 -filled drift tube (3.9 ± 2.0 Torr) under the influence of an applied electric field and were subsequently separated according to their drift time in an inert N 2 gas. The maximum drift time in these experiments was set to 70 ms with a 40 ms ion funnel trap time and a 0.2 ms release time.…”

Section: ■ Experimental Methodologymentioning

confidence: 99%

Molecular and Structural Characterization of Isomeric Compounds in Atmospheric Organic Aerosol Using Ion Mobility-Mass Spectrometry

et al. 2023

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Secondary organic aerosol (SOA) formed through multiphase atmospheric chemistry makes up a large fraction of airborne particles. The chemical composition and molecular structures of SOA constituents vary between different emission sources and aging processes in the atmosphere, which complicates their identification. In this work, we employ drift tube ion mobility spectrometry with quadrupole time-of-flight mass spectrometry (IM-MS) detection for rapid gas-phase separation and multidimensional characterization of isomers in two biogenic SOAs produced from ozonolysis of isomeric monoterpenes, d-limonene (LSOA) and α-pinene (PSOA). SOA samples were ionized using electrospray ionization (ESI) and characterized using IM-MS in both positive and negative ionization modes. The IM-derived collision cross sections in nitrogen gas (DTCCSN2 ) for individual SOA components were obtained using multifield and single-field measurements. A novel application of IM multiplexing/high-resolution demultiplexing methodology was employed to increase sensitivity, improve peak shapes, and augment mobility baseline resolution, which revealed several isomeric structures for the measured ions. For LSOA and PSOA samples, we report significant structural differences of the isomer structures. Molecular structural calculations using density functional theory combined with the theoretical modeling of CCS values provide insights into the structural differences between LSOA and PSOA constituents. The average DTCCSN2 values for monomeric SOA components observed as [M + Na]+ ions are 3–6% higher than those of their [M – H]− counterparts. Meanwhile, dimeric and trimeric isomer components in both samples showed an inverse trend with the relevant values of [M – H]− ions being 3–7% higher than their [M + Na]+ counterparts, respectively. The results indicate that the structures of Na+-coordinated oligomeric ions are more compact than those of the corresponding deprotonated species. The coordination with Na+ occurs on the oxygen atoms of the carbonyl groups leading to a compact configuration. Meanwhile, deprotonated molecules have higher DTCCSN2 values due to their elongated structures in the gas phase. Therefore, DTCCSN2 values of isomers in SOA mixtures depend strongly on the mode of ionization in ESI. Additionally, PSOA monomers and dimers exhibit larger DTCCSN2 values (1–4%) than their LSOA counterparts owing to more rigid structures. A cyclobutane ring is present with functional groups pointing in opposite directions in PSOA compounds, as compared to noncyclic flexible LSOA structures, forming more compact ions in the gas phase. Lastly, we investigated the effects of direct photolysis on the chemical transformations of selected individual PSOA components. We use IM-MS to reveal structural changes associated with aerosol aging by photolysis. This study illustrates the detailed molecular and structural descriptors for the detection and annotation of structural isomers in complex SOA mixtures.

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Ion Mobility Spectrometry Characterization of the Intermediate Hydrogen-Containing Gold Cluster Au₇(PPh₃)₇H₅²⁺

Cited by 12 publications

References 64 publications

A Review of State of the Art in Phosphine Ligated Gold Clusters and Application in Catalysis

A Review of State of the Art in Phosphine Ligated Gold Clusters and Application in Catalysis

Structural and energetic analysis of cyclic peptide-gold nano-drug delivery system: a DFT study

Molecular and Structural Characterization of Isomeric Compounds in Atmospheric Organic Aerosol Using Ion Mobility-Mass Spectrometry

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