Soft-landing preparative mass spectrometry

Verbeck, Guido F.; Hoffmann, William D.; Walton, Barbara L.

doi:10.1039/c2an35550g

Cited by 71 publications

(81 citation statements)

References 134 publications

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“…Combined with depth profiling capabilities, this technique may be used in the future for 3D chemical imaging of individual particles on substrates. Although images of individual particles deposited on the substrates may be affected by transformations of particle morphologies upon sample collection, these effects can be minimised by gentle deposition of charged particles using ion soft landing [214][215][216] that can be further developed for particle deposition. Alternatively, the advent of novel coherent light source facilities based on X-ray free electron laser technology has opened up an additional unique opportunity for on-the-fly imaging and mass spectrometric characterisation of individual particles [217].…”

Section: Discussionmentioning

confidence: 99%

New mass spectrometry techniques for studying physical chemistry of atmospheric heterogeneous processes

Laskin

Nizkorodov

2013

International Reviews in Physical Chemistry

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Ambient particles and droplets have a significant effect on climate, visibility and human health. Once formed, they undergo continuous transformations through condensation and evaporation of water, uptake of low-volatility organic molecules and photochemical reactions involving various gaseous and condensed-phase species in the atmosphere. These transformations determine the physical and chemical properties of airborne particles, such as their ability to absorb and scatter solar radiation and nucleate cloud droplets. The complexity, heterogeneity and size of ambient particles make it challenging to understand the kinetics and mechanisms of their formation and chemical transformations. Mass spectrometry (MS) is a powerful analytical technique that enables detailed chemical characterisation of both small and large molecules in complex matrices. This capability makes MS a promising tool for studying chemical transformations of particles and droplets in the atmosphere. This review is focused on new and emerging experimental MS-based approaches for understanding the kinetics and mechanisms of such transformations. Some of the techniques discussed herein are best suited for ambient samples, while the others work best in laboratory applications. However, in combination, they provide a comprehensive arsenal of methods for characterisation of particles and droplets. In addition, we emphasise the role of fundamental physical chemistry studies in the development of new methods for chemical analysis of ambient particles and droplets.

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Section: Discussionmentioning

confidence: 99%

New mass spectrometry techniques for studying physical chemistry of atmospheric heterogeneous processes

Laskin

Nizkorodov

2013

International Reviews in Physical Chemistry

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“…In this study, we report the development of a unique approach that enables in situ electrochemical characterization of ions on a nanostructured solid-state EEI precisely designed using soft-landing (SL) of mass-and charge-selected ions (6)(7)(8)(9)(10)(11)(12). Previously, the superior performance of EEIs prepared using SL in comparison with drop casting and electrospray deposition was demonstrated (13).…”

mentioning

confidence: 99%

In situ solid-state electrochemistry of mass-selected ions at well-defined electrode–electrolyte interfaces

Prabhakaran

Johnson

Wang

et al. 2016

Proc. Natl. Acad. Sci. U.S.A.

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Molecular-level understanding of electrochemical processes occurring at electrode-electrolyte interfaces (EEIs) is key to the rational development of high-performance and sustainable electrochemical technologies. This article reports the development and application of solid-state in situ thin-film electrochemical cells to explore redox and catalytic processes occurring at well-defined EEIs generated using soft-landing (SL) of mass-and charge-selected cluster ions. In situ cells with excellent mass-transfer properties are fabricated using carefully designed nanoporous ionic liquid membranes. SL enables deposition of pure active species that are not obtainable with other techniques onto electrode surfaces with precise control over charge state, composition, and kinetic energy. SL is, therefore, demonstrated to be a unique tool for studying fundamental processes occurring at EEIs. Using an aprotic cell, the effect of charge state ) and the contribution of building blocks of Keggin polyoxometalate (POM) clusters to redox processes are characterized by populating EEIs with POM anions generated by electrospray ionization and gasphase dissociation. Additionally, a proton-conducting cell has been developed to characterize the oxygen reduction activity of bare Pt clusters (Pt 30 ∼1 nm diameter), thus demonstrating the capability of the cell for probing catalytic reactions in controlled gaseous environments. By combining the developed in situ electrochemical cell with ion SL we established a versatile method to characterize the EEI in solid-state redox systems and reactive electrochemistry at precisely defined conditions. This capability will advance the molecular-level understanding of processes occurring at EEIs that are critical to many energy-related technologies.in situ electrochemistry | electrode-electrolyte interface | ion soft-landing | ionic liquid membrane | clusters U nderstanding the intrinsic properties of electroactive species on electrode surfaces is critical to the rational design of stable and efficient electrode-electrolyte interfaces (EEIs) in numerous technologically important solid-state electrochemical systems (1, 2). Performance degradation and instability of electrochemical systems mostly stems from undesired side reactions occurring at EEIs (3). Agglomeration and decomposition of redox-active species in supercapacitors, evolution of resistive lithium metal dendrites at the solid-electrolyte interphase in batteries, and dissolution and Ostwald ripening of oxygen reduction reaction (ORR) catalysts such as supported Pt clusters and nanoparticles (NPs) in polymer electrolyte membrane fuel cell (PEMFC) electrodes, are just a few examples of common undesirable processes occurring at EEI that require detailed in situ characterization (3). A fundamental understanding of molecular mechanisms and electrode kinetics is key to the future improvement of the performance of EEIs and the longevity and commercial success of electrochemical technologies. The distribution and adsorption/desorption of counterions o...

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“…Soft landing of mass-selected ions onto surfaces remains a subject of current research interest due to the demonstrated capabilities of the technique for the highly-controlled preparation of novel materials [1][2][3][4][5][6] . Recent efforts have indicated potential future applications of soft landing of mass-selected ions in the preparation of peptide and protein arrays for use in high-throughput biological screening 7,8 , separation of proteins and conformational enrichment of peptides [9][10][11][12] , covalent attachment of peptides to surfaces 9,10,13,14 , chiral enrichment of organic compounds 15 , electrochemical characterization of specific redox-active proteins [16][17][18] , production of thin molecular films 19,20 , processing of macromolecules such as graphene 21 and preparation of model catalyst systems through soft landing of ionic clusters [22][23][24][25][26][27][28][29][30][31][32][33][34][35][36][37][38][39] , nanoparticles [40][41]…”

Section: Introductionmentioning

confidence: 99%

“…The concept of modifying surfaces through soft landing of polyatomic ions was initially proposed by Cooks and co-workers in 1977 57 . In the subsequent years a wide range of instrumental approaches have been developed for the controlled deposition of mass-selected ions from the gas-phase onto surfaces 1,4,5 . Ions have been produced through processes such as electrospray ionization (ESI) 10,58,59 , matrix-assisted laser desorption/ionization (MALDI) 21 , electron impact ionization (EI) 60,61 , pulsed arc discharge 62 , inert gas condensation 36,63 , magnetron sputtering 64,65 , and laser vaporization 25,66,67 .…”

Section: Introductionmentioning

confidence: 99%

<em>In Situ</em> SIMS and IR Spectroscopy of Well-defined Surfaces Prepared by Soft Landing of Mass-selected Ions

Johnson

Gunaratne

Laskin

2014

JoVE

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Soft landing of mass-selected ions onto surfaces is a powerful approach for the highly-controlled preparation of materials that are inaccessible using conventional synthesis techniques. Coupling soft landing with in situ characterization using secondary ion mass spectrometry (SIMS) and infrared reflection absorption spectroscopy (IRRAS) enables analysis of well-defined surfaces under clean vacuum conditions. The capabilities of three soft-landing instruments constructed in our laboratory are illustrated for the representative system of surface-bound organometallics prepared by soft landing of mass-selected ruthenium tris(bipyridine) dications, [Ru(bpy) 3 ] 2+ (bpy = bipyridine), onto carboxylic acid terminated self-assembled monolayer surfaces on gold (COOH-SAMs). In situ time-of-flight (TOF)-SIMS provides insight into the reactivity of the soft-landed ions. In addition, the kinetics of charge reduction, neutralization and desorption occurring on the COOH-SAM both during and after ion soft landing are studied using in situ Fourier transform ion cyclotron resonance (FT-ICR)-SIMS measurements. In situ IRRAS experiments provide insight into how the structure of organic ligands surrounding metal centers is perturbed through immobilization of organometallic ions on COOH-SAM surfaces by soft landing. Collectively, the three instruments provide complementary information about the chemical composition, reactivity and structure of well-defined species supported on surfaces. Video LinkThe video component of this article can be found at

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Soft-landing preparative mass spectrometry

Cited by 71 publications

References 134 publications

New mass spectrometry techniques for studying physical chemistry of atmospheric heterogeneous processes

New mass spectrometry techniques for studying physical chemistry of atmospheric heterogeneous processes

In situ solid-state electrochemistry of mass-selected ions at well-defined electrode–electrolyte interfaces

<em>In Situ</em> SIMS and IR Spectroscopy of Well-defined Surfaces Prepared by Soft Landing of Mass-selected Ions

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