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Chemically Functionalized Surfaces through Ion Soft Landing and their Utilization in Heterogeneous Reactions


EMSL Project ID
34913

Abstract

Interaction of hyperthermal energy polyatomic ions with surfaces is an active area of research which falls within the purview of material science, mass spectrometry, imaging and spectroscopy, all relevant to the scientific disciplines supported by the DOE Office of Science. Specific aims include preparation of surfaces with appropriate chemical functionalities via soft-landing (SL) of molecular or cluster ions by transferring functionalization from gas phase to surfaces, confirming the nature of the landed group by in situ secondary ion mass spectrometry and investigating heterogeneous phase reactivity of these surfaces. The heterogeneous reactions will be monitored in situ by surface enhanced Raman spectroscopy (SERS). Improved methods of measuring charge neutralization/retention/build-up at surfaces and increasing the speed of surface preparation using an ion source array for higher total ion currents are also likely to be accomplished. Achievement of these objectives should increase the understanding of ion/surface collisions at hyperthermal energy, especially chemical transformations in the nature of the surface-bound products. These experiments aim to evaluate mass spectrometry as a method for the preparation of customized, reactive surfaces. This includes surfaces that serve as models for reactions of particular biological molecules from complex mixtures as well as surfaces that show selective reactivity in polymerization reactions, epoxidations, hydrogenation reactions, etc. The ability to create surfaces with controlled biomolecule and/or small molecule heterogeneous phase reactivity is expected to have significant impacts in surface science and bioanalysis. Practical implications in the longer term might include the development of new methodology to generate catalytic materials.

Project Details

Project type
Large-Scale EMSL Research
Start Date
2009-10-05
End Date
2012-09-30
Status
Closed

Team

Principal Investigator

Robert Cooks
Institution
Purdue University

Team Members

Grant Johnson
Institution
Pacific Northwest National Laboratory

Jobin Cyriac
Institution
Purdue University

Qichi Hu
Institution
Pacific Northwest National Laboratory

Julia Laskin
Institution
Purdue University

Related Publications

Hu Q, P Wang, and J Laskin. 2010. "Effect of the surface on the secondary structure of soft landed peptide ions." Physical Chemistry Chemical Physics. PCCP 12(39):12802-12810. doi:10.1039/C0CP00825G
Hu Q, P Wang, PL Gassman, and J Laskin.  2009.  "In situ Studies of Soft- and Reactive Landing of Mass-Selected Ions Using Infrared Reflection Absorption Spectroscopy."  Analytical Chemistry 81(17):7302-7308.  doi:10.1021/ac901149s
Johnson GE, M Lysonski, and J Laskin.  2010.  "In Situ Reactivity and TOF SIMS Analysis of Surfaces Prepared by Soft and Reactive Landing of Mass Selected Ions."  Analytical Chemistry 82(13):5718-5727.  doi:10.1021/ac100734g
Johnson GE, Q Hu, and J Laskin. 2011. "Soft Landing of Complex Molecules on Surfaces." Annual Review of Analytical Chemistry 4(1):83-104. doi:10.1146/annurev-anchem-061010-114028
Johnson GE, TA Priest, and J Laskin. 2012. "Charge Retention by Gold Clusters on Surfaces Prepared Using Soft Landing of Mass Selected Ions ." ACS Nano 6(1):573-582. doi:10.1021/nn2039565