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Designing Fuel Cell Catalysts at the Molecular Scale with Ion Soft Landing and Spray Ionization


EMSL Project ID
48305

Abstract

Structure-reactivity relationships that are derived from molecular-level investigation of the properties of well-defined supported nanoparticles (NPs) are critical to the rational development of improved catalysts that will promote the efficient utilization of renewable biofuels. It is currently challenging to develop such a predictive understanding due to the polydisperse and often poorly-defined nature of supported NPs prepared through conventional synthesis techniques. Two alternative approaches involving magnetron sputtering combined with ion soft landing and ambient electrospray ion deposition will be developed to address this challenge. Soft landing of mass-selected NPs under vacuum conditions will be employed to create precisely-defined model catalysts for in-depth characterization. NPs that are identified as catalytically promising from these atomically-precise studies in vacuum will be prepared in increased quantities using a novel technique, in which ambient electrodissolution of a metal is followed by electrospray ionization and wet soft landing onto solid or liquid surfaces. Chemical functionality will be introduced to these NPs by incorporating ligands into the solvent. NPs synthesized using both methods will be characterized using cutting-edge EMSL capabilities in electron microscopy and spectroscopy. Medium energy ion scattering at DGIST in Korea will also be used to determine the elemental composition and structure of NPs. Catalytic activity will be measured in both heterogeneous and homogeneous phase reactors at the Indian Institute of Technology, Madras and Purdue University. The electrochemical activity of NPs towards the oxidation of alcohol biofuels will be characterized at EMSL. Insight gained from characterization of atomically-precise NPs prepared by ion soft landing will guide the scalable synthesis of superior catalysts for fuel cells using ambient spray ionization. This multidisciplinary project involving researchers from leading institutions around the world is relevant to the EMSL science theme of Energy Materials and Processes. Specifically, 1) establishing the fundamental predictive understanding needed to design new catalysts to enhance the production and quality of biofuels and 2) use in situ experimental tools to accelerate understanding of critical material characteristics and molecular processes that will enable new approaches to catalysis design.

Project Details

Project type
Large-Scale EMSL Research
Start Date
2014-10-01
End Date
2016-09-30
Status
Closed

Team

Principal Investigator

Robert Cooks
Institution
Purdue University

Co-Investigator(s)

Grant Johnson
Institution
Pacific Northwest National Laboratory

Team Members

Mary King
Institution
Pacific Northwest National Laboratory

Zachary Norberg
Institution
Pacific Northwest National Laboratory

Jonas Warneke
Institution
Universitat Bremen

David Kalb
Institution
Pacific Northwest National Laboratory

Son Nguyen
Institution
Pacific Northwest National Laboratory

Marshall Ligare
Institution
Pacific Northwest National Laboratory

Venkateshkumar Prabhakaran
Institution
Pacific Northwest National Laboratory

T Pradeep
Institution
Indian Institute of Technology

DaeWon Moon
Institution
Daegu Gyeongbuk Institute of Science and Technology

Related Publications

Gunaratne KDD, V Prabhakaran, YM Ibrahim, RV Norheim, GE Johnson, and J Laskin. 2015. "Design and Performance of a High-Flux Electrospray Ionization Source for Ion Soft-Landing." Analyst. doi:10.1039/C5AN00220F
Johnson GE, RJ Colby, and J Laskin. 2015. "Soft Landing of Bare Nanoparticles with Controlled Size, Composition, and Morphology ." Nanoscale (8):3491-3503. doi:10.1039/C4NR06758D
Laskin J, GE Johnson, and V Prabhakaran. 2016. "Soft Landing of Complex Ions for Studies in Catalysis and Energy Storage." Journal of Physical Chemistry C 120(41):23305-23322. doi:10.1021/acs.jpcc.6b06497
Li A, Z Baird, S Bag, D Sarkar, A Prabhath, T Pradeep, and RG Cooks. 2014. "Using Ambient Ion Beams to Write Nanostructured Patterns for Surface Enhanced Raman Spectroscopy ." Angewandte Chemie International Edition 53(46):12528-12531. doi:10.1002/anie.201406660