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Fundamental Mechanistic Studies of Catalytic Reactions Using a Combined Steady-State Isotopic Transient Kinetic Analysis (SSITKA)/Fourier Transform Infrared (FTIR) Spectroscopy Apparatus


EMSL Project ID
48593

Abstract

This project will apply a unique capability in the EMSL at PNNL for heterogeneous catalysis R&D employing steady-state isotopic transient kinetic analysis (SSITKA) techniques with mass spectroscopic detection that is coupled with in-situ transmission fourier transform infrared (FTIR) spectroscopy. The apparatus provides an in situ probe of adsorbed reactants/intermediates/ products on catalyst surfaces, as well as measuring gas phase concentrations to elucidate reaction mechanisms and kinetic parameters. The resulting data will be interpreted and applied to develop microkinetic models for catalytic reactions of importance to the US's future energy, environment, and economic security. This instrument was developed primarily with PNNL LDRD funding and capital equipment was procured with PNNL GRE funds. The instrument does provide unique capabilities for catalysis research that greatly complements existing EMSL resources, and has been a valuable resource to EMSL users. As such, it has been always located in EMSL and has greatly benefited from being available to EMSL collaborative users. Still, because of difficulty in operating the instrument and a lack of available EMSL support for an operator during its collaborative EMSL use, it is still primarily used by the Resource Owner's (C.H.F. Peden) group. This "Resource Owner" EMSL user proposal documents some of the science being done on this instrument.

Project Details

Start Date
2014-10-01
End Date
2017-09-30
Status
Closed

Team

Principal Investigator

Charles Peden
Institution
Pacific Northwest National Laboratory

Team Members

Yongchun Hong
Institution
University of California, Berkeley

Feng Gao
Institution
Pacific Northwest National Laboratory

Junming Sun
Institution
Washington State University

Charles Mims
Institution
University of Toronto

Cheol-woo Yi
Institution
Sungshin Women's University

Yong Yang
Institution
University of Washington

Janos Szanyi
Institution
Pacific Northwest National Laboratory

Charles Campbell
Institution
University of Washington

Yong Wang
Institution
Washington State University

Kenneth Rappe
Institution
Pacific Northwest National Laboratory

Related Publications

Yang Y, D Mei, CHF Peden, CT Campbell, and CA Mims. 2015. "Surface-Bound Intermediates in Low-Temperature Methanol Synthesis on Copper: Participants and Spectators." ACS Catalysis 5(12):7328-7337. doi:10.1021/acscatal.5b02060