(382a) Fundamental Mechanistic Studies of H2O2 Direct Catalytic Synthesis and Decomposition
AIChE Annual Meeting
2014
2014 AIChE Annual Meeting
Catalysis and Reaction Engineering Division
Fundamentals of Surface Reactivity II
Tuesday, November 18, 2014 - 3:15pm to 3:35pm
Fundamental mechanistic studies of H2O2 direct catalytic synthesis and decomposition
A. Plauck1, A. C. Alba-Rubio1, E. Stangland2, J. A. Dumesic1, M. Mavrikakis1
1Department of Chemical & Biological Engineering, University of Wisconsin â?? Madison
2Core Research and Development, The Dow Chemical Company, Midland MI
Hydrogen peroxide (H2O2) is a versatile and environmentally benign oxidizing agent that has the potential to decrease the environmental impact of numerous manufacturing processes â?? both chemical and non-chemical. Currently, the anthraquinone process accounts for over 95% of worldwide H2O2 production but is complex and only implemented on the large scale[1]. This has limited the introduction and expansion of new processes that would benefit from on-site H2O2 production.
Here we focus on an alternative process, the direct synthesis of H2O2, wherein H2 and O2 are combined in a single reactor over a transition metal catalyst. Although Pd-based catalysts for the direct synthesis of H2O2 have been a subject of intense study, especially those modified with Au[2,3], there is still an inadequate understanding of the fundamental details of the active site(s) and elementary transformations. To that end, we combine experimental reaction kinetics studies on a promoter-free Pd catalyst with periodic, self-consistent Density Functional Theory (DFT) calculations on multiple Pd facets to construct a mean-field microkinetic model. This presentation will focus on fundamental mechanistic aspects determining synthesis selectivity to H2O2, and the H2O2 decomposition reaction on Pd-based catalysts.
[1] Centi, G., Perathoner, S., & Abate, S. Direct Synthesis of Hydrogen Peroxide: Recent Advances in Modern Heterogeneous Oxidation Catalysis: Design, Reactions and Characterization. Wiley-VCH, Weinheim, 2009.
[2] Edwards, J. K. et al. Switching Off Hydrogen Peroxide Hydrogenation in the Direct Synthesis Process.
Science 323, 1037-1041 (2009).
[3] Campos-Martin, J. M., Blanco-Brieva, G. & Fierro, J. L. G. Hydrogen Peroxide Synthesis: An Outlook beyond the Anthraquinone Process. Angewandte Chemie-International Edition 45, 6962-6984 (2006).
Topics
Checkout
This paper has an Extended Abstract file available; you must purchase the conference proceedings to access it.
Do you already own this?
Log In for instructions on accessing this content.
Pricing
Individuals
AIChE Pro Members | $150.00 |
AIChE Graduate Student Members | Free |
AIChE Undergraduate Student Members | Free |
AIChE Explorer Members | $225.00 |
Non-Members | $225.00 |