4.4 Article

Using microkinetic analysis to search for novel anhydrous formaldehyde production catalysts

期刊

SURFACE SCIENCE
卷 641, 期 -, 页码 105-111

出版社

ELSEVIER SCIENCE BV
DOI: 10.1016/j.susc.2015.04.028

关键词

Methanol; Formaldehyde; Heterogeneous catalysis; Density functional theory; Scaling relations; Microkinetic model

资金

  1. U.S. Department of Energy's Office of Basic Energy Science [FWP-100167]

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Direct dehydrogenation of methanol to produce anhydrous formaldehyde is investigated using periodic density functional theory (DFT) and combining the microkinetic model to estimate rates and selectivities on stepped (211) surfaces under a desired reaction condition. Binding energies of reaction intermediates and transition state energies for each elementary reaction can be accurately scaled with CHO and OH binding energies as the only descriptors. Based on these two descriptors, a steady-state microkinetic model is constructed with a piece-wise adsorbate-adsorbate interaction model that explicitly includes the effects of adsorbate coverage on the rates and selectivities as well as the volcano plots are obtained. Our results show that most of the stepped (211) pure-metallic surfaces such as Au, Pt, Pd, Rh, Ru, Ni, Fe, and Co are located in a region of low activity and selectivity toward CH2O production due to higher rate for CH2O dehydrogenation than CH2O desorption. The selectivities toward CH2O production on Zn, Cu, and Ag surfaces are located on the boundary between the high and low selectivity regions. To find suitable catalysts for anhydrous CH2O production, a large number of A(3)B-type transition metal alloys are screened based on their predicted rates and selectivities, as well as their estimated stabilities and prices. We finally propose several promising candidates for the dehydrogenation of CH3OH. Published by Elsevier B.V.

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