Title: Multi-scale simulation of reaction, transport and deactivation in a SBA-16 supported catalyst for the conversion of ethanol to butadiene

Abstract

Effective design of heterogeneous catalytic systems requires careful coordination of physiochemical phenomena that span orders or magnitude in length and time scales. Multiscale modeling and simulation tools can provide useful insight for understanding and improving the performance of such systems. Mesoporous silica catalyst support materials present a versatile platform wherein support attributes may be tuned to control transport phenomena throughout the system. In this study we develop an integrated multiscale modeling approach for the conversion of ethanol to butadiene over an SBA-16 mesoporous silica supported catalyst. We use molecular dynamics simulations to calculate domain specific diffusivities of reactants and products in the various domains of SBA-16’s nanostructure. This is used to calculate a resultant effective diffusivity (Deff) through its microstructure using finite element method (FEM) models of the tessellated unit cell. The resultant effective diffusivity enables the development of a reduced-order reactor level FEM model that is able to implicitly account for the SBA-16’s transport effects without the explicit consideration of its detailed geometry. Experimental bench-scale conversion data for the ethanol to butadiene process over SBA-16 is used to extract intrinsic kinetic rate constants for a simplified reaction mechanism using this reduced order bench-scale reactor FEM model. The model ismore » able to reproduce experimental trends in conversion and activity lifetimes. The impact of varying key support attributes such as pore-size and particle size on catalytic activity lifetimes is then explored. We demonstrate the utility of this multi-scale modelling strategy in guiding catalyst design for the development of rational strategies to improve the performance of heterogeneous supported catalytic systems.« less

Authors:

Bharadwaj, Vivek S.  ^[1];

• Search DOE PAGES for author "Bharadwaj, Vivek S."
• Search DOE PAGES for ORCID "0000-0001-5851-9807"

Pecha, Michael B.  ^[1];

• Search DOE PAGES for author "Pecha, Michael B."
• Search DOE PAGES for ORCID "0000-0002-0894-8504"

Bu, Lintao ^[1]; Dagle, Vanessa Lebarbier ^[2]; Dagle, Robert A. ^[2]; Ciesielski, Peter N.  ^[1]

• Search DOE PAGES for author "Ciesielski, Peter N."
• Search DOE PAGES for ORCID "0000-0003-3360-9210"

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+ Show Author Affiliations

1. National Renewable Energy Lab. (NREL), Golden, CO (United States)
2. Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Publication Date:

Thu May 23 00:00:00 EDT 2019

Research Org.:

National Renewable Energy Lab. (NREL), Golden, CO (United States); Pacific Northwest National Lab. (PNNL), Richland, WA (United States)

Sponsoring Org.:

USDOE Office of Energy Efficiency and Renewable Energy (EERE), Sustainable Transportation Office. Bioenergy Technologies Office

OSTI Identifier:

1525763

Alternate Identifier(s):

OSTI ID: 1573020

Report Number(s):

NREL/JA-2700-74122; PNNL-SA-139387
Journal ID: ISSN 0920-5861

Grant/Contract Number:  

AC36-08GO28308; AC05-76RL01830

Resource Type:

Accepted Manuscript

Journal Name:

Catalysis Today

Additional Journal Information:

Journal Volume: 338; Journal Issue: C; Journal ID: ISSN 0920-5861

Publisher:

Elsevier

Country of Publication:

United States

Language:

English

Subject:

09 BIOMASS FUELS; 37 INORGANIC, ORGANIC, PHYSICAL, AND ANALYTICAL CHEMISTRY; multi-scale catalysis; finite element method; molecular dynamics; reaction; diffusion; deactivation; catalyst design