Layer structured bifunctional monolith catalysts for energy-efficient conversion of CO2 to dimethyl ether

Hai Ying Chen; Josh Pihl; Todd J. Toops; Sreshtha Sinha Majumdar

doi:10.1016/j.apcata.2023.119140

Layer structured bifunctional monolith catalysts for energy-efficient conversion of CO₂ to dimethyl ether

Hai Ying Chen, Josh Pihl, Todd J. Toops, Sreshtha Sinha Majumdar

Research output: Contribution to journal › Article › peer-review

2 Scopus citations

Abstract

A monolith supported bifunctional catalyst for the direct conversion of CO₂ to dimethyl ether was developed and evaluated. The catalyst consists of a layer structured configuration, in which a CuO/ZnO/ZrO₂ component for methanol synthesis using CO₂ as feedstock and a Ferrierite zeolite component for the subsequent dehydration reaction are washcoated onto the channel surfaces of a metallic monolith substrate as two consecutive layers. The metal substrate provides heat conduction to regulate the catalyst bed temperature. The layered configuration significantly improves the synergistic effects of the two components, resulting in a 20% increase in the productivity for dimethyl ether at 240 ℃ as compared with the conventional catalysts with the two components being blended in various levels of proximity. Additionally, the layer structured design minimizes the undesirable interaction between the two components and drastically improves the on-stream durability of the catalyst. No activity decline was observed in a 146-h performance test.

Original language	English
Article number	119140
Journal	Applied Catalysis A: General
Volume	656
DOIs	https://doi.org/10.1016/j.apcata.2023.119140
State	Published - Apr 25 2023

Funding

This work was sponsored by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory, managed by UT-Battelle, LLC, for the U. S. Department of Energy. The authors thank Junyan Zhang for conducting the XRD and Xiaohan Ma for the SEM analysis. H.-Y.C. conceived the monolith catalyst concept, designed, and conducted the experiment. J.P. contributed ideas to the concept and set up the reactor system. T.J.T. contributed ideas to the concept and facilitated experimental design. S.S.M. prepared some of the catalysts. H.-Y.C wrote the manuscript with input of all co-authors. Notice: This manuscript has been authored by UT-Battelle, LLC under Contract No. DE-AC05–00OR22725 with the U.S. Department of Energy. The United States Government retains and the publisher, by accepting the article for publication, acknowledges that the United States Government retains a non-exclusive, paid-up, irrevocable, world-wide license to publish or reproduce the published form of this manuscript, or allow others to do so, for United States Government purposes. The Department of Energy will provide public access to these results of federally sponsored research in accordance with the DOE Public Access Plan ( http://energy.gov/downloads/doe-public-access-plan ). This work was sponsored by the Laboratory Directed Research and Development Program of Oak Ridge National Laboratory , managed by UT-Battelle, LLC, for the U. S. Department of Energy . The authors thank Junyan Zhang for conducting the XRD and Xiaohan Ma for the SEM analysis.

Funders	Funder number
Xiaohan Ma
U.S. Department of Energy
Oak Ridge National Laboratory

Keywords

CO conversion
Catalyst durability
Layer structured configuration
Monolith catalyst
Synergistic effect

UN SDGs

This output contributes to the following UN Sustainable Development Goals (SDGs)

Access to Document

10.1016/j.apcata.2023.119140

Cite this

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title = "Layer structured bifunctional monolith catalysts for energy-efficient conversion of CO2 to dimethyl ether",

abstract = "A monolith supported bifunctional catalyst for the direct conversion of CO2 to dimethyl ether was developed and evaluated. The catalyst consists of a layer structured configuration, in which a CuO/ZnO/ZrO2 component for methanol synthesis using CO2 as feedstock and a Ferrierite zeolite component for the subsequent dehydration reaction are washcoated onto the channel surfaces of a metallic monolith substrate as two consecutive layers. The metal substrate provides heat conduction to regulate the catalyst bed temperature. The layered configuration significantly improves the synergistic effects of the two components, resulting in a 20% increase in the productivity for dimethyl ether at 240 ℃ as compared with the conventional catalysts with the two components being blended in various levels of proximity. Additionally, the layer structured design minimizes the undesirable interaction between the two components and drastically improves the on-stream durability of the catalyst. No activity decline was observed in a 146-h performance test.",

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N2 - A monolith supported bifunctional catalyst for the direct conversion of CO2 to dimethyl ether was developed and evaluated. The catalyst consists of a layer structured configuration, in which a CuO/ZnO/ZrO2 component for methanol synthesis using CO2 as feedstock and a Ferrierite zeolite component for the subsequent dehydration reaction are washcoated onto the channel surfaces of a metallic monolith substrate as two consecutive layers. The metal substrate provides heat conduction to regulate the catalyst bed temperature. The layered configuration significantly improves the synergistic effects of the two components, resulting in a 20% increase in the productivity for dimethyl ether at 240 ℃ as compared with the conventional catalysts with the two components being blended in various levels of proximity. Additionally, the layer structured design minimizes the undesirable interaction between the two components and drastically improves the on-stream durability of the catalyst. No activity decline was observed in a 146-h performance test.

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