Hydrothermally stable Pd/SiO2@Zr Core@Shell catalysts for diesel oxidation applications

Chih Han Liu; Junjie Chen; Todd J. Toops; Jae Soon Choi; Cyril Thomas; Michael J. Lance; Eleni A. Kyriakidou

doi:10.1016/j.cej.2021.130637

Hydrothermally stable Pd/SiO₂@Zr Core@Shell catalysts for diesel oxidation applications

Chih Han Liu, Junjie Chen, Todd J. Toops, Jae Soon Choi, Cyril Thomas, Michael J. Lance, Eleni A. Kyriakidou

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

13 Scopus citations

Abstract

Hydrothermally stable diesel oxidation catalysts (DOCs) with improved low-temperature activity are desired for the abatement of emissions from diesel vehicles. Herein, novel palladium(Pd)/SiO₂(core)@Zr(shell) structured DOCs were developed. SiO₂ was completely covered by an 8.4 nm thickness Zr-based shell using a hard template method. The SiO₂@Zr support was decorated by Pd and evaluated under a simulated diesel exhaust stream. Degreened 1 wt% Pd/SiO₂@Zr achieved 90% CO and total hydrocarbon conversion at 178 and 372 °C, respectively (feed: 6% CO₂, 12% O₂, 6% H₂O, 400 ppm H₂, 2000 ppm CO, 100 ppm NO, 1667 ppm C₂H₄, 1000 ppm C₃H₆, 333 ppm C₃H₈; HCs in C₁ basis and GHSV = 113,000 h⁻¹). After hydrothermal aging, only a minor deactivation was observed, while the surface area of 1 wt% Pd/SiO₂@Zr was as high as 104 m²/g. The hydrothermal stability of 1 wt% Pd/SiO₂@Zr was attributed to the poor crystallinity of SiO₂@Zr, possibly due to the formation of Si-O-Zr bonds. This work highlights the promising potential of utilizing durable Pd/SiO₂@Zr catalysts for diesel oxidation applications.

Original language	English
Article number	130637
Journal	Chemical Engineering Journal
Volume	425
DOIs	https://doi.org/10.1016/j.cej.2021.130637
State	Published - Dec 1 2021

Funding

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 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).

Funders	Funder number
DOE Public Access Plan
United States Government
U.S. Department of Energy

Keywords

Core@shell
Diesel oxidation catalyst
Heterogeneous catalysis
Hydrothermal stability
Oxidation

UN SDGs

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

Access to Document

10.1016/j.cej.2021.130637

Cite this

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title = "Hydrothermally stable Pd/SiO2@Zr Core@Shell catalysts for diesel oxidation applications",

abstract = "Hydrothermally stable diesel oxidation catalysts (DOCs) with improved low-temperature activity are desired for the abatement of emissions from diesel vehicles. Herein, novel palladium(Pd)/SiO2(core)@Zr(shell) structured DOCs were developed. SiO2 was completely covered by an 8.4 nm thickness Zr-based shell using a hard template method. The SiO2@Zr support was decorated by Pd and evaluated under a simulated diesel exhaust stream. Degreened 1 wt% Pd/SiO2@Zr achieved 90% CO and total hydrocarbon conversion at 178 and 372 °C, respectively (feed: 6% CO2, 12% O2, 6% H2O, 400 ppm H2, 2000 ppm CO, 100 ppm NO, 1667 ppm C2H4, 1000 ppm C3H6, 333 ppm C3H8; HCs in C1 basis and GHSV = 113,000 h−1). After hydrothermal aging, only a minor deactivation was observed, while the surface area of 1 wt% Pd/SiO2@Zr was as high as 104 m2/g. The hydrothermal stability of 1 wt% Pd/SiO2@Zr was attributed to the poor crystallinity of SiO2@Zr, possibly due to the formation of Si-O-Zr bonds. This work highlights the promising potential of utilizing durable Pd/SiO2@Zr catalysts for diesel oxidation applications.",

keywords = "Core@shell, Diesel oxidation catalyst, Heterogeneous catalysis, Hydrothermal stability, Oxidation",

author = "Liu, {Chih Han} and Junjie Chen and Toops, {Todd J.} and Choi, {Jae Soon} and Cyril Thomas and Lance, {Michael J.} and Kyriakidou, {Eleni A.}",

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doi = "10.1016/j.cej.2021.130637",

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AU - Liu, Chih Han

AU - Chen, Junjie

AU - Toops, Todd J.

AU - Choi, Jae Soon

AU - Thomas, Cyril

AU - Lance, Michael J.

AU - Kyriakidou, Eleni A.

PY - 2021/12/1

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N2 - Hydrothermally stable diesel oxidation catalysts (DOCs) with improved low-temperature activity are desired for the abatement of emissions from diesel vehicles. Herein, novel palladium(Pd)/SiO2(core)@Zr(shell) structured DOCs were developed. SiO2 was completely covered by an 8.4 nm thickness Zr-based shell using a hard template method. The SiO2@Zr support was decorated by Pd and evaluated under a simulated diesel exhaust stream. Degreened 1 wt% Pd/SiO2@Zr achieved 90% CO and total hydrocarbon conversion at 178 and 372 °C, respectively (feed: 6% CO2, 12% O2, 6% H2O, 400 ppm H2, 2000 ppm CO, 100 ppm NO, 1667 ppm C2H4, 1000 ppm C3H6, 333 ppm C3H8; HCs in C1 basis and GHSV = 113,000 h−1). After hydrothermal aging, only a minor deactivation was observed, while the surface area of 1 wt% Pd/SiO2@Zr was as high as 104 m2/g. The hydrothermal stability of 1 wt% Pd/SiO2@Zr was attributed to the poor crystallinity of SiO2@Zr, possibly due to the formation of Si-O-Zr bonds. This work highlights the promising potential of utilizing durable Pd/SiO2@Zr catalysts for diesel oxidation applications.

AB - Hydrothermally stable diesel oxidation catalysts (DOCs) with improved low-temperature activity are desired for the abatement of emissions from diesel vehicles. Herein, novel palladium(Pd)/SiO2(core)@Zr(shell) structured DOCs were developed. SiO2 was completely covered by an 8.4 nm thickness Zr-based shell using a hard template method. The SiO2@Zr support was decorated by Pd and evaluated under a simulated diesel exhaust stream. Degreened 1 wt% Pd/SiO2@Zr achieved 90% CO and total hydrocarbon conversion at 178 and 372 °C, respectively (feed: 6% CO2, 12% O2, 6% H2O, 400 ppm H2, 2000 ppm CO, 100 ppm NO, 1667 ppm C2H4, 1000 ppm C3H6, 333 ppm C3H8; HCs in C1 basis and GHSV = 113,000 h−1). After hydrothermal aging, only a minor deactivation was observed, while the surface area of 1 wt% Pd/SiO2@Zr was as high as 104 m2/g. The hydrothermal stability of 1 wt% Pd/SiO2@Zr was attributed to the poor crystallinity of SiO2@Zr, possibly due to the formation of Si-O-Zr bonds. This work highlights the promising potential of utilizing durable Pd/SiO2@Zr catalysts for diesel oxidation applications.

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