Development of ceria-supported metal-oxide (MOx/CeO2) catalysts via a one-pot chemical vapor deposition (OP-CVD) technique: Structure and reverse water gas shift reaction study

• CeO 2 -supported MO x catalysts made via one-pot chemical vapor deposition (OP-CVD). • Precursor selection procedure and synthesis methodology for OP-CVD were developed. • MO x /CeO 2 achieved homogeneous dispersion and desired loading of surface species. • Small-sized metal oxide (e.g. 2.7–3.1 Å for CoO x ) was confirmed from XAS analysis. • High RWGS activity (>0.1 mol/h g-cat) and selectivity (100%) for CO were reported. Current synthesis techniques for metal oxide (MO x )-supported catalysts have certain limitations of undesired target loading, ineffective dispersion of active species over the surface, uncontrolled particle size of active species, and complicated synthesis steps. We developed a one-pot chemical vapor deposition (OP-CVD) methodology; by using which a solid metal precursor forms a vapor in a controlled condition and gets supported over the surrounding matrix. The theoretical stability followed by experimental validation using TGA is crucial for selecting the metal precursors. Three simple steps viz. premixing, dispersion, and rapid fixation by calcination are involved in the catalyst development via the OP-CVD approach. This study solely focused on the synthesis of 3d transition MO x over ceria support. The physicochemical characterizations of the prepared catalysts were performed by XRD, ICP-OES, SEM-EDX, CO pulse chemisorption, XANES, and EXAFS analyses to understand the crystal structure of involved species, target metal loading, dispersion, and particle size and prove the feasibility and viability of OP-CVD. The prepared catalysts were further tested for reverse water gas shift (RWGS) reaction to link their structural information with activity. The RWGS reaction data showed that the CO activity and CO selectivity were metal - and metal precursor-dependent. Higher CO activity of > 0.1 mol/h g-cat was observed for Cu and Co-based catalysts, with CO selectivity of ∼100 %. This study provides an opportunity to produce efficient supported catalysts in a convenient way, providing effective catalytic activity.

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Publication Details

Journal
Chemical Engineering Journal
Published
2024-12-18
DOI
https://doi.org/10.1016/j.cej.2024.158726
Citations
8
Primary Topic
Catalytic Processes in Materials Science
Type
article
Field-Weighted Citation Impact
0.94
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article

Development of ceria-supported metal-oxide (MOx/CeO2) catalysts via a one-pot chemical vapor deposition (OP-CVD) technique: Structure and reverse water gas shift reaction study

Gihan Kwon, Kwangsuk Yoon, Hocheol Song, Anatoly I. Frenkel et al.
8 citations
Chemical Engineering Journal
Catalytic Processes in Materials Science
0.94
article

Development of ceria-supported metal-oxide (MOx/CeO2) catalysts via a one-pot chemical vapor deposition (OP-CVD) technique: Structure and reverse water gas shift reaction study

Gihan Kwon, Kwangsuk Yoon, Hocheol Song, Anatoly I. Frenkel, Jangeon Roh, Amol Pophali, Do Heui Kim, Ryuichi Shimogawa, Lihua Zhang, Taejin Kim
article en
8 citations

Abstract

• CeO 2 -supported MO x catalysts made via one-pot chemical vapor deposition (OP-CVD). • Precursor selection procedure and synthesis methodology for OP-CVD were developed. • MO x /CeO 2 achieved homogeneous dispersion and desired loading of surface species. • Small-sized metal oxide (e.g. 2.7–3.1 Å for CoO x ) was confirmed from XAS analysis. • High RWGS activity (>0.1 mol/h g-cat) and selectivity (100%) for CO were reported. Current synthesis techniques for metal oxide (MO x )-supported catalysts have certain limitations of undesired target loading, ineffective dispersion of active species over the surface, uncontrolled particle size of active species, and complicated synthesis steps. We developed a one-pot chemical vapor deposition (OP-CVD) methodology; by using which a solid metal precursor forms a vapor in a controlled condition and gets supported over the surrounding matrix. The theoretical stability followed by experimental validation using TGA is crucial for selecting the metal precursors. Three simple steps viz. premixing, dispersion, and rapid fixation by calcination are involved in the catalyst development via the OP-CVD approach. This study solely focused on the synthesis of 3d transition MO x over ceria support. The physicochemical characterizations of the prepared catalysts were performed by XRD, ICP-OES, SEM-EDX, CO pulse chemisorption, XANES, and EXAFS analyses to understand the crystal structure of involved species, target metal loading, dispersion, and particle size and prove the feasibility and viability of OP-CVD. The prepared catalysts were further tested for reverse water gas shift (RWGS) reaction to link their structural information with activity. The RWGS reaction data showed that the CO activity and CO selectivity were metal - and metal precursor-dependent. Higher CO activity of > 0.1 mol/h g-cat was observed for Cu and Co-based catalysts, with CO selectivity of ∼100 %. This study provides an opportunity to produce efficient supported catalysts in a convenient way, providing effective catalytic activity.

Chemical Engineering JournalVol. 504
Seoul National University (KR), Mitsubishi Chemical (Japan) (JP), Brookhaven National Laboratory (US), National Synchrotron Light Source II, Center for Functional Nanomaterials, Hanyang University (KR), Stony Brook University (US)
Clean water and sanitation
Openalex Percentile: Top 22%
Catalytic Processes in Materials Science
0.94
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