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

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

doi:10.1016/j.cej.2024.158726

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

Journal Article · 16 December 2024 · Chemical Engineering Journal

DOI: https://doi.org/10.1016/j.cej.2024.158726 · OSTI ID:2510447

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Stony Brook Univ., NY (United States)
Stony Brook Univ., NY (United States); Mitsubishi Chemical Corporation (Japan)
Brookhaven National Laboratory (BNL), Upton, NY (United States). Center for Functional Nanomaterials (CFN)
Brookhaven National Laboratory (BNL), Upton, NY (United States). National Synchrotron Light Source II (NSLS-II)
Hanyang Univ., Seoul (Korea, Republic of)
Seoul National Univ. (Korea, Republic of)
Stony Brook Univ., NY (United States); Brookhaven National Laboratory (BNL), Upton, NY (United States)

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. Here, 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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Research Organization:: Brookhaven National Laboratory (BNL), Upton, NY (United States)

Sponsoring Organization:: USDOE Office of Science (SC), Basic Energy Sciences (BES). Scientific User Facilities (SUF)

Grant/Contract Number:: SC0012704

OSTI ID:: 2510447

Report Number(s):: BNL--227542-2025-JAAM

Journal Information:: Chemical Engineering Journal, Journal Name: Chemical Engineering Journal Vol. 504; ISSN 1385-8947

Publisher:: ElsevierCopyright Statement

Country of Publication:: United States

Language:: English

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Title: 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

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