2019
DOI: 10.1021/acs.iecr.9b01169
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Short Contact Time Catalytic Partial Oxidation of Methane over Rhodium Supported on Ceria Based 3-D Printed Supports

Abstract: Three different ceria containing catalyst supports and an alumina (control) support have been deposited with rhodium and used in the short contact time catalytic partial oxidation of methane. The goal of this paper is to compare reactor performance from powder catalyst studies to determine how they translate into structured high gas hourly space velocity catalysts operating at millisecond contact times. The supports were synthesized by 3-D printing of powders allowing for the first time the use of a catalyst s… Show more

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Cited by 11 publications
(5 citation statements)
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“…Contrary to the SRM reaction, the partial oxidation of methane (POM) that follows the reaction of CH 4 + O 2 → 2H 2 + CO 2 enables the generation of highly exothermic H 2 (Δ H 298 = −3.31 eV) and it is considered as a promising strategy to yield H 2 from an economical perspective. , However, limited by the inertness of CH 4 and O 2 molecules, the spontaneous POM reaction could occur only at high temperatures ( T > 700 °C) in the absence of a catalyst . Since the first experimental detection of free H 2 from POM reaction catalyzed by Ni/Al 2 O 3 in 1929, various heterogeneous catalysts supported with base and precious metals have been engineered for CH 4 conversion at relatively low temperatures. The dominant size-dependent catalytic behavior of supported metals motivates elaborate controls of metal species spanning from nanoparticles to subnanoclusters, aiming for optimization of the catalytic performance toward the POM reaction and the conservation of metal resources particularly for precious metals (e.g., supported rhodium catalysts with sizes of 30.5 nm → 2.5 nm → 1.3 nm → 0.6 nm have been tailored). However, it remains challenging experimentally to achieve catalytic hydrogen production under mild conditions. The genuine mechanisms of H 2 production from POM reaction have also not been completely clarified at a strictly molecular level.…”
Section: Introductionmentioning
confidence: 99%
“…Contrary to the SRM reaction, the partial oxidation of methane (POM) that follows the reaction of CH 4 + O 2 → 2H 2 + CO 2 enables the generation of highly exothermic H 2 (Δ H 298 = −3.31 eV) and it is considered as a promising strategy to yield H 2 from an economical perspective. , However, limited by the inertness of CH 4 and O 2 molecules, the spontaneous POM reaction could occur only at high temperatures ( T > 700 °C) in the absence of a catalyst . Since the first experimental detection of free H 2 from POM reaction catalyzed by Ni/Al 2 O 3 in 1929, various heterogeneous catalysts supported with base and precious metals have been engineered for CH 4 conversion at relatively low temperatures. The dominant size-dependent catalytic behavior of supported metals motivates elaborate controls of metal species spanning from nanoparticles to subnanoclusters, aiming for optimization of the catalytic performance toward the POM reaction and the conservation of metal resources particularly for precious metals (e.g., supported rhodium catalysts with sizes of 30.5 nm → 2.5 nm → 1.3 nm → 0.6 nm have been tailored). However, it remains challenging experimentally to achieve catalytic hydrogen production under mild conditions. The genuine mechanisms of H 2 production from POM reaction have also not been completely clarified at a strictly molecular level.…”
Section: Introductionmentioning
confidence: 99%
“…The technology of additive manufacturing, broadly known as three‐dimensional (3d) printing, has been evolving extensively in the last decades, and recently catalytically active 3d printed objects started to emerge . Indeed, 3d printing provides potential for creating objects not only with desired catalytic properties, but at the same time with required shapes, e. g. for batch or flow reactors with heterogeneous solid catalysts.…”
Section: Introductionmentioning
confidence: 99%
“…Indeed, 3d printing provides potential for creating objects not only with desired catalytic properties, but at the same time with required shapes, e. g. for batch or flow reactors with heterogeneous solid catalysts. A number of reports emerged recently on new catalysts for various reactions, produced by 3d printing with and without chemical post‐processing of the printed objects. Among these reports, the majority utilizes fused deposition modelling (FDM) or robocasting, selective laser melting (SLM), and in some cases stereolithography (SL) methods.…”
Section: Introductionmentioning
confidence: 99%
“…[1][2][3][4] To date, several different hydrogen production processes have been studied and applied, including water electrolysis, 5 water photolysis 6 and hydrocarbon partial oxidation and reforming. [7][8][9][10] In addition to these processes, thermochemical pathways for the production of hydrogen/syngas by decomposition of methane, 11,12 ethanol, 13,14 as well as catalytic cracking of waste cooking oil (WCO), [15][16][17] are receiving increasing attention. WCO refers to a variety of oil wastes from natural vegetable oils and animal fats that lose edible value in the process of cooking or deep processing.…”
Section: Introductionmentioning
confidence: 99%