Zirconium‐assistierte Aktivierung von Palladium zur Steigerung der Produktion von Synthesegas in der Trockenreformierung von Methan

Köpfle, Norbert; Götsch, Thomas; Grünbacher, Matthias; Carbonio, Emilia A.; Hävecker, Michael; Knop‐Gericke, Axel; Schlicker, Lukas; Doran, Andrew; Kober, Delf; Gurlo, Aleksander; Penner, Simon; Klötzer, Bernhard

doi:10.1002/ange.201807463

Cited by 3 publications

(2 citation statements)

References 51 publications

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“…From a fundamental viewpoint, these materials are of high interest as the findings on those systems can help to elucidate mechanistic insights and help to transfer the particular coking resilience to less costly, non-noble metal catalysts. In an in situ near-ambient pressure (NAP)-XPS study of our group, the anticoking stability and carbonconverting role of the Pd/ZrO 2 phase boundary (in the following denoted as PB) were highlighted [15]. The results showed that carbon-saturated Pd 0 nanoparticles evolve from an in situ activated PdZr intermetallic precatalyst, leading to the formation of extended C-saturated Pd-metal/Zr-oxide phase boundaries under methane dry reforming conditions.…”

Section: Introductionmentioning

confidence: 99%

“…The results showed that carbon-saturated Pd 0 nanoparticles evolve from an in situ activated PdZr intermetallic precatalyst, leading to the formation of extended C-saturated Pd-metal/Zr-oxide phase boundaries under methane dry reforming conditions. The generation of these PBs results in a highly active state fostering a bifunctional mechanism by effectively activating CO 2 at the oxidic PB sites and CH 4 at the Pd 0 particles forming Pd x C, which provides a fast supply of carbon atoms toward the PB for enhanced CO evolution [15,16]. However, even if noble metals such as Pd do actually exhibit superior properties with respect to DRM activity and stability, as mentioned above, they will inevitably remain little attractive for an industrial application simply due to their high costs.…”

Section: Introductionmentioning

confidence: 99%

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Pivotal Role of Ni/ZrO2 Phase Boundaries for Coke-Resistant Methane Dry Reforming Catalysts

et al. 2023

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To identify the synergistic action of differently prepared Ni-ZrO2 phase boundaries in methane dry reforming, we compared an “inverse” near-surface intermetallic NiZr catalyst precursor with the respective bulk-intermetallic NixZry material and a supported Ni-ZrO2 catalyst. In all three cases, stable and high methane dry reforming activity with enhanced anticoking properties can be assigned to the presence of extended Ni-ZrO2 phase boundaries, which result from in situ activation of the intermetallic Ni-Zr model catalyst systems under DRM conditions. All three catalysts operate bifunctionally; methane is essentially decomposed to carbon at the metallic Ni0 surface sites, whereas CO2 reacts to CO at reduced Zr centers induced by a spillover of carbon to the phase boundaries. On pure bulk Ni0, dissolved carbon accumulates in surface-near regions, leading to a sufficiently supersaturated state for completely surface-blocking graphitic carbon segregation. In strong contrast, surface-ZrO2 modified bulk Ni0 exhibits virtually the best decoking and carbon conversion conditions due to the presence of highly dispersed ZrO2 islands with a particularly large contribution of interfacial Ni0-ZrO2 sites and short C-diffusion pathways to the latter.

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Section: Introductionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Pivotal Role of Ni/ZrO2 Phase Boundaries for Coke-Resistant Methane Dry Reforming Catalysts

et al. 2023

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Zirkonkarbid ermöglicht verkokungsresistente Methan‐Trockenreformierung auf Nickel‐Zirkon‐Katalysatoren

et al. 2022

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Graphitische Ablagerungen lösen sich in Ni 0 -Nanopartikeln auf, um rezyklierte CH 4 -Adsorptionsstellen und oberflächennahe/gelöste C-Atome bereitzustellen, die zur Ni 0 /ZrO 2 -Grenzfläche wandern und eine lokale Zr x C y -Bildung induzieren. Die daraus resultierenden sauerstoffarmen karbidischen Phasengrenzflächen unterstützen die Kinetik der CO 2 -Aktivierung zu CO(g). Dieser Grenzflächen-Karbid-Mechanismus ermöglicht einen verstärkten Übertritt von Kohlenstoff auf den ZrO 2 -Träger und stellt einen alternativen Weg der Katalysatorregeneration im Vergleich zum umgekehrten Sauerstoffübertritt auf Ni/CeZr x O y -Katalysatoren dar. Er ist daher eher auf Trägern mit begrenzter Sauerstoffspeicher-bzw. Austausch-Kinetik, aber signifikanter karbothermischer Reduzierbarkeit, wahrscheinlich.

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Zirconium Carbide Mediates Coke‐Resistant Methane Dry Reforming on Nickel‐Zirconium Catalysts

et al. 2022

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Graphitic deposits anti-segregate into Ni 0 nanoparticles to provide restored CH 4 adsorption sites and near-surface/dissolved C atoms, which migrate to the Ni 0 /ZrO 2 interface and induce local Zr x C y formation. The resulting oxygen-deficient carbidic phase boundary sites assist in the kinetically enhanced CO 2 activation toward CO(g). This interface carbide mechanism allows for enhanced spillover of carbon to the ZrO 2 support, and represents an alternative catalyst regeneration pathway with respect to the reverse oxygen spillover on Ni-CeZr x O y catalysts. It is therefore rather likely on supports with limited oxygen storage/exchange kinetics but significant carbothermal reducibility.

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Zirconium‐assistierte Aktivierung von Palladium zur Steigerung der Produktion von Synthesegas in der Trockenreformierung von Methan

Cited by 3 publications

References 51 publications

Pivotal Role of Ni/ZrO2 Phase Boundaries for Coke-Resistant Methane Dry Reforming Catalysts

Pivotal Role of Ni/ZrO2 Phase Boundaries for Coke-Resistant Methane Dry Reforming Catalysts

Zirkonkarbid ermöglicht verkokungsresistente Methan‐Trockenreformierung auf Nickel‐Zirkon‐Katalysatoren

Zirconium Carbide Mediates Coke‐Resistant Methane Dry Reforming on Nickel‐Zirconium Catalysts

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