Journal
CATALYSIS SCIENCE & TECHNOLOGY
Volume 11, Issue 23, Pages 7563-7577Publisher
ROYAL SOC CHEMISTRY
DOI: 10.1039/d1cy01149a
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Funding
- ETH [ETH 57 12-2]
- Swiss National Science Foundation [200020_156015]
- European Research Council under the European Union's [819573]
- Swiss National Science Foundation (SNF) [200020_156015] Funding Source: Swiss National Science Foundation (SNF)
- European Research Council (ERC) [819573] Funding Source: European Research Council (ERC)
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The Al2O3-coated Ni/SiO2 catalyst prepared by ALD method showed improved stability and resistance to coke deposition in dry reforming of methane, suppressing the sintering of Ni and coke formation. The in-depth structural characterization provided insights into the interaction between the ALD-grown Al2O3 layer and the support, leading to the high stability of the catalyst under harsh conditions.
The development of stable Ni-based dry reforming of methane (DRM) catalysts is a key challenge owing to the high operating temperatures of the process and the propensity of Ni for promoting carbon deposition. In this work, Al2O3-coated Ni/SiO2 catalysts have been developed by employing atomic layer deposition (ALD). The structure of the catalyst at each individual preparation step was characterized in detail through a combination of in situ XAS-XRD, ex situ(27)Al NMR and Raman spectroscopy. Specifically, in the calcination step, the ALD-grown Al2O3 layer reacts with the SiO2 support and Ni, forming aluminosilicate and NiAl2O4. The Al2O3-coated Ni/SiO2 catalyst exhibits an improved stability for DRM when compared to the benchmark Ni/SiO2 and Ni/Al2O3 catalysts. In situ XAS-XRD during DRM together with ex situ Raman spectroscopy and TEM of the spent catalysts confirm that the ALD-grown Al2O3 layer suppresses the sintering of Ni, in turn reducing also coke formation significantly. In addition, the formation of an amorphous aluminosilicate phase by the reaction of the ALD-grown Al2O3 layer with the SiO2 support inhibited catalysts deactivation via NiAl2O4 formation, in contrast to the reference Ni/Al2O3 system. The in-depth structural characterization of the catalysts provided an insight into the structural dynamics of the ALD-grown Al2O3 layer, which reacts both with the support and the active metal, allowing to rationalize the high stability of the catalyst under the harsh DRM conditions.
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