Dataset Information

Propane Steam Reforming over Catalysts Derived from Noble Metal (Ru, Rh)-Substituted LaNiO₃ and La_0.8Sr_0.2NiO₃ Perovskite Precursors.

ABSTRACT: The propane steam reforming (PSR) reaction was investigated over catalysts derived from LaNiO₃ (LN), La_0.8Sr_0.2NiO₃ (LSN), and noble metal-substituted LNM_x and LSNM_x (M = Ru, Rh; x = 0.01, 0.1) perovskites. The incorporation of foreign cations in the A and/or B sites of the perovskite structure resulted in an increase in the specific surface area, a shift of XRD lines toward lower diffraction angles, and a decrease of the mean primary crystallite size of the parent material. Exposure of the as-prepared samples to reaction conditions resulted in the in situ development of new phases including metallic Ni and La₂O₂CO₃, which participate actively in the PSR reaction. The LN-derived catalyst exhibited higher activity compared to LSN, and its performance for the title reaction did not change appreciably following partial substitution of Ru for Ni. In contrast, incorporation of Ru and, especially, Rh in the LSN perovskite matrix resulted in the development of catalysts with significantly enhanced catalytic performance, which improved by increasing the noble metal content. The best results were obtained for the LSNRh_0.1-derived sample, which exhibited excellent long-term stability for 40 hours on stream as well as high propane conversion (X_C3H8 = 92%) and H₂ selectivity (S_H2 = 97%) at 600 °C.

SUBMITTER: Ramantani T

PROVIDER: S-EPMC8401020 | biostudies-literature |

REPOSITORIES: biostudies-literature

ACCESS DATA

Similar Datasets

Project description:To elucidate the role of earth alkaline doping in perovskite-based dry reforming of methane (DRM) catalysts, we embarked on a comparative and exemplary study of a Ni-based Sm perovskite with and without Sr doping. While the Sr-doped material appears as a structure-pure Sm1.5Sr0.5NiO4 Ruddlesden Popper structure, the undoped material is a NiO/monoclinic Sm2O3 composite. Hydrogen pre-reduction or direct activation in the DRM mixture in all cases yields either active Ni/Sm2O3 or Ni/Sm2O3/SrCO3 materials, with albeit different short-term stability and deactivation behavior. The much smaller Ni particle size after hydrogen reduction of Sm1.5Sr0.5NiO4, and of generally all undoped materials stabilizes the short and long-term DRM activity. Carbon dioxide reactivity manifests itself in the direct formation of SrCO3 in the case of Sm1.5Sr0.5NiO4, which is dominant at high temperatures. For Sm1.5Sr0.5NiO4, the CO : H2 ratio exceeds 1 at these temperatures, which is attributed to faster direct carbon dioxide conversion to SrCO3 without catalytic DRM reactivity. As no Sm2O2CO3 surface or bulk phase as a result of carbon dioxide activation was observed for any material - in contrast to La2O2CO3 - we suggest that oxy-carbonate formation plays only a minor role for DRM reactivity. Rather, we identify surface graphitic carbon as the potentially reactive intermediate. Graphitic carbon has already been shown as a crucial reaction intermediate in metal-oxide DRM catalysts and appears both for Sm1.5Sr0.5NiO4 and NiO/monoclinic Sm2O3 after reaction as crystalline structure. It is significantly more pronounced for the latter due to the higher amount of oxygen-deficient monoclinic Sm2O3 facilitating carbon dioxide activation. Despite the often reported beneficial role of earth alkaline dopants in DRM catalysis, we show that the situation is more complex. In our studies, the detrimental role of earth alkaline doping manifests itself in the exclusive formation of the sole stable carbonated species and a general destabilization of the Ni/monoclinic Sm2O3 interface by favoring Ni particle sintering.

Dataset Information

Propane Steam Reforming over Catalysts Derived from Noble Metal (Ru, Rh)-Substituted LaNiO₃ and La_0.8Sr_0.2NiO₃ Perovskite Precursors.

Similar Datasets

OmicsDI is part of the ELIXIR infrastructure

Tweets

Dataset Information

Propane Steam Reforming over Catalysts Derived from Noble Metal (Ru, Rh)-Substituted LaNiO3 and La0.8Sr0.2NiO3 Perovskite Precursors.

Similar Datasets

OmicsDI is part of the ELIXIR infrastructure

Tweets

Propane Steam Reforming over Catalysts Derived from Noble Metal (Ru, Rh)-Substituted LaNiO₃ and La_0.8Sr_0.2NiO₃ Perovskite Precursors.