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Start of funding 01.01.2021

In2O3/Pd(111) Catalysed CO2 Hydrogenation: Observation of In situ Surface Reconstruction

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Methanol synthesis by CO₂ hydrogenation is attractive in respect to avoiding the environmental implications associated with the production of the traditional syngas feedstock and mitigating global warming. To date, there is still a lack of efficient catalysts for alternative processes, but indium oxide, In₂O₃, is a very promising candidate in respect of selectivity and stability, two key factors that usually prevent the industrialization of CO₂ hydrogenation reactions. However, the influence of the carrier substrate of the In₂O₃ and how the reaction mechanism pathway is selected (i.e., methanol synthesis) needs to be understood more fundamentally. The present project aims at investigating the chemical and structural evolution and dynamics at the In₂O₃/Pd(111) surface and interface in situ during CO₂ hydrogenation, by combining ambient pressure X-ray photoelectron spectroscopy (APXPS) and ambient pressure scanning tunneling microscopy (APSTM).

Final report:
The grant through BaCaTeC enabled the joint investigation of In₂O₃/Pd(111) catalysts during CO2 hydrogenation by the two research groups of Prof. Barbara A. J. Lechner at TU Munich and Dr. Moni Blum at the Lawrence Berkeley National Lab. Methanol synthesis by CO₂ hydrogenation is an attractive alternative to the traditional production of syngas, which is associated with environmental pollution and thus global warming. To date, there is still a lack of efficient catalysts for alternative processes, but indium oxide, In₂O₃, is a very promising candidate both in terms of selectivity and stability.

In the project funded here, the chemical and structural evolution and dynamics at the In₂O₃/Pd(111) surface and interface during CO₂ hydrogenation were monitored. For this purpose, the expertise of the two groups in X-ray photoelectron spectroscopy and scanning tunneling microscopy under ambient pressure (APXPS and APSTM) was combined, leading to exciting results. The combination of the two methods has allowed the identification of an In-Pd mixed oxide as the active species and demonstrated that the catalyst surface exhibits a dynamic equilibrium.

In addition to the scientific output which is being prepared for publication, BaCaTeC has enabled a close collaboration between the Lechner and Blum groups. In November 2022, Moni Blum visited the lab in Munich where the In₂O₃/Pd(111) samples were investigated in the APSTM, and in June and December 2022, early career scientists from TUM traveled to Berkeley to perform APXPS measurements. BaCaTeC funding has thus contributed significantly to the continuing education of scientists in both locations. In fact, further projects between the two groups are in preparation and a more long-term collaboration is being discussed, thanks to the support from BaCaTeC.