HAXPES measurements at room temperature were performed to evaluate the electronic structures experimentally at the BL15XU undulator beamline (40) of SPring-8. The sample ingots were cut into about 1-mm by 1-mm by 10-mm rods, fixed on a copper holder using a silver paste, and then placed in a preparation chamber (base pressure, 2.0 × 10−7 Pa) connected with a measurement chamber (base pressure, <1.0 × 10−7 Pa). After evacuation of the preparation chamber, the rods were fractured in situ to obtain a clean surface and then moved into the measurement chamber. The excitation photon energy and total energy resolution were set to 5.95 keV and 240 meV, respectively. The binding energy was referred to the Fermi level of an evaporated gold film. Details of the experimental setup are described elsewhere (40). The electric field vector of the incident beam was parallel to the photoelectron trajectory to the analyzer. Because of this geometry, a high-intensity structure originating from the s-bands at binding energies >4 eV is evident in Fig. 4 (B1 and B2) (22). We also performed the measurement for Co2FeGa0.5Ge0.5 powders before and after the alkyne hydrogenation in the presence of alkene, which indicated no surface segregation and no carbon deposition (coking or oil production) within the sensitivity, as shown in fig. S7.

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