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  • Title: Probing the Reaction Mechanism in CO2 Hydrogenation on Bimetallic Ni/Cu(100) with Near-Ambient Pressure X-Ray Photoelectron Spectroscopy.
    Author: Ren Y, Xin C, Hao Z, Sun H, Bernasek SL, Chen W, Xu GQ.
    Journal: ACS Appl Mater Interfaces; 2020 Jan 15; 12(2):2548-2554. PubMed ID: 31850736.
    Abstract:
    Bimetallic Ni-Cu catalysts feature high activity in CO2 hydrogenation. However, the primary surface intermediates during reaction are still elusive, making the understanding of the reaction mechanism inadequate. Herein, taking advantage of near-ambient pressure X-ray photoelectron spectroscopy (NAP-XPS), we focused on the mechanistic exploration of CO2 hydrogenation on the Ni/Cu(100) model catalyst under millibar pressures. We show that CO2 dissociates into CO and atomic oxygen on the Ni/Cu(100) surface and gives rise to the formation of chemisorbed O and nickel oxide (NiO). The CO3* species is formed through the reaction of CO2 with surface oxygen during CO2 activation. With the presence of H2, the conversion of adsorbed CO3* into the formate intermediate, HCOO*, is unambiguously demonstrated by the C 1s and O 1s core-level spectra as well as ultraviolet photoelectron spectroscopy. Based on these observations, we conclude that the CO2 hydrogenation route via CO2 dissociation, the formation of CO3*, the conversion of CO3* to formate, and the ensuing hydrogenation of formate to methanol on the Ni-Cu catalyst are feasible.
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