2023 article
Surfactants Used in Colloidal Synthesis Modulate Ni Nanoparticle Surface Evolution for Selective CO2 Hydrogenation
Wei, X., Johnson, G., Ye, Y., Cui, M., Yu, S.-W., Ran, Y., … Zhang, S. (2023, June 22). JOURNAL OF THE AMERICAN CHEMICAL SOCIETY.
UN Sustainable Development Goal Categories
7. Affordable and Clean Energy
(Web of Science)
13. Climate Action
(Web of Science)
Source: Web Of Science
Added: July 19, 2023
Colloidal chemistry holds promise to prepare uniform and size-controllable pre-catalysts; however, it remains a challenge to unveil the atomic-level transition from pre-catalysts to active catalytic surfaces under the reaction conditions to enable the mechanistic design of catalysts. Here, we report an ambient-pressure X-ray photoelectron spectroscopy study, coupled with in situ environmental transmission electron microscopy, infrared spectroscopy, and theoretical calculations, to elucidate the surface catalytic sites of colloidal Ni nanoparticles for CO2 hydrogenation. We show that Ni nanoparticles with phosphine ligands exhibit a distinct surface evolution compared with amine-capped ones, owing to the diffusion of P under oxidative (air) or reductive (CO2 + H2) gaseous environments at elevated temperatures. The resulting NiPx surface leads to a substantially improved selectivity for CO production, in contrast to the metallic Ni, which favors CH4. The further elimination of surface metallic Ni sites by designing multi-step P incorporation achieves unit selectivity of CO in high-rate CO2 hydrogenation.