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The Regulation of O₂ Spin State and Direct Oxidation of CO at Room Temperature Using Triboelectric Plasma by Harvesting Mechanical Energy.

ABSTRACT: Oxidation reactions play a critical role in processes involving energy utilization, chemical conversion, and pollutant elimination. However, due to its spin-forbidden nature, the reaction of molecular dioxygen (O₂) with a substrate is difficult under mild conditions. Herein, we describe a system that activates O₂ via the direct modulation of its spin state by mechanical energy-induced triboelectric corona plasma, enabling the CO oxidation reaction under normal temperature and pressure. Under optimized reaction conditions, the activity was 7.2 μmol h^-1, and the energy consumption per mole CO was 4.2 MJ. The results of kinetic isotope effect, colorimetry, and density functional theory calculation studies demonstrated that electrons generated in the triboelectric plasma were directly injected into the antibonding orbital of O₂ to form highly reactive negative ions O₂^-, which effectively promoted the rate-limiting step of O₂ dissociation. The barrier of the reaction of O₂^- ions and CO molecular was 3.4 eV lower than that of O₂ and CO molecular. This work provides an effective strategy for using renewable and green mechanical energy to realize spin-forbidden reactions of small molecules.

SUBMITTER: Shi X

PROVIDER: S-EPMC8703925 | biostudies-literature |

REPOSITORIES: biostudies-literature

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