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

Nanomaterials

Yifei Zhu¹  Jiao Wang²  Gang Cheng²  Xiaochen Xiang²  Peng Cui²  Zuliang Du²  Junmeng Guo²  Xue Shi²  Bao Zhang²  Sumin Li²  Ke Zhao²  Wanyu Shang²  Guangqin Gu² 

[1] Institute of Aero-Engine, School of Mechanical Engineering, Xi’an Jiaotong University, Xi’an 710049, China;Key Lab for Special Functional Materials, Ministry of Education, National & Local Joint Engineering Research Center for High-Efficiency Display and Lighting Technology, School of Materials Science and Engineering, Collaborative Innovation Center of Nano Functional Materials and Applications, Henan University, Kaifeng 475004, China;

关键词: triboelectric nanogenerator;    mechanical energy;    dioxygen activation;    triboelectric corona plasma;    O₂⁻ reactive species;    spin conversion;   

DOI  :  10.3390/nano11123408

来源: DOAJ

【 摘 要 】

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.

【 授权许可】

Unknown