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

Nanomaterials ◽  
2021 ◽  
Vol 11 (12) ◽  
pp. 3408
Author(s):  
Xue Shi ◽  
Sumin Li ◽  
Bao Zhang ◽  
Jiao Wang ◽  
Xiaochen Xiang ◽  
...  

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.

2016 ◽  
Vol 18 (4) ◽  
pp. 3322-3330 ◽  
Author(s):  
Ken-Huang Lin ◽  
Shin-Pon Ju ◽  
Jia-Yun Li ◽  
Hsin-Tsung Chen

Two CO oxidation reactions (CO + O2 → CO2 + O and CO + O → CO2) were considered in the Eley–Rideal (ER) reaction mechanism.


2021 ◽  
Vol 9 (12) ◽  
pp. 4316-4321
Author(s):  
L.-B. Meng ◽  
S. Ni ◽  
Z. M. Zhang ◽  
S. K. He ◽  
W. M. Zhou

Density functional theory calculation predicts a novel ordered boron phosphorus codoped graphene realizing a widely tunable Dirac-cone gap.


2021 ◽  
Vol 12 (1) ◽  
Author(s):  
Xiaowen Chen ◽  
Mi Peng ◽  
Xiangbin Cai ◽  
Yunlei Chen ◽  
Zhimin Jia ◽  
...  

AbstractMetal nanoparticle (NP), cluster and isolated metal atom (or single atom, SA) exhibit different catalytic performance in heterogeneous catalysis originating from their distinct nanostructures. To maximize atom efficiency and boost activity for catalysis, the construction of structure–performance relationship provides an effective way at the atomic level. Here, we successfully fabricate fully exposed Pt3 clusters on the defective nanodiamond@graphene (ND@G) by the assistance of atomically dispersed Sn promoters, and correlated the n-butane direct dehydrogenation (DDH) activity with the average coordination number (CN) of Pt-Pt bond in Pt NP, Pt3 cluster and Pt SA for fundamentally understanding structure (especially the sub-nano structure) effects on n-butane DDH reaction at the atomic level. The as-prepared fully exposed Pt3 cluster catalyst shows higher conversion (35.4%) and remarkable alkene selectivity (99.0%) for n-butane direct DDH reaction at 450 °C, compared to typical Pt NP and Pt SA catalysts supported on ND@G. Density functional theory calculation (DFT) reveal that the fully exposed Pt3 clusters possess favorable dehydrogenation activation barrier of n-butane and reasonable desorption barrier of butene in the DDH reaction.


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