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1.
Sci Bull (Beijing) ; 2024 Jun 28.
Article in English | MEDLINE | ID: mdl-38987090

ABSTRACT

Elastic strain in Cu catalysts enhances their selectivity for the electrochemical CO2 reduction reaction (eCO2RR), particularly toward the formation of multicarbon (C2+) products. However, the reasons for this selectivity and the effect of catalyst precursors have not yet been clarified. Hence, we employed a redox strategy to induce strain on the surface of Cu nanocrystals. Oxidative transformation was employed to convert Cu nanocrystals to CuxO nanocrystals; these were subsequently electrochemically reduced to form Cu catalysts, while maintaining their compressive strain. Using a flow cell configuration, a current density of 1 A/cm2 and Faradaic efficiency exceeding 80% were realized for the C2+ products. The selectivity ratio of C2+/C1 was also remarkable at 9.9, surpassing that observed for the Cu catalyst under tensile strain by approximately 7.6 times. In-situ Raman and infrared spectroscopy revealed a decrease in the coverage of K+ ion-hydrated water (K·H2O) on the compressively strained Cu catalysts, consistent with molecular dynamics simulations and density functional theory calculations. Finite element method simulations confirmed that reducing the coverage of coordinated K·H2O water increased the probability of intermediate reactants interacting with the surface, thereby promoting efficient C-C coupling and enhancing the yield of C2+ products. These findings provide valuable insights into targeted design strategies for Cu catalysts used in the eCO2RR.

2.
iScience ; 26(10): 108054, 2023 Oct 20.
Article in English | MEDLINE | ID: mdl-37822502

ABSTRACT

Peroxymonosulfate (PMS)-based advanced oxidation processes in liquid phase systems can actively degrade toluene. In this work, the catechol structural surfactant was introduced to synthesize the dispersed and homogeneous CoFe2O4 nanospheres and embedded into MoS2 nanoflowers to form magnetically separable heterojunction catalysts. The innovative approach effectively mitigated the traditionally low reduction efficiency of transition metal ions during the heterogeneous activation process. In CoFe2O4/MoS2/PMS system, the toluene removal efficiency remained 95% within 2 h. The contribution of SO4⋅-, ·O2-, ·OH, and 1O2 was revealed by radical quenching experiment and electron paramagnetic resonance spectroscopy. The results illustrated that MoS2 offers ample reduction sites for facilitating PMS activation via Fe3+/Fe2+ redox interactions. Furthermore, an investigation into the toluene degradation pathway within the CoFe2O4/MoS2/PMS system revealed its capability to suppress the formation of toxic byproducts. This ambient-temperature liquid-phase method presented promising route for the removal of industrial volatile organic pollutants.

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