Nitrogen-doped graphene-supported single atoms convert CO2 to CO, but fail to provide further hydrogenation to methane – a finding attributable to the weak adsorption of CO intermediates. To regulate the adsorption energy, here we investigate the metal-supported single atoms to enable CO2 hydrogenation. We find a copper-supported iron-single-atom catalyst producing a high-rate methane. Density functional theory calculations and in-situ Raman spectroscopy show that the iron atoms attract surrounding intermediates and carry out hydrogenation to generate methane. The catalyst is realized by assembling iron phthalocyanine on the copper surface, followed by in-situ formation of single iron atoms during electrocatalysis, identified using operando X-ray absorption spectroscopy. The copper-supported iron-single-atom catalyst exhibits a CO2-to-methane Faradaic efficiency of 64% and a partial current density of 128 mA cm−2, while the nitrogen-doped graphene-supported one produces only CO. The activity is 32 times higher than a pristine copper under the same conditions of electrolyte and bias.
We report an effective route for the preparation of layered reduced graphene oxide (rGO) with uniformly coated polyaniline (PANI) layers. These nanocomposites are synthesized by chemical oxidative polymerization of aniline monomer in the presence of layered rGO. SEM, TEM, X-ray photoelectron spectroscopy (XPS), FTIR, and Raman spectroscopy analysis results demonstrated that reduced graphene oxide-polyaniline (rGO-PANI) nanocomposites are successfully synthesized. Because of synergistic effects, rGO-PANI nanocomposites prepared by this approach exhibit excellent capacitive performance with a high specific capacitance of 286 F g(-1) and high cycle reversibility of 94 % after 2000 cycles.
The electronic configuration is crucial in governing the binding strength of intermediates with catalysts, yet it is still challenging to control the catalysts' surface electronic spin state. Here, it is demonstrated that through surface metal–organic framework transformation followed by acid etching, the electronic spin state of surface Co3+ ions on spinel Co3O4 can be transformed from t2g6 to the high electronic spin state of t2g4eg2 by expanding the surface lattice constant, which significantly enhances the overlap of the eg orbital of cobalt with the oxygen adsorbates, and greatly improves the intermediates adsorption and thus the oxygen evolution reaction activity. The high electronic spin rich Co3O4 electrode exhibits an anodic current density of 10 mA cm−2 at an overpotential of 280 mV. The finding offers a rational design strategy to manipulate the electronic spin state of catalyst and the hybridization of molecular orbitals in water electrolysis.
Abstractβ-Ga2O3 thin films with both a 45 nm Si-doped conductive epilayer and unintentionally doped epilayer were grown on c-plane sapphire substrate by metalorganic chemical vapor deposition. β-Ga2O3 based metal–oxide–semiconductor field-effect transistors (MOSFETs) were fabricated with gate recess depths of 20 nm and 40 nm (it indicated gate depth with 70 nm and 50 nm, respective), respectively, and without said recessing process. The conductivity of β-Ga2O3 epilayers was improved through low in situ doping using a tetraethoxysilane precursor to increase MOSFET forward current density. After recessing, MOSFET operation was transferred from depletion to enhanced mode. In this study, the maximum breakdown voltage of the recessed 40 nm transistor was 770 V. The etching depth of a recessed-gate device demonstrates its influence on device electrical performance.
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