Tetrahedral amorphous carbon (ta-C) consists of a mixture of sp(3)- and sp(2)-bonded carbon ranging from 60 to 40% (sp(3)/sp(3)+sp(2)) depending on the deposition conditions. The physical, chemical, and electrochemical properties depend on the sp(2)/sp(3) bonding ratio as well as the presence of incorporated impurities, such as hydrogen or nitrogen. The ability to grow ta-C at lower temperatures (25-100 °C) on a wider variety of substrates as compared to CVD diamond is an advantage of this material. Herein, we report on the structural and electrochemical properties of nitrogen-incorporated ta-C thin films (ta-C:N). The incorporation of nitrogen into the films decreases the electrical resistivity from 613 ± 60 (0 sccm N(2)) to 1.10 ± 0.07 Ω-cm (50 sccm N(2)), presumably by increasing the sp(2)-bonded carbon content and the connectedness of these domains. Similar to boron-doped diamond, these materials are characterized by a low background voltammetric current, a wide working potential window (~ 3 V), and relatively rapid electron-transfer kinetics for aqueous redox systems, including Fe(CN)(6)(-3/-4) and Ru(NH(3))(6)(+3/+2), without conventional pretreatment. Additionally, there is weak molecular adsorption of polar molecules (methylene blue) on the ta-C surface. Overall, the properties of the ta-C and ta-C:N electrodes are such that they could be excellent new choices for electroanalytical measurements.
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http://dx.doi.org/10.1021/ac301124r | DOI Listing |
Nat Commun
January 2025
School of Environment, Tsinghua University, Beijing, 100084, P. R. China.
Modulation of electronic spin states in cobalt-based catalysts is an effective strategy for molecule activations. Crystalline-amorphous interfaces often exhibit unique catalytic properties due to disruptions of long-range order and alterations in electronic structure. However, the mechanisms of molecule activation and spin states at interfaces remain elusive.
View Article and Find Full Text PDFAdv Mater
December 2024
WA School of Mines: Minerals, Energy and Chemical Engineering, Curtin University, Perth, WA, 6102, Australia.
ACS Appl Nano Mater
November 2024
Laboratory of Inorganic Materials and Catalysis, Department of Chemical Engineering and Chemistry, Eindhoven University of Technology, PO Box 513, Eindhoven, MB 5600, the Netherlands.
Well-defined amorphous silica-alumina (ASA) with a relatively low Al loading were synthesized by homogeneous deposition-precipitation of Al on SiO nanoparticles to understand the nature and formation of Brønsted acid sites (BAS). The amount of Al grafted relative to the silanol density was varied by variation of the size of SiO nanoparticles, reflected by their surface areas between 90 and 380 m·g. Two sets of ASA were synthesized, one aiming at a SiOH/Al ratio of 3, corresponding to the maximum amount of BAS represented by Al perturbation of SiOH groups, and the second one aimed at studying the impact of Al dispersion by using a constant Al loading (Si/Al ≈ 103).
View Article and Find Full Text PDFJ Biomed Mater Res A
January 2025
Department of Orthopaedic Surgery, Otto-von-Guericke University, Magdeburg, Germany.
Premature implant failure, a critical concern in biomedical applications, is often attributed to poor biocompatibility and vulnerability to bacterial colonization. These issues are addressed by creating an endoprosthetic material with natural biocompatibility and antibacterial properties. In this in vitro study, the relaxed and unrelaxed tetrahedral amorphous carbon (ta-C) coatings were examined, both fabricated by the improved patented Pulsed Laser Deposition (PLD) technology.
View Article and Find Full Text PDFJ Am Chem Soc
October 2024
Department Chemie, Ludwig-Maximilians-Universität München, Butenandtstraße 5-13(D), München D-81377, Germany.
The cesium-poor alkali-metal suboxidometalates CsO ( = In, Sc) were prepared from the respective cesium-rich suboxidometalates CsO by thermolysis in a dynamic vacuum at temperatures below 150 °C. They crystallize in a new structure type, comprising isolated tetrahedral oxidometalate anions [O] immersed in a matrix of metallic cesium atoms. This structural separation into alternating ionic and metallic building units is typical for subvalent compounds.
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