Catalytic decomposition of organic/inorganic peroxides via 1-3D carbon matrices: empirical and quantum-chemical study
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Catalytic decomposition of organic/inorganic peroxides via 1-3D carbon matrices: empirical and quantum-chemical study K. V. Voitko1 · E. M. Demianenko2 · V. S. Kuts2 · O. M. Bakalinska1 · A. G. Grebenyuk2 · M. T. Kartel1 Received: 4 August 2020 / Accepted: 18 October 2020 / Published online: 29 October 2020 © Akadémiai Kiadó, Budapest, Hungary 2020
Abstract The catalytic decomposition of the inorganic (hydrogen peroxide) and organic (benzoyl and lauroyl) peroxides by a different type of carbon matrices has been investigated. The activity of the carbon-based catalyst, such as carbon nanotubes (1D), graphene (2D), activated carbon (3D), and their modified forms (O- and N-doped) was analyzing and comparing. The effects of the carbon’s electronic structure on catalytic performance have been established by the quantum-chemical study. Obtained DFT results correlate with experimental ones and demonstrate increases in the carbon’s catalytic activity in the presence of electron-donating groups. This observation is fair despite the type of carbocatalyst as well as the type of peroxide. A comprehensive assessment of obtained results allows for the conclusion that it is the uniform mechanism of peroxides decomposition that proceeds through electron transfer. However, textural characteristics and diffusion limitations are also affecting the catalytic activity and should not be ignored, especially for 1D and 3D matrices. Keywords carbon matrix · peroxide decomposition · electron transfer · electronic structure
Electronic supplementary material The online version of this article (https://doi.org/10.1007/s1114 4-020-01891-9) contains supplementary material, which is available to authorized users. * K. V. Voitko [email protected] 1
Department of Physico‑chemistry of Carbon Materials, Chuiko Institute of Surface Chemistry, NAS of Ukraine, 17 General Naumov Str., Kyiv 03164, Ukraine
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Department of Quantum Chemistry and Chemical Physics of Nanosystems, Chuiko Institute of Surface Chemistry, NAS of Ukraine, 17 General Naumov Str., Kyiv 03164, Ukraine
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Vol.:(0123456789)
584
Reaction Kinetics, Mechanisms and Catalysis (2020) 131:583–597
Introduction Carbon matrix (CM) is a system of the polycondensed aromatic rings and basic structural elements of a wide range of solid materials (activated carbon (AC), CNT, graphene (Gr), fullerene, etc.) that are extensively used in catalysis. In this context, carbon-based materials have a set of important features such as large surface area, high porosity, and thermal stability, excellent electron conductivity, and relatively easy surface chemical tuning. Moreover, they are not expensive, do not have noxious metals, easy to handling, and could operate under different conditions that correspond to the World’s standard principles of sustainable and green chemistry. It is generally accepted, that 3D carbons, such as AC, with mixed sp+sp2+sp3 hybridization carbons, have a more disordered structure that gives a significant increase in the catalytic activity [1–4]. Simultaneously, the
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