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Resolving the dilemma of Fe-N-C catalysts by the selective synthesis of tetrapyrrolic active sites via an imprinting strategy
Davide Menga, Jian Liang Low, Yan-Sheng Li, Iztok Arčon, Burak Koyutürk, Friedrich Wagner, Francisco Ruiz-Zepeda, Miran Gaberšček, Beate Paulus, Tim-Patrick Fellinger, 2021, izvirni znanstveni članek

Opis: Combining the abundance and inexpensiveness of their constituent elements with their atomic dispersion, atomically dispersed Fe−N−C catalysts represent the most promising alternative to precious-metal-based materials in proton exchange membrane (PEM) fuel cells. Due to the high temperatures involved in their synthesis and the sensitivity of Fe ions toward carbothermal reduction, current synthetic methods are intrinsically limited in type and amount of the desired, catalytically active Fe− N4 sites, and high active site densities have been out of reach (dilemma of Fe−N−C catalysts). We herein identify a paradigm change in the synthesis of Fe−N−C catalysts arising from the developments of other M−N−C single-atom catalysts. Supported by DFT calculations we propose fundamental principles for the synthesis of M−N−C materials. We further exploit the proposed principles in a novel synthetic strategy to surpass the dilemma of Fe−N−C catalysts. The selective formation of tetrapyrrolic Zn−N4 sites in a tailor-made Zn−N−C material is utilized as an active-site imprint for the preparation of a corresponding Fe−N−C catalyst. By successive low- and high-temperature ion exchange reactions, we obtain a phase-pure Fe−N−C catalyst, with a high loading of atomically dispersed Fe (>3 wt %). Moreover, the catalyst is entirely composed of tetrapyrrolic Fe−N4 sites. The density of tetrapyrrolic Fe−N4 sites is more than six times as high as for previously reported tetrapyrrolic single-site Fe−N−C fuel cell catalysts
Ključne besede: Fe-N-C catalysts, selective synthesis, tetrapyrrolic active sites, EXAFS, XANES, single atom, DFT
Objavljeno v RUNG: 25.10.2021; Ogledov: 1784; Prenosov: 54
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3.
On the GeV Emission of the Type I BdHN GRB 130427A
Remo Ruffini, Rahim Moradi, Jorge Armando Rueda, Carlo Luciano Bianco, Christian Cherubini, Simonetta Filippi, Yen-Chen Chen, Mile Karlica, Narek Sahakyan, Yu Wang, She Sheng Xue, Laura Beccera, 2019, izvirni znanstveni članek

Opis: We propose that the inner engine of a type I binary-driven hypernova (BdHN) is composed of Kerr black hole (BH) in a non-stationary state, embedded in a uniform magnetic field B_0 aligned with the BH rotation axis and surrounded by an ionized plasma of extremely low density of 10^−14 g cm−3. Using GRB 130427A as a prototype, we show that this inner engine acts in a sequence of elementary impulses. Electrons accelerate to ultrarelativistic energy near the BH horizon, propagating along the polar axis, θ = 0, where they can reach energies of ~10^18 eV, partially contributing to ultrahigh-energy cosmic rays. When propagating with $\theta \ne 0$ through the magnetic field B_0, they produce GeV and TeV radiation through synchroton emission. The mass of BH, M = 2.31M ⊙, its spin, α = 0.47, and the value of magnetic field B_0 = 3.48 × 10^10 G, are determined self consistently to fulfill the energetic and the transparency requirement. The repetition time of each elementary impulse of energy ${ \mathcal E }\sim {10}^{37}$ erg is ~10^−14 s at the beginning of the process, then slowly increases with time evolution. In principle, this "inner engine" can operate in a gamma-ray burst (GRB) for thousands of years. By scaling the BH mass and the magnetic field, the same inner engine can describe active galactic nuclei.
Ključne besede: black hole physics, binaries, gamma-ray burst, neutron stars, supernovae, Astrophysics - High Energy Astrophysical Phenomena
Objavljeno v RUNG: 20.07.2020; Ogledov: 2755; Prenosov: 0
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