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1.
Designing atomic interface in ▫$Sb_2S_3/CdS$▫ heterojunction for efficient solar water splitting
Minji Yang, Zeyu Fan, Jinyan Du, Chao Feng, Ronghua Li, Beibei Zhang, Nadiia Pastukhova, Matjaž Valant, Matjaž Finšgar, Andraž Mavrič, Yanbo Li, 2024, izvirni znanstveni članek

Opis: In the emerging Sb2S3‐based solar energy conversion devices, a CdS buffer layer prepared by chemical bath deposition is commonly used to improve the separation of photogenerated electron‐hole pairs. However, the cation diffusion at the Sb2S3/CdS interface induces detrimental defects but is often overlooked. Designing a stable interface in the Sb2S3/CdS heterojunction is essential to achieve high solar energy conversion efficiency. As a proof of concept, this study reports that the modification of the Sb2S3/CdS heterojunction with an ultrathin Al2O3 interlayer effectively suppresses the interfacial defects by preventing the diffusion of Cd2+ cations into the Sb2S3 layer. As a result, a water‐splitting photocathode based on Ag:Sb2S3/Al2O3/CdS heterojunction achieves a significantly improved half‐cell solar‐to‐hydrogen efficiency of 2.78% in a neutral electrolyte, as compared to 1.66% for the control Ag:Sb2S3/CdS device. This work demonstrates the importance of designing atomic interfaces and may provide a guideline for the fabrication of high‐performance stibnite‐type semiconductor‐based solar energy conversion devices.
Ključne besede: alumina, defect passivation, interface engineering, photoelectrochemical water splitting
Objavljeno v RUNG: 11.03.2024; Ogledov: 152; Prenosov: 2
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2.
Infrared spectra in amorphous alumina
Luigi Giacomazzi, Nikita S Shcheblanov, Mikhail E Povarnitsyn, Yanbo Li, Andraž Mavrič, Barbara Zupančič, Jože Grdadolnik, Alfredo Pasquarello, zaključena znanstvena zbirka raziskovalnih podatkov

Opis: We present a combined study based on experimental measurements of infrared (IR) dielectric function and first-principles calculations of IR spectra and vibrational density of states (VDOS) of amorphous alumina (am-Al₂O₃). In particular, we show that the main features of the imaginary part of the dielectric function ε₂(ω) at ~380 and 630 cm-¹ are related to the motions of threefold coordinated oxygen atoms, which are the vast majority of oxygen atoms in am-Al₂O₃. Our analysis (involving three model structures) provides an alternative point of view with respect to an earlier suggested assignment of the vibrational modes, which relates them to the stretching and bending vibrational modes of AlOₙ (n = 4, 5, and 6) polyhedra. Our assignment is based on the additive decomposition of the VDOS and ε₂(ω) spectra, which shows that: (i) the band at ~380 cm-¹ features oxygen motions occurring in a direction normal to the plane defined by the three nearest-neighbor aluminum atoms, i.e. out-of-plane motions of oxygen atoms; (ii) Al-O stretching vibrations (i.e. in-plane motions of oxygen atoms) appear at frequencies above ~500 cm-¹, which characterize the vibrational modes underlying the band at ~630 cm-¹.
Ključne besede: amorphous alumina, infrared spectra, first-principles calculations
Objavljeno v RUNG: 15.09.2023; Ogledov: 686; Prenosov: 7
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3.
Infrared spectra in amorphous alumina : a combined ab initio and experimental study
Luigi Giacomazzi, Nikita S. Shcheblanov, Mikhail E. Povarnitsyn, Yanbo Li, Andraž Mavrič, Barbara Zupančič, Jože Grdadolnik, Alfredo Pasquarello, 2023, izvirni znanstveni članek

Opis: We present a combined study based on the experimental measurements of an infrared (IR) dielectric function and first-principles calculations of IR spectra and the vibrational density of states (VDOS) of amorphous alumina (am−Al2O3). In particular, we show that the main features of the imaginary part of the dielectric function ε2(ω) at ∼380 and 630 cm−1 are related to the motions of threefold-coordinated oxygen atoms, which are the vast majority of oxygen atoms in am-Al2O3. Our analysis provides an alternative point of view with respect to an earlier suggested assignment of the vibrational modes, which relates them to the stretching and bending vibrational modes of AlOn (n=4, 5, and 6) polyhedra. Our assignment is based on the additive decomposition of the VDOS and ε2(ω) spectra, which shows that (i) the band at ∼380cm−1 features oxygen motions occurring in a direction normal to the plane defined by the three nearest-neighbor aluminum atoms, i.e., out-of-plane motions of oxygen atoms; (ii) Al-O stretching vibrations (i.e., in-plane motions of oxygen atoms) appear at frequencies above ∼500cm−1, which characterize the vibrational modes underlying the band at ∼630cm−1. Aluminum and fourfold-coordinated oxygen atoms contribute uniformly to the VDOS and ε2(ω) spectra in the frequency region ∼350–650 cm−1 without causing specific features. Our numerical results are in good agreement with the previous and presently obtained experimental data on the IR dielectric function of am−Al2O3 films. Finally, we show that the IR spectrum can be modeled successfully by assuming isotropic Born charges for aluminum atoms and fourfold-coordinated oxygen atoms, while requiring the use of three parameters, defined in a local reference frame, for the anisotropic Born charges of threefold-coordinated oxygen atoms.
Ključne besede: dielectric properties, microstructure, amorphous materials, density functional calculations, infrared techniques, aluminium oxide
Objavljeno v RUNG: 10.05.2023; Ogledov: 1119; Prenosov: 6
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4.
Stable seawater oxidation with a self-healing oxygen-evolving catalyst
Xiaojian Zhang, Chao Feng, Zeyu Fan, Beibei Zhang, Yequan Xiao, Andraž Mavrič, Nadiia Pastukhova, Matjaž Valant, Yi-Fan Han, Yanbo Li, 2023, izvirni znanstveni članek

Opis: Direct seawater electrolysis is key to massive hydrogen fuel production without the depletion of precious freshwater resources and the need for high-purity electrolytes. However, the presence of high-concentration chloride ions (Cl−) and alkaline-earth metal ions (Mg2+, Ca2+) poses great challenges to the stability and selectivity of the catalysts for seawater splitting. Here, we demonstrate a self-healing oxygen evolution reaction (OER) catalyst for long-term seawater electrolysis. By suppressing the competitive chlorine evolution reaction and precipitating the alkaline-earth metal ions through an alkaline treatment of the seawater, stable seawater oxidation is achieved owing to the self-healing ability of the borate-intercalated nickel–cobalt–iron oxyhydroxides (NiCoFe-Bi) OER catalyst under highly-alkaline conditions. The self-healing NiCoFe-Bi catalyst achieves stable seawater oxidation at a large current density of 500 mA cm−2 for 1000 h with near unity Faraday efficiency. Our results have demonstrated strong durability and high OER selectivity of the self-healing catalyst under harsh conditions, paving the way for industrial large-scale seawater electrolysis.
Ključne besede: chemistry, electrocatalysis, seawater oxidation, oxygen evolution reaction
Objavljeno v RUNG: 08.05.2023; Ogledov: 998; Prenosov: 2
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5.
Coevaporation of doped inorganic carrier-selective layers for high-performance inverted planar perovskite solar cells
Jiexuan Jiang, Andraž Mavrič, Nadiia Pastukhova, Matjaž Valant, Qiugui Zeng, Zeyu Fan, Beibei Zhang, Yanbo Li, 2022, izvirni znanstveni članek

Opis: Inorganic carrier selective layers (CSLs), whose conductivity can be effectively tuned by doping, offer low-cost and stable alternatives for their organic counterparts in perovskite solar cells (PSCs). Herein, we employ a dual-source electron-beam co-evaporation method for the controlled deposition of copper-doped nickel oxide (Cu:NiO) and tungsten-doped niobium oxide (W:Nb2O5) as hole and electron transport layers, respectively. The mechanisms for the improved conductivity using dopants are investigated. Owing to the improved conductivity and optimized band alignment of the doped CSLs, the all-inorganic-CSLs-based PSCs achieves a maximum power conversion efficiency (PCE) of 20.47%. Furthermore, a thin titanium buffer layer is inserted between the W:Nb2O5 and the silver electrode to prevent the halide ingression and improve band alignment. This leads to a further improvement of PCE to 21.32% and a long-term stability (1200 h) after encapsulation. Finally, the large-scale applicability of the doped CSLs by co-evaporation is demonstrated for the device with 1 cm2 area showing a PCE of over 19%. Our results demonstrate the potential application of the co-evaporated CSLs with controlled doping in PSCs for commercialization.
Ključne besede: carrier selective layers, Cu-doped nickel oxide, electron-beam evaporation, perovskite solar cells, W-doped niobium oxide
Objavljeno v RUNG: 17.03.2022; Ogledov: 1696; Prenosov: 121
.pdf Celotno besedilo (1,38 MB)
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6.
Interface engineering of Ta[sub]3N[sub]5 thin film photoanode for highly efficient photoelectrochemical water splitting
Jie Fu, Zeyu Fan, Mamiko Nakabayashi, Huanxin Ju, Nadiia Pastukhova, Yequan Xiao, Chao Feng, Naoya Shibata, Kazunari Domen, Yanbo Li, 2022, izvirni znanstveni članek

Opis: Interface engineering is a proven strategy to improve the efficiency of thin film semiconductor based solar energy conversion devices. Ta3N5 thin film photoanode is a promising candidate for photoelectrochemical (PEC) water splitting. Yet, a concerted effort to engineer both the bottom and top interfaces of Ta3N5 thin film photoanode is still lacking. Here, we employ n-type In:GaN and p-type Mg:GaN to modify the bottom and top interfaces of Ta3N5 thin film photoanode, respectively. The obtained In:GaN/Ta3N5/Mg:GaN heterojunction photoanode shows enhanced bulk carrier separation capability and better injection efficiency at photo- anode/electrolyte interface, which lead to a record-high applied bias photon-to-current efficiency of 3.46% for Ta3N5-based photoanode. Furthermore, the roles of the In:GaN and Mg:GaN layers are distinguished through mechanistic studies. While the In:GaN layer con- tributes mainly to the enhanced bulk charge separation efficiency, the Mg:GaN layer improves the surface charge inject efficiency. This work demonstrates the crucial role of proper interface engineering for thin film-based photoanode in achieving efficient PEC water splitting.
Ključne besede: photocatalysis, renewable energy
Objavljeno v RUNG: 09.02.2022; Ogledov: 1676; Prenosov: 73
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7.
Atomic layer deposition for the photoelectrochemical applications
Nadiia Pastukhova, Andraž Mavrič, Yanbo Li, 2021, pregledni znanstveni članek

Opis: Substantial progress has been made in the photoelectrochemical (PEC) field to understand the photoelectrode behavior, semiconductor‐electrolyte interface, and photocorrosion, enabling new photoelectrode architectures with higher photocurrent, reduced photovoltage losses, and longer lifetime. Nevertheless, for practical PEC applications additional efforts are still needed to optimize all components of the photoelectrodes, including the light absorbing semiconductors, the layers for charge extraction, charge transfer, corrosion protection, and catalysis. In this regard, atomic layer deposition (ALD) offers new opportunities due to the monolayer‐by‐monolayer deposition approach, allowing preparation of conformal films with precisely controlled thickness and composition. As the ALD instruments are becoming widely accessible, this review aims to make an overview of the applications for photoelectrodes fabrication. The deposition of semiconductors onto flat and nano‐textured substrates, the deposition of ultrathin interlayers to ease charge transport by energy band alignment and surface states passivation, the deposition of corrosion protection layers, and finally, the possibilities for high catalyst dispersion is presented.
Ključne besede: atomic layer deposition, charge recombination, charge transfer, photocorrosion, photoelectrochemical water splitting
Objavljeno v RUNG: 25.02.2021; Ogledov: 2165; Prenosov: 138
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8.
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