1. Stable seawater oxidation with a self-healing oxygen-evolving catalystXiaojian Zhang, Chao Feng, Zeyu Fan, Beibei Zhang, Yequan Xiao, Andraž Mavrič, Nadiia Pastukhova, Matjaz 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: 133; Prenosov: 0
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2. Time-of-flight photoconductivity investigation of high charge carrier mobility in Ti3C2Tx MXenes thin-filmJurij Urbančič, Erika Tomsič, Manisha Chhikara, Nadiia Pastukhova, Vadym Tkachuk, Andraž Mavrič, Gvido Bratina, Egon Pavlica, 2023, izvirni znanstveni članek Opis: Charge transport through a randomly oriented multilayered network of two-dimensional (2D) Ti3C2Tx (where Tx is the surface termination and corresponds to O, OH and F) was studied using time-of-flight photoconductivity (TOFP) method, which is highly sensitive to the distribution of charge carrier velocities. We prepared samples comprising Ti3C2Tx with thickness of 12 nm or 6-monolayers. MXene flakes of size up to 16 μm were randomly deposited on the surface by spin-coating from water solution. Using TOFP, we have measured electron mobility that reached values up to 279 cm2/Vs and increase with electric-field in a Poole-Frenkel manner. These values are approximately 50 times higher than previously reported field-effect mobility. Interestingly, our zero-electric-field extrapolate approaches electron mobility measured using terahertz absorption method, which represents intra-flake transport. Our data suggest that macroscopic charge transport is governed by two distinct mechanisms. The high mobility values are characteristic for the intra-flake charge transport via the manifold of delocalized states. On the other hand, the observed Poole-Frenkel dependence of charge carrier mobility on the electric field is typical for the disordered materials and suggest the existence of an important contribution of inter-flake hopping to the overall charge transport.
Ključne besede: Charge transport in multilayered network of flakes, Time-of-flight photoconductivity, MXene exfoliation, High-mobility solution-cast thin-film, Semiconducting mxene
Objavljeno v RUNG: 31.03.2023; Ogledov: 198; Prenosov: 0
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3. Photoexcited charge mobility in quasi two-dimensional polyacetyleneNadiia Pastukhova, Kejun Liu, Renhao Dong, Gvido Bratina, Xinliang Feng, Egon Pavlica, 2022, objavljeni povzetek znanstvenega prispevka na konferenci Opis: Two-dimensional conjugated polymers (2DCPs) have been described and recognised as crystalline, one- to two-layer polymer nanosheets prepared by 2D covalent polymerization exhibiting strong in-plane π-electron delocalization with two orthogonal directions and weak out-of-plane π-π stacking.[1,2] The extension of polymer dimensionality into two dimensions improves the alignment of individual polymer sheets and overcomes the limitations associated with charge carrier hopping between polymer chains in one-dimensional and crosslinked polymers.[3] Compared to other two-dimensional materials such as graphene or transition metal dichalcogenides, 2DCPs offer a high degree of flexibility in chemical design and are compatible with liquid-based processing methods. Various 2DCPs have been synthesised by surfactant monolayer-assisted interfacial synthesis (SMAIS).[5]
Of particular interest is the photoresponse of these materials due to their tunable properties, such as bandgap and associated wavelength-dependent photoexcitation, which enables a wide range of applications in optoelectronic devices. Using time-of-flight photoconductivity (TOF-PC) measurements [4], we investigate the charge transport properties of 2D polyacetylene prepared by SMAIS method. We preform TOF-PC measurement of 2D polyacetylene using a focused nanosecond pulse laser at 325 nm and electrode separation of 250 µm. From the bias polarity and time duration of the photocurrent, we can determine the polarity, velocity and mobility of photoexcited charge carriers as a function of applied bias voltage and excitation wavelength. Using excitation at 325 m, we observed an electron mobility in the range of 150 cm2 V-1 s-1, which is in the realm of most advances small-molecule single-crystal organic semiconductors and almost an order of magnitude higher than linear polymeric semiconductors.
Ključne besede: Two-dimensional conjugated polymers, 2DCPs, 2Dpolymers, charge mobility, time-of-flight photoconductivity
Objavljeno v RUNG: 29.11.2022; Ogledov: 347; Prenosov: 0
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4. Plasma-enhanced atomic layer deposition of amorphous Ga2O3 for solar-blind photodetectionZe-Yu Fan, Min-Ji Yang, Bo-Yu Fan, Andraž Mavrič, Nadiia Pastukhova, Matjaž Valant, Bo-Lin Li, Kuang Feng, Dong-Liang Liu, Guang-Wei Deng, Qiang Zhou, Yan-Bo Li, 2022, izvirni znanstveni članek Opis: Wide-bandgap gallium oxide (Ga2O3) is one of the most promising semiconductor materials for solar-blind (200 nm–280 nm) photodetection. In its amorphous form, a-Ga2O3 maintains its intrinsic optoelectronic properties while can be prepared at a low growth temperature, thus is compatible with Si integrated circuits (ICs) technology. Herein, the a-Ga2O3 film is directly deposited on pre-fabricated Au interdigital electrodes by plasma enhanced atomic layer deposition (PE-ALD) at a growth temperature of 250 °C. The stoichiometric a-Ga2O3 thin film with a low defect density is achieved owing to the mild PE-ALD condition. As a result, the fabricated Au/a-Ga2O3/Au photodetector shows a fast time response, high responsivity, and excellent wavelength selectivity for solar-blind photodetection. Furthermore, an ultra-thin MgO layer is deposited by PE-ALD to passivate the Au/a-Ga2O3/Au interface, resulting in the responsivity of 788 A/W (under 254 nm at 10 V), a 250-nm-to-400-nm rejection ratio of 9.2×103, and the rise time and the decay time of 32 ms and 6 ms, respectively. These results demonstrate that the a-Ga2O3 film grown by PE-ALD is a promising candidate for high-performance solar-blind photodetection and potentially can be integrated with Si ICs for commercial production.
Ključne besede: Amorphous gallium oxide, Passivation layer, Plasma enhanced atomic layer deposition, Responsivity, Solar-blind photodetector
Objavljeno v RUNG: 25.10.2022; Ogledov: 422; Prenosov: 0
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5. Enhancement of indacenodithiophene–benzothiadiazole copolymer field-effect mobility with MXenesJurij Urbančič, Nadiia Pastukhova, Manisha Chhikara, Hu Chen, Iain Mcculloch, Huanhuan Shi, Ali Shaygan Nia, Xinliang Feng, Egon Pavlica, Gvido Bratina, 2022, objavljeni povzetek znanstvenega prispevka na konferenci Opis: The predominant mode of charge carrier transport in thin layers of organic semiconductors (OSs) is thermally-activated hopping between localized states. This results in lower charge mobility compared to inorganic semiconductors precluding the use of OSs in high-speed electronic devices. Therefore, significant effort is invested to improve charge carrier mobility of OS thin layers, which form the basis of most of the organic electronic devices. Recent advances in the field of two-dimensional (2D) materials stimulated their use as addition to OS thin layers to boost the charge carrier mobility. MXenes promise to deliver most of the benefits of 2D materials coupled with large scale fabrication capability. Herein we examined Ti3C2X (X is O or OH group termination) MXene, as a candidate to improve charge carrier mobility in thin layer of indacenodithiophene-co-benzothiadiazole (IDTBT), a polymer exhibiting high electron mobility in defect-free crystalline layers. In our work we demonstrate that improvement in electron mobility in solution-cast IDTBT thin layers can be achieved by depositing a non-connected network of MXene flakes at the gate-dielectric/IDBT interface. Bottom-gate field-effect transistors (FETs) comprising of Au electrodes on n-doped silicon wafer covered with 230 nm of thermally deposited SiO2 were prepared and characterized. Charge carrier mobilities determined from transfer characteristics of FETs composing neat IDTBT channels were found to be in the range of 1 - 2×10−2 cm2/Vs. Devices comprising MXene flakes at the interface between SiO2 and IDTBT, instead exhibited a factor of four increase in electron mobility, while preserving the on/off ratio of 104.
Ključne besede: MXene, IDTBT, charge carrier mobility, OFET
Objavljeno v RUNG: 20.10.2022; Ogledov: 414; Prenosov: 4
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6. Coevaporation of doped inorganic carrier-selective layers for high-performance inverted planar perovskite solar cellsJiexuan 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: 913; Prenosov: 111
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7. Interface engineering of Ta[sub]3N[sub]5 thin film photoanode for highly efficient photoelectrochemical water splittingJie 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: 967; Prenosov: 68
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8. Atomic layer deposition for the photoelectrochemical applicationsNadiia 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: 1586; Prenosov: 134
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9. A pyrrolopyridazinedione-based copolymer for fullerene-free organic solar cellsAstrid-Caroline Knall, Samuel Rabensteiner, Sebastian F. Hoefler, Matiss Reinfelds, Mathias Hobisch, Heike M. A. Ehmann, Nadiia Pastukhova, Egon Pavlica, Gvido Bratina, Illie Hanzu, Shuguang Wen, Renqiang Yang, Gregor Trimmel, Thomas Rath, 2021, izvirni znanstveni članek Opis: The recent success of non-fullerene acceptors in organic photovoltaics also entails a change in the requirements to the polymer donor in terms of optical and morphological properties leading to a demand for novel conjugated polymers. Herein, we report on the synthesis of a 1,4-bis-(thiophene-2-yl)-pyrrolopyridazinedione based copolymer with 2-ethylhexyl substituents on the pyrrolopyridazinedione moiety. A 2D conjugated benzodithiophene (BDT) was chosen as comonomer. The resulting copolymer T-EHPPD-T-EHBDT showed a molecular weight of 10.2 kDa, an optical band gap of 1.79 eV, a hole mobility of 1.8 × 10−4 cm2 V−1 s−1 and a preferred face-on orientation with regard to the substrate. The comparably wide band gap as well as the determined energy levels (HOMO: −5.47 eV, LUMO: −3.68 eV) match well with the narrow band gap non-fullerene acceptor ITIC-F, which was used as the acceptor phase in the bulk heterojunction absorber layers in the investigated solar cells. The solar cells, prepared in inverted architecture, revealed power conversion efficiencies up to 7.4% using a donor:acceptor ratio of 1 : 1 in the absorber layer.
Ključne besede: non-fullerene solar cells, charge transport, charge mobility, power conversion efficiency
Objavljeno v RUNG: 27.01.2021; Ogledov: 1803; Prenosov: 0
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