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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, original scientific article

Abstract: 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.
Keywords: alumina, defect passivation, interface engineering, photoelectrochemical water splitting
Published in RUNG: 11.03.2024; Views: 630; Downloads: 2
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An in situ proton filter covalent organic framework catalyst for highly efficient aqueous electrochemical ammonia production
Kayaramkodath C. Ranjeesh, Sukhjot Kaur, Abdul K. Mohammed, Safa Gaber, Divyani Gupta, Khaled Badawy, Mohamed Aslam, Nirpendra Singh, Tina Škorjanc, Matjaž Finšgar, 2023, original scientific article

Abstract: The electrocatalytic nitrogen reduction reaction (NRR) driven by renewable electricity provides a green synthesis route for ammonia (NH3) production under ambient conditions but suffers from a low conversion yield and poor Faradaic efficiency (F.E.) because of strong competition from hydrogen evolution reaction (HER) and the poor solubility of N2 in aqueous systems. Herein, an in situ proton filter covalent organic framework catalyst (Ru-Tta-Dfp) is reported with inherent Ruthenium (Ru) sites where the framework controls reactant diffusion by suppressing proton supply and enhancing N2 flux, causing highly selective and efficient catalysis. The smart catalyst design results in a remarkable ammonia production yield rate of 2.03 mg h−1 mgcat−1 with an excellent F.E. of ≈52.9%. The findings are further endorsed with the help of molecular dynamics simulations and control COF systems without in situ proton filter feasibility. The results point to a paradigm shift in engineering high-performance NRR electrocatalysts for more feasible green NH3 production.
Keywords: covalent organic frameworks, ammonia, electrochemical synthesis, electrochemistry, nitrogen reduction reaction, ruthenium
Published in RUNG: 11.12.2023; Views: 840; Downloads: 6
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Utilizing structurally disordered AlMg-oxide phase in Cu/ZnO catalyst for efficient ▫$CO_2$▫ hydrogenation to methanol
Andraž Mavrič, Gregor Žerjav, Blaž Belec, Matevž Roškarič, Matjaž Finšgar, Albin Pintar, Matjaž Valant, 2023, published scientific conference contribution abstract

Keywords: carbon dioxide, methanol, catalysis
Published in RUNG: 15.09.2023; Views: 1183; Downloads: 4
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A rational design of isoindigo-based conjugated microporous n-type semiconductors for high electron mobility and conductivity
Kayaramkodath C. Ranjeesh, Ayman Rezk, Jose Ignacio Martinez, Safa Gaber, Areej Merhi, Tina Škorjanc, Matjaž Finšgar, Gisha Elizabeth Luckachan, Ali Trabolsi, Bilal R. Kaafarani, 2023, original scientific article

Abstract: The development of n-type organic semiconductors has evolved significantly slower in comparison to that of p-type organic semiconductors mainly due to the lack of electron-deficient building blocks with stability and processability. However, to realize a variety of organic optoelectronic devices, high-performance n-type polymer semiconductors are essential. Herein, conjugated microporous polymers (CMPs) comprising isoindigo acceptor units linked to benzene or pyrene donor units (BI and PI) showing n-type semiconducting behavior are reported. In addition, considering the challenges of deposition of a continuous and homogeneous thin film of CMPs for accurate Hall measurements, a plasma-assisted fabrication technique is developed to yield uniform thin films. The fully conjugated 2D networks in PI- and BI-CMP films display high electron mobility of 6.6 and 3.5 cm2 V−1 s−1, respectively. The higher carrier concentration in PI results in high conductivity (5.3 mS cm−1). Both experimental and computational studies are adequately combined to investigate structure–property relations for this intriguing class of materials in the context of organic electronics.
Keywords: conjugated microporous polymers, isoindigo, semiconductors, conductivity, electron mobility
Published in RUNG: 18.08.2023; Views: 1067; Downloads: 7
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Structural disorder of AlMg-oxide phase supporting Cu/ZnO catalyst improves efficiency and selectivity for ▫$CO_2$▫ hydrogenation to methanol
Andraž Mavrič, Gregor Žerjav, Blaž Belec, Matevž Roškarič, Matjaž Finšgar, Albin Pintar, Matjaž Valant, 2023, original scientific article

Abstract: The performance of the Cu/ZnO catalyst system with the AlMg-oxide phase is studied for CO2 hydrogenation to methanol. The catalyst is prepared by thermal treatment of the hydrotalcite phase containing intimately mixed metal cations in the hydroxide form. CuO in the presence of ZnO and disordered AlMg-oxide phase gets easily reduced to Cu during the hydrogenation reaction. Its catalytic activity at relatively low Cu metal content (∼14 at.%) remains stable during 100 hours on stream at 260 °C with constant space-time yield for methanol (∼1.8 gMeOH gcat−1 h−1) and high methanol selectivity (>85 %) The improved performance is attributed to the neutralization of surface acidity, increased number of weak basic sites in the disordered phase, and lower tendency for coke formation.
Keywords: carbon dioxide hydrogenation, heterogenous catalysis, methanol, reducibility
Published in RUNG: 02.06.2023; Views: 1300; Downloads: 15
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