| 1. |
- Bharmoria, Pankaj, 1985, et al.
(författare)
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Triplet-triplet annihilation based near infrared to visible molecular photon upconversion
- 2020
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Ingår i: Chemical Society Reviews. - : Royal Society of Chemistry (RSC). - 1460-4744 .- 0306-0012. ; 49:18, s. 6529-6554
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Forskningsöversikt (refereegranskat)abstract
- Triplet-triplet annihilation based molecular photon upconversion (TTA-UC) is an exciting research area for a broad range of photonic applications due to its tunable spectral range and possible operation at non-coherent solar irradiance. Most of the TTA-UC studies are limited to Visible to Visible (Vis to Vis) energy upconversion. However, for several practical photonic applications, efficient near infrared (NIR) to Vis upconversion is preferred. Examples include, (i) photovoltaics where TTA-UC could lead to utilization of a larger part of the solar spectrum and (ii) in NIR stimulated biological applications where the deep penetration and non-invasive nature of NIR light coupled to TTA-UC offers new opportunities. Although, NIR to Vis TTA-UC is known since 2007, the recent five years have witnessed quite a progress in terms of the development of new chromophores, hybrid systems and fabrication techniques to increase the UC quantum yield at low excitation intensity. With this tutorial review we are reviewing recent progress, identifying existing challenges and discus possible future directions and opportunities.
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| 2. |
- Blomberg, Margareta R. A.
(författare)
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Activation of O(2)and NO in heme-copper oxidases - mechanistic insights from computational modelling
- 2020
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Ingår i: Chemical Society Reviews. - : Royal Society of Chemistry (RSC). - 0306-0012 .- 1460-4744. ; 49:20, s. 7301-7330
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Forskningsöversikt (refereegranskat)abstract
- Heme-copper oxidases are transmembrane enzymes involved in aerobic and anaerobic respiration. The largest subgroup contains the cytochromecoxidases (CcO), which reduce molecular oxygen to water. A significant part of the free energy released in this exergonic process is conserved as an electrochemical gradient across the membrane,viatwo processes, electrogenic chemistry and proton pumping. A deviant subgroup is the cytochromecdependent NO reductases (cNOR), which reduce nitric oxide to nitrous oxide and water. This is also an exergonic reaction, but in this case none of the released free energy is conserved. Computational studies applying hybrid density functional theory to cluster models of the bimetallic active sites in the heme-copper oxidases are reviewed. To obtain a reliable description of the reaction mechanisms, energy profiles of the entire catalytic cycles, including the reduction steps have to be constructed. This requires a careful combination of computational results with certain experimental data. Computational studies have elucidated mechanistic details of the chemical parts of the reactions, involving cleavage and formation of covalent bonds, which have not been obtainable from pure experimental investigations. Important insights regarding the mechanisms of energy conservation have also been gained. The computational studies show that the reduction potentials of the active site cofactors in the CcOs are large enough to afford electrogenic chemistry and proton pumping,i.e.efficient energy conservation. These results solve a conflict between different types of experimental data. A mechanism for the proton pumping, involving a specific and crucial role for the active site tyrosine, conserved in all CcOs, is suggested. For thecNORs, the calculations show that the low reduction potentials of the active site cofactors are optimized for fast elimination of the toxic NO molecules. At the same time, the low reduction potentials lead to endergonic reduction steps with high barriers. To prevent even higher barriers, which would lead to a too slow reaction, when the electrochemical gradient across the membrane is present, the chemistry must occur in a non-electrogenic manner. This explains why there is no energy conservation incNOR.
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| 3. |
- Du, Jian, et al.
(författare)
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Metal-organic frameworks and their derivatives as electrocatalysts for the oxygen evolution reaction
- 2021
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Ingår i: Chemical Society Reviews. - : Royal Society of Chemistry (RSC). - 0306-0012 .- 1460-4744. ; 50:4, s. 2663-2695
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Forskningsöversikt (refereegranskat)abstract
- Electrochemical water splitting is an appealing and promising approach for energy conversion and storage. As a key half-reaction of electricity-driven water splitting, the oxygen evolution reaction (OER) is a sluggish process due to the transfer of four protons and four electrons. Therefore, development of low-cost and robust OER electrocatalysts is of great importance for improving the efficiency of water splitting. Based on the merits of high surface area, rich pore structure, diverse composition and well-defined metal centers, metal-organic frameworks (MOFs) and their derivatives have been widely exploited as OER electrocatalysts. Herein, the current progress on MOFs and their derivatives for OER electrolysis is summarized, highlighting the design principle, synthetic methods and performance for MOF-based materials. In addition, the structure-performance relationships of MOFs and their derivatives toward the OER are discussed, providing valuable insights into rationally developing OER catalysts with high efficiency. The current scientific and technological challenges and future perspectives towards the purpose of sustainable industrial applications are addressed at the end.
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| 4. |
- Duo, Y, et al.
(författare)
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Noncancerous disease-targeting AIEgens
- 2023
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Ingår i: Chemical Society reviews. - : Royal Society of Chemistry (RSC). - 1460-4744 .- 0306-0012. ; 52:3, s. 1024-1067
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Tidskriftsartikel (refereegranskat)abstract
- Schematic diagram of noncancerous disease-targeting AIEgens.
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| 5. |
- Han, Jianhua, et al.
(författare)
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Understanding photochemical degradation mechanisms in photoactive layer materials for organic solar cells
- 2024
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Ingår i: Chemical Society Reviews. - 1460-4744 .- 0306-0012. ; 53:14, s. 7426-7454
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Forskningsöversikt (refereegranskat)abstract
- Over the past decades, the field of organic solar cells (OSCs) has witnessed a significant evolution in materials chemistry, which has resulted in a remarkable enhancement of device performance, achieving efficiencies of over 19%. The photoactive layer materials in OSCs play a crucial role in light absorption, charge generation, transport and stability. To facilitate the scale-up of OSCs, it is imperative to address the photostability of these electron acceptor and donor materials, as their photochemical degradation process remains a challenge during the photo-to-electric conversion. In this review, we present an overview of the development of electron acceptor and donor materials, emphasizing the crucial aspects of their chemical stability behavior that are linked to the photostability of OSCs. Throughout each section, we highlight the photochemical degradation pathways for electron acceptor and donor materials, and their link to device degradation. We also discuss the existing interdisciplinary challenges and obstacles that impede the development of photostable materials. Finally, we offer insights into strategies aimed at enhancing photochemical stability and discuss future directions for developing photostable photo-active layers, facilitating the commercialization of OSCs.
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| 6. |
- Kanyolo, Godwill Mbiti, et al.
(författare)
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Honeycomb layered oxides: Structure, energy storage, transport, topology and relevant insights
- 2021
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Ingår i: Chemical Society Reviews. - : Royal Society of Chemistry (RSC). - 1460-4744 .- 0306-0012. ; 50:6, s. 3990-4030
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Forskningsöversikt (refereegranskat)abstract
- The advent of nanotechnology has hurtled the discovery and development of nanostructured materials with stellar chemical and physical functionalities in a bid to address issues in energy, environment, telecommunications and healthcare. In this quest, a class of two-dimensional layered materials consisting of alkali or coinage metal atoms sandwiched between slabs exclusively made of transition metal and chalcogen (or pnictogen) atoms arranged in a honeycomb fashion have emerged as materials exhibiting fascinatingly rich crystal chemistry, high-voltage electrochemistry, fast cation diffusion besides playing host to varied exotic electromagnetic and topological phenomena. Currently, with a niche application in energy storage as high-voltage materials, this class of honeycomb layered oxides serves as ideal pedagogical exemplars of the innumerable capabilities of nanomaterials drawing immense interest in multiple fields ranging from materials science, solid-state chemistry, electrochemistry and condensed matter physics. In this review, we delineate the relevant chemistry and physics of honeycomb layered oxides, and discuss their functionalities for tunable electrochemistry, superfast ionic conduction, electromagnetism and topology. Moreover, we elucidate the unexplored albeit vastly promising crystal chemistry space whilst outlining effective ways to identify regions within this compositional space, particularly where interesting electromagnetic and topological properties could be lurking within the aforementioned alkali and coinage-metal honeycomb layered oxide structures. We conclude by pointing towards possible future research directions, particularly the prospective realisation of Kitaev-Heisenberg-Dzyaloshinskii-Moriya interactions with single crystals and Floquet theory in closely-related honeycomb layered oxide materials. This journal is
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| 7. |
- Massaro, Luca, et al.
(författare)
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Enantioconvergent and enantiodivergent catalytic hydrogenation of isomeric olefins
- 2020
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Ingår i: Chemical Society Reviews. - : Royal Society of Chemistry (RSC). - 0306-0012 .- 1460-4744. ; 49:8, s. 2504-2522
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Forskningsöversikt (refereegranskat)abstract
- The asymmetric catalytic hydrogenation of olefins is one of the most widely studied and utilised transformations in asymmetric synthesis. This straightforward and atom-economical strategy can provide excellent enantioselectivity for a broad variety of substrates and is widely relevant for both industrial applications and academic research. In many instances the hydrogenation is stereospecific in the regard that the E-Z-geometry of the olefin governs the stereochemistry of the hydrogenation, producing an enantiodivergent outcome. Interestingly, the possibility to hydrogenate E- and Z-isomer mixtures to a single stereoisomer in an enantioconvergent manner has been reported. This avoids the need for synthesis of geometrically pure alkene starting materials and therefore constitutes a significant practical advantage. This review article aims to provide an overview of the different stereochemical outcomes in the hydrogenation of olefins. Although the field is well developed and selectivity models have been proposed for a number of catalytic systems, an organized collection of enantioconvergent results, as opposed to the more common enantiodivergent case, might promote new investigation into these phenomena.
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| 8. |
- Mosquera-Lois, Irea, et al.
(författare)
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Imperfections are not 0 K: free energy of point defects in crystals
- 2023
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Ingår i: Chemical Society Reviews. - : ROYAL SOC CHEMISTRY. - 0306-0012 .- 1460-4744. ; 52:17, s. 5812-5826
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Forskningsöversikt (refereegranskat)abstract
- Defects determine many important properties and applications of materials, ranging from doping in semiconductors, to conductivity in mixed ionic-electronic conductors used in batteries, to active sites in catalysts. The theoretical description of defect formation in crystals has evolved substantially over the past century. Advances in supercomputing hardware, and the integration of new computational techniques such as machine learning, provide an opportunity to model longer length and time-scales than previously possible. In this Tutorial Review, we cover the description of free energies for defect formation at finite temperatures, including configurational (structural, electronic, spin) and vibrational terms. We discuss challenges in accounting for metastable defect configurations, progress such as machine learning force fields and thermodynamic integration to directly access entropic contributions, and bottlenecks in going beyond the dilute limit of defect formation. Such developments are necessary to support a new era of accurate defect predictions in computational materials chemistry.
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| 9. |
- Munoz-Garcia, Ana Belen, et al.
(författare)
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Dye-sensitized solar cells strike back
- 2021
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Ingår i: Chemical Society Reviews. - : Royal Society of Chemistry. - 0306-0012 .- 1460-4744. ; 50:22, s. 12450-12550
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Forskningsöversikt (refereegranskat)abstract
- Dye-sensitized solar cells (DSCs) are celebrating their 30th birthday and they are attracting a wealth of research efforts aimed at unleashing their full potential. In recent years, DSCs and dye-sensitized photoelectrochemical cells (DSPECs) have experienced a renaissance as the best technology for several niche applications that take advantage of DSCs' unique combination of properties: at low cost, they are composed of non-toxic materials, are colorful, transparent, and very efficient in low light conditions. This review summarizes the advancements in the field over the last decade, encompassing all aspects of the DSC technology: theoretical studies, characterization techniques, materials, applications as solar cells and as drivers for the synthesis of solar fuels, and commercialization efforts from various companies.
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| 10. |
- Muratov, E. N., et al.
(författare)
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QSAR without borders
- 2020
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Ingår i: Chemical Society Reviews. - : Royal Society of Chemistry (RSC). - 0306-0012 .- 1460-4744. ; 49:11, s. 3525-3564
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Tidskriftsartikel (refereegranskat)abstract
- Prediction of chemical bioactivity and physical properties has been one of the most important applications of statistical and more recently, machine learning and artificial intelligence methods in chemical sciences. This field of research, broadly known as quantitative structure-activity relationships (QSAR) modeling, has developed many important algorithms and has found a broad range of applications in physical organic and medicinal chemistry in the past 55+ years. This Perspective summarizes recent technological advances in QSAR modeling but it also highlights the applicability of algorithms, modeling methods, and validation practices developed in QSAR to a wide range of research areas outside of traditional QSAR boundaries including synthesis planning, nanotechnology, materials science, biomaterials, and clinical informatics. As modern research methods generate rapidly increasing amounts of data, the knowledge of robust data-driven modelling methods professed within the QSAR field can become essential for scientists working both within and outside of chemical research. We hope that this contribution highlighting the generalizable components of QSAR modeling will serve to address this challenge.
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