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Inorganics, Volume 9, Issue 4 (April 2021) – 8 articles

Cover Story (view full-size image): The development of catalysts for the selective hydrolysis of proteins is challenging, yet important, for many applications in biotechnology and proteomics. The hydrolysis of hydrophobic proteins is particularly challenging as, due to their poor solubility, the use of surfactants is often required. In this study, the potential of catalyst systems based on the Zr(IV)-substituted Keggin polyoxometalate (Et2NH2)10[Zr(PW11O39)2] (Zr-K 1:2) and three different surfactants, which differ in structure and polarity, has been investigated toward hydrolysis of ovalbumin as a model protein. The study revealed that the presence of surfactants did not alter the selectivity of protein hydrolysis, but the efficiency of the reaction was affected differently depending on the type of surfactant. View this paper.
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Open AccessArticle
Metal-Rich Metallaboranes: Synthesis, Structures and Bonding of Bi- and Trimetallic Open-Faced Cobaltaboranes
Inorganics 2021, 9(4), 28; https://0-doi-org.brum.beds.ac.uk/10.3390/inorganics9040028 - 13 Apr 2021
Viewed by 358
Abstract
Synthesis, isolation, and structural characterization of unique metal rich diamagnetic cobaltaborane clusters are reported. They were obtained from reactions of monoborane as well as modified borohydride reagents with cobalt sources. For example, the reaction of [Cp*CoCl]2 with [LiBH4·THF] and subsequent [...] Read more.
Synthesis, isolation, and structural characterization of unique metal rich diamagnetic cobaltaborane clusters are reported. They were obtained from reactions of monoborane as well as modified borohydride reagents with cobalt sources. For example, the reaction of [Cp*CoCl]2 with [LiBH4·THF] and subsequent photolysis with excess [BH3·THF] (THF = tetrahydrofuran) at room temperature afforded the 11-vertex tricobaltaborane nido-[(Cp*Co)3B8H10] (1, Cp* = η5-C5Me5). The reaction of Li[BH2S3] with the dicobaltaoctaborane(12) [(Cp*Co)2B6H10] yielded the 10-vertex nido-2,4-[(Cp*Co)2B8H12] cluster (2), extending the library of dicobaltadecaborane(14) analogues. Although cluster 1 adopts a classical 11-vertex-nido-geometry with one cobalt center and four boron atoms forming the open pentagonal face, it disobeys the Polyhedral Skeletal Electron Pair Theory (PSEPT). Compound 2 adopts a perfectly symmetrical 10-vertex-nido framework with a plane of symmetry bisecting the basal boron plane resulting in two {CoB3} units bridged at the base by two boron atoms and possesses the expected electron count. Both compounds were characterized in solution by multinuclear NMR and IR spectroscopies and by mass spectrometry. Single-crystal X-ray diffraction analyses confirmed the structures of the compounds. Additionally, density functional theory (DFT) calculations were performed in order to study and interpret the nature of bonding and electronic structures of these complexes. Full article
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Open AccessReview
Metal–Organic Frameworks as Versatile Platforms for Organometallic Chemistry
Inorganics 2021, 9(4), 27; https://0-doi-org.brum.beds.ac.uk/10.3390/inorganics9040027 - 09 Apr 2021
Cited by 1 | Viewed by 513
Abstract
Metal–organic frameworks (MOFs) are emerging porous materials with highly tunable structures developed in the 1990s, while organometallic chemistry is of fundamental importance for catalytic transformation in the academic and industrial world for many decades. Through the years, organometallic chemistry has been incorporated into [...] Read more.
Metal–organic frameworks (MOFs) are emerging porous materials with highly tunable structures developed in the 1990s, while organometallic chemistry is of fundamental importance for catalytic transformation in the academic and industrial world for many decades. Through the years, organometallic chemistry has been incorporated into functional MOF construction for diverse applications. Here, we will focus on how organometallic chemistry is applied in MOF design and modifications from linker-centric and metal-cluster-centric perspectives, respectively. Through structural design, MOFs can function as a tailorable platform for traditional organometallic transformations, including reaction of alkenes, cross-coupling reactions, and C–H activations. Besides, an overview will be made on other application categories of organometallic MOFs, such as gas adsorption, magnetism, quantum computing, and therapeutics. Full article
(This article belongs to the Special Issue Functional Coordination Polymers and Metal–Organic Frameworks)
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Open AccessReview
Anticancer Half-Sandwich Rhodium(III) Complexes
Inorganics 2021, 9(4), 26; https://0-doi-org.brum.beds.ac.uk/10.3390/inorganics9040026 - 08 Apr 2021
Viewed by 431
Abstract
Platinum-based anticancer drugs are most likely the most successful group of bioinorganic compounds. Their apparent disadvantages have led to the development of anticancer compounds of other noble metals, resulting in several ruthenium-based drugs which have entered clinical trials on oncological patients. Besides ruthenium, [...] Read more.
Platinum-based anticancer drugs are most likely the most successful group of bioinorganic compounds. Their apparent disadvantages have led to the development of anticancer compounds of other noble metals, resulting in several ruthenium-based drugs which have entered clinical trials on oncological patients. Besides ruthenium, numerous rhodium complexes have been recently reported as highly potent antiproliferative agents against various human cancer cells, making them potential alternatives to Pt- and Ru-based metallodrugs. In this review, half-sandwich Rh(III) complexes are overviewed. Many representatives show higher in vitro potency than and different mechanisms of action (MoA) from the conventional anticancer metallodrugs (cisplatin in most cases) or clinically studied Ru drug candidates. Furthermore, some of the reviewed Rh(III) arenyl complexes are also anticancer in vivo. Pioneer anticancer organorhodium compounds as well as the recent advances in the field are discussed properly, and adequate attention is paid to their anticancer activity, solution behaviour and various processes connected with their MoA. In summary, this work summarizes the types of compounds and the most important biological results obtained in the field of anticancer half-sandwich Rh complexes. Full article
(This article belongs to the Special Issue Metal Arene Complexes)
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Open AccessArticle
Hydrothermal Synthesis and Structural Investigation of a Crystalline Uranyl Borosilicate
Inorganics 2021, 9(4), 25; https://0-doi-org.brum.beds.ac.uk/10.3390/inorganics9040025 - 06 Apr 2021
Viewed by 342
Abstract
The relevance of multidimensional and porous crystalline materials to nuclear waste remediation and storage applications has motivated exploratory research focused on materials discovery of compounds, such as actinide mixed-oxoanion phases, which exhibit rich structural chemistry. The novel phase K1.8Na1.2[(UO [...] Read more.
The relevance of multidimensional and porous crystalline materials to nuclear waste remediation and storage applications has motivated exploratory research focused on materials discovery of compounds, such as actinide mixed-oxoanion phases, which exhibit rich structural chemistry. The novel phase K1.8Na1.2[(UO2)BSi4O12] has been synthesized using hydrothermal methods, representing the first example of a uranyl borosilicate. The three-dimensional structure crystallizes in the orthorhombic space group Cmce with lattice parameters a = 15.5471(19) Å, b = 14.3403(17) Å, c = 11.7315(15) Å, and V = 2615.5(6) Å3, and is composed of UO6 octahedra linked by [BSi4O12]5− chains to form a [(UO2)BSi4O12]3− framework. The synthesis method, structure, results of Raman, IR, and X-ray absorption spectroscopy, and thermal stability are discussed. Full article
(This article belongs to the Special Issue Cornerstones in Contemporary Inorganic Chemistry)
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Open AccessArticle
Synthesis of a Ru(II) Complex with a Naphthoquinone-Annelated Imidazole Ligand Exhibiting Proton-Responsive Redox and Luminescent Behavior
Inorganics 2021, 9(4), 24; https://0-doi-org.brum.beds.ac.uk/10.3390/inorganics9040024 - 03 Apr 2021
Viewed by 384
Abstract
A mononuclear ruthenium complex, [RuII(L)(bpy)2](PF6), with a naphthoquinone-annelated imidazole ligand HL (2-(pyridin-2-yl)-1H-naphtho[2,3-d]imidazole-4,9-dione) was synthesized and structurally characterized. Electrochemical study reveals that the Ru complex shows four reversible redox waves at +0.98 V, −1.13 [...] Read more.
A mononuclear ruthenium complex, [RuII(L)(bpy)2](PF6), with a naphthoquinone-annelated imidazole ligand HL (2-(pyridin-2-yl)-1H-naphtho[2,3-d]imidazole-4,9-dione) was synthesized and structurally characterized. Electrochemical study reveals that the Ru complex shows four reversible redox waves at +0.98 V, −1.13 V, −1.53 V, and −1.71 V versus SCE in acetonitrile, which are assigned to Ru(II)/Ru(III), L/L•2−, and two bpy/bpy•− redox couples, respectively. The redox potential of Ru(II)/Ru(III) was positively shifted upon the addition of trifluoromethanesulfonic acid due to protonation of the L moiety, leading to stabilization of the Ru 4d orbital. In UV-vis absorption measurements for the Ru complex in acetonitrile, a metal-to-ligand charge transfer (MLCT) band was observed at 476 nm, which was shifted to 450 nm by protonation, which might be due to a decrease in the electron delocalization and stabilization of the π orbitals in L. The blue shift of the MLCT band by protonation was associated with a shift of an emission band from 774 nm to 620 nm, which could be caused by the decreased electronic delocalization in the MLCT excited state. These electrochemical and spectroscopic changes were reversible for the protonation/deprotonation stimuli. Full article
(This article belongs to the Special Issue Redox-Active Ligand Complexes)
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Open AccessArticle
Optimization of the Synthesis and Energy Transfer of Ca2MgWO6:Cr3+,Nd3+
Inorganics 2021, 9(4), 23; https://0-doi-org.brum.beds.ac.uk/10.3390/inorganics9040023 - 31 Mar 2021
Viewed by 336
Abstract
This work pertains to Cr3+ and Nd3+ co-activated Ca2MgWO6 phosphors synthesized by high temperature solid-state method using oxides and carbonates as raw materials. All luminescent samples according to Ca2MgWO6:Cr3+,Nd3+ include Cr [...] Read more.
This work pertains to Cr3+ and Nd3+ co-activated Ca2MgWO6 phosphors synthesized by high temperature solid-state method using oxides and carbonates as raw materials. All luminescent samples according to Ca2MgWO6:Cr3+,Nd3+ include Cr3+ for the absorption of UV and visible radiation (230–800 nm) prior to energy transfer to Nd3+. As a result of the energy transfer between Cr3+ and Nd3+, we observe line emission originating from Nd3+ in the near infrared range additionally to the broad band near infrared emission from Cr3+ assigned to the spin-allowed 4T24A2 transition. The energy transfer from Cr3+ to Nd3+ is discussed via the variations of the lifetime data of Cr3+ and Nd3+. The strong absorption of Cr3+ in the ultraviolet range and the efficient energy transfer from Cr3+ to Nd3+ indicate that the herein presented material type can serve as a radiation converter for near infrared region light emitting diodes (NIR-LEDs) comprising an UV-A emitting (Al,Ga)N chip. Full article
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Open AccessArticle
Broadening the Scope of Polyoxometalates as Artificial Proteases in Surfactant Solutions: Hydrolysis of Ovalbumin by Zr(IV)-Substituted Keggin Complex
Inorganics 2021, 9(4), 22; https://0-doi-org.brum.beds.ac.uk/10.3390/inorganics9040022 - 26 Mar 2021
Viewed by 401
Abstract
Development of catalysts for the selective hydrolysis of proteins is challenging, yet important for many applications in biotechnology and proteomics. The hydrolysis of hydrophobic proteins is particularly challenging, as due to their poor solubility, the use of surfactants is often required. In this [...] Read more.
Development of catalysts for the selective hydrolysis of proteins is challenging, yet important for many applications in biotechnology and proteomics. The hydrolysis of hydrophobic proteins is particularly challenging, as due to their poor solubility, the use of surfactants is often required. In this study, the proteolytic potential of catalyst systems based on the Zr(IV)-substituted Keggin polyoxometalate (Et2NH2)10[Zr(PW11O39)2] (Zr-K 1:2) and three different surfactants (ionic SDS (sodium dodecyl sulfate); zwitterionic Zw3-12 (n-dodecyl-N,N-dimethyl-3-ammonio-1-propanesulfonate); and CHAPS (3-[(3-cholamidopropyl)dimethylammonio]-1-propanesulfonate)), which differ in structure and polarity, has been investigated. Hydrolysis of ovalbumin (OVA) was examined in the presence of Zr-K 1:2 and surfactants by sodium dodecyl sulfate poly(acrylamide) gel electrophoresis (SDS-PAGE), which showed the appearance of new polypeptide fragments at lower molecular weight, indicating that selective hydrolysis of OVA took place for all three catalyst systems. The same fragmentation pattern was observed, showing that the selectivity was not affected by surfactants. However, the surfactants influenced the performance of the catalyst. Hence, the interactions of OVA with surfactants and Zr-K 1:2 were investigated using different techniques such as tryptophan fluorescence, Circular Dichroism, and Dynamic Light Scattering. The speciation of the catalyst in surfactant solutions was also followed by 31P Nuclear Magnetic Resonance spectroscopy providing insight into its stability under reaction conditions. Full article
(This article belongs to the Section Bioinorganic Chemistry)
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Open AccessArticle
Photocatalytic Activity of Multicompound TiO2/SiO2 Nanoparticles
Inorganics 2021, 9(4), 21; https://0-doi-org.brum.beds.ac.uk/10.3390/inorganics9040021 - 25 Mar 2021
Viewed by 401
Abstract
Multicompound TiO2/SiO2 nanoparticles with a diameter of 50–70 nm were generated using a liquid flame spray (LFS) nanoparticle deposition in a single flame. Here, we study the photocatalytic activity of deposited multicompound nanoparticles in gas-phase via oxidation of acetylene into [...] Read more.
Multicompound TiO2/SiO2 nanoparticles with a diameter of 50–70 nm were generated using a liquid flame spray (LFS) nanoparticle deposition in a single flame. Here, we study the photocatalytic activity of deposited multicompound nanoparticles in gas-phase via oxidation of acetylene into carbon dioxide that gives new insight about the multicompound nanoparticle morphology. A small addition of SiO2 content of 0.5%, 1.0% and 3.0% significantly suppressed the photocatalytic activity by 33%, 44% and 70%, respectively, whereas 5.0% SiO2 addition completely removed the activity. This may be due to a formation of a thin passivating SiO2 layer on top of the of the TiO2 nanostructures during the LFS nanoparticle deposition. Surface wetting results support this hypothesis with a significant increase in water contact angle as the SiO2 content is increased. Full article
(This article belongs to the Section Inorganic Solid-State Chemistry)
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