Inorganic oxide materials are used in semiconductor electronics, ion exchange, catalysis, coatings, gas sensors and as separation materials. Although their synthesis is well understood, the scope for new materials is reduced because of the stability limits imposed by high-temperature processing and top-down synthetic approaches. In this Review, we describe the derivatization of polyoxometalate (POM) clusters, which enables their assembly into a range of frameworks by use of organic or inorganic linkers. Additionally, bottom-up synthetic approaches can be used to make metal oxide framework materials, and the features of the molecular POM precursors are retained in these structures. Highly robust all-inorganic frameworks can be made using metal-ion linkers, which combine molecular synthetic control without the need for organic components. The resulting frameworks have high stability, and high catalytic, photochemical and electrochemical activity. Conceptually, these inorganic oxide materials bridge the gap between zeolites and metal–organic frameworks (MOFs) and establish a new class of all-inorganic POM frameworks that can be designed using topological and reactivity principles similar to MOFs. Inorganic oxide materials are used in semiconductor electronics, ion exchange, catalysis, coatings, gas sensors and as separation materials. In this Review, we explain how polyoxometalate clusters are amenable to molecular control and can be assembled into inorganic frameworks owing to the molecular nature of their building blocks.

Design and synthesis of polyoxometalate-framework materials from cluster precursors

Metal–organic frameworks (MOFs) are a widely investigated class of crystalline
solids with tunable structures that make it possible to impart specific
chemical functionality tailored for a given application However, the enormous
number of possible MOFs that can be synthesized makes it difficult to determine
which materials would be the most promising candidates, especially for
applications governed by electronic structure properties that are often
computationally demanding to simulate and time-consuming to probe
experimentally Here, we have developed the first publicly available quantum-chemical
database for MOFs (the “QMOF database”), which consists of properties derived
from density functional theory (DFT) for over 14,000 experimentally synthesized
MOFs Throughout this study, we demonstrate how this new database can be used
to identify MOFs with targeted electronic structure properties As a
proof-of-concept, we use the QMOF database to evaluate the performance of
several machine learning models for the prediction of DFT-computed band gaps
and find that crystal graph convolutional neural networks are capable of
achieving superior predictive performance, making it possible to circumvent
computationally expensive quantum-chemical calculations We also show how
unsupervised learning methods can aid the discovery of otherwise subtle structure–property
relationships using the computational findings in this work We conclude by
highlighting several MOFs with low band gaps, a challenging task given the
electronically insulating nature of most MOF structures The data and
predictive models generated in this work, as well as the database of MOF
structures, should be highly useful to other researchers interested in the
predictive design and discovery of MOFs for the many applications dictated by
quantum-chemical phenomena

Machine Learning the Quantum-Chemical Properties of Metal–Organic Frameworks for Accelerated Materials Discovery with a New Electronic Structure Database

Progress in selenium based metal-organic precursors for main group and transition metal selenide thin films and nanomaterials

A series of organic–inorganic hybrid complexes based on different types of polyoxomolybdates and transition metal complexes, namely, [Zn2(TPMA)2(H2P2Mo5O23)]·11H2O (1), [Zn2(TPMA)2(Mo8O26)] (2), [Co2(TPMA)2(Mo8O26)] (3), [Ni2(TPMA)2(Mo8O26)(H2O)2] (4), [Ni2(TPMA)2(2-PA)(H2O)](PMo12O40) (5) [Cu2(TPMA)2(Mo8O26)] (6), 2[Cu(TPMA)(CrMo6(OH)6O18)]·H[Cu2(TPMA)2(CrMo6(OH)6O18)]·4H2O (7) (TPMA = Tris[(2-pyridyl)methyl]amine, 2-PA = 2-picolinic acid), have been successfully synthesized under hydrothermal conditions. All complexes were characterized by single-crystal X-ray structural analysis, powder X-ray diffraction, IR spectroscopy and TG analysis. All the complexes showed polyoxomolybdate-based zero-dimensional (0D) structures, and could be further extended into three-dimensional (3D) supramolecular frameworks through hydrogen bonding interactions. In addition, the electrochemical properties of complexes 1–7 have been investigated. Interestingly, some complexes have efficient photocatalytic activities to degradate pararosaniline hydrochloride dye molecules.

A series of organic–inorganic hybrid materials consisting of flexible organic amine modified polyoxomolybdates: synthesis, structures and properties

Base promoted synthesis of novel indole-dithiocarbamate compounds as potential anti-inflammatory therapeutic agents for treatment of acute lung injury.

A series of five heteronuclear zinc tin chalcogenide complexes with the general formula [(tmeda)Zn(SnR2)2E3] (1-R, E = S; R = Me, Ph, tBu; 2-R, E = Se; R = Ph, tBu) have been synthesized and characterized by X-ray crystal structure analysis. In all cases, the six-membered ZnSn2E3 rings exhibit twist boat conformation. The presence of the molecular structures in solution is confirmed by 119Sn and 77Se NMR spectroscopy. Cothermolysis experiments using a mixture of complexes 1-R or 2-R and [(iPr3PCu)2(EC2H4E)]2 as a copper source were monitored by thermogravimetry and temperature dependent X-ray powder diffraction to examine the thermolysis reaction. According to Rietveld refinement, the solid residue consists of Cu2ZnSnS4 (up to 78 wt %) or Cu2ZnSnSe4 (up to 43 wt %) as the main product, respectively.

Zinc Tin Chalcogenide Complexes and Their Evaluation as Molecular Precursors for Cu2ZnSnS4 (CZTS) and Cu2ZnSnSe4 (CZTSe)

Reactions of the tris(2-pyridyl)lead(II) compound [LiPb(2-py6OtBu)3] (1) with trialkyl compounds of the group 13 elements gallium and indium resulted in the bis(2-pyridyl) and tris(2-pyridyl) gallate complexes [LiGaEt2(2-py6OtBu)2]2 (2), [LiGaR2(2-py6OtBu)2(THF)] (R = iPr (3), tBu (4)), [LiGatBu2(2-py6OtBu)2]2 (4′), and [LiGaMe(2-py6OtBu)3] (6), as well as corresponding indium complexes of general composition [LiInR(2-py6OtBu)3] (R = Me (7), Et (8)). The formation of these compounds can be assumed as a rapid degradation of initially formed Pb–M adducts (M = Ga or In) as found for [tBu3Ga{Pb(2-py6OtBu)3Li}] (5). In addition, the redox transmetalation route was used for the synthesis of [LiInI(2-py6OtBu)3(THF)] (9). The structures of all compounds have been verified by single-crystal X-ray diffraction analysis, NMR spectroscopy, and mass spectrometry.

Bis(2-pyridyl) and Tris(2-pyridyl) Compounds of Gallium and Indium via a Redox-Transmetalation Route.

With the 5C46 AZUR SPACE is introducing its new CPV cell into the market. This upright metamorphic AlInGaP/InGaP/AlInGaAs/InGaAs/Ge 5-junction cell uses sub-cell materials comparable to AZUR’s 4G32 space solar cell but has an additional InGaP junction. The cell design is laid out for optimum module performance at operating conditions. As reported earlier, the bandgaps of the sub-cells have been selected to avoid the dips in the AM1.5d spectrum for cell temperatures up to 90°C. The optimization of the 5C46 has been monitored by the manufacture of 5C46-based commercial CPV modules equipped with secondary lenses and rating of these modules at Fraunhofer ISE. A very good efficiency of 31.7% at Concentrator Standard Operating Conditions (CSOC, lens array aperture) has been reached corresponding to a power boost of 17.5% compared to reference modules equipped with 3C44 cells. In the last optimization step, the thicknesses of the sub-cells have been adjusted to achieve current matching under operating conditions on module level. The paper describes the method used for modelling and the calculation of the optimum thicknesses. It involves the determination of the absolute quantum efficiency of the bare cell and accounts for the thermal band-gap shifts as well as the optical effects due to mounting of the secondary and the transmission of the primary lens. First outdoor results of modules equipped with the final 5C46 design confirm that the current-matching for operating condition on module level was successfully achieved by the described method. 

AZUR’s new 5C46 CPV cell: Final design for optimized outdoor performance

Metal-organic frameworks with hydroxamate linkers are an emerging new class of stable porous crystalline materials. Due to the difficulty in controlling reversible formation of strong metal-hydroxamate bonds and the limitation of available hydroxamate ligands, hydroxamate MOFs are rarely reported and their applications are underexplored. Herein, we report on a lanthanum MOF, La-ONDI, containing the redox-active hydroxamate ligand ONDI2-. Due to the presence of strong coordinative bonds of chelating hydroxamate groups to metal nodes, La-ONDI not only displays high framework stability in aqueous solutions ranging from pH 3 to pH 13, but also exhibits good structural integrity in common organic solvents and harsh reagents. In addition, La-ONDI shows paramagnetic behaviour due to the presence of unpaired electrons. The amount of unpaired electrons can be modified by the reducing environment during synthesis. Although without π-π interactions between neighbouring ligands, La-ONDI still exhibits good electrically conductive performance with the conductivity reaching 10-6 S cm-1.

A stable lanthanum hydroxamate metal-organic framework with radical character and electrical conductivity.

The structures of [(iPr3P)2Cu(μ-SSiMe3)(InMe3)] and [(iPr3P)2Cu(μ-SeSiMe3)(InMe3)] were determined by single-crystal X-ray diffraction. Both complexes are Lewis acid–base adducts of the InMe3 acceptor and the chalcogen donor atom linking a Me3Si group and a (iPr3P)2Cu moiety. They are very unstable under atmospheric conditions and decompose at ambient temperatures. Results of DFT calculations for these complexes and the related hypothetical [(Me3P)2Cu(μ-SSiMe3)(InMe3)] compound show that the unusual planar coordination of the chalcogen atoms is due to steric crowding.

Synthesis and Crystal Structures of [(iPr3P)2Cu(μ-ESiMe3)(InMe3)] (E = S, Se): Lewis Acid–Base Adducts with Chalcogen Atoms in Planar Coordination

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