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Our research deals with the application of computational chemistry methods to a variety of topics, in most cases in close collaboration with experimental groups at ICIQ and at other institutions. These topics fall into three main categories:
  • Structure and reactivity of organometallic compounds and homogeneous catalysis related issues: characterization in-silico of reactive intermediates, elucidation of reaction mechanisms, origin of the chemo-, regio- and enantioselectivity, ligand effects, ligand design and structure-selectivity relationships.
  • Polyoxometalates: electronic structure, mechanism of catalytic oxidation reactions, dynamic structure of cations and solvent water molecules around and inside POMs.
  • Supramolecular chemistry: structure of host-guest systems, assessment of non-bonding interactions and supramolecular catalysis.

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Alkali-Driven Disassembly and Reassembly of Molecular Niobium Oxide in Water DOI: 10.19061/iochem-bd-1-88

Alkali counterions for polyoxometalate (POM) clusters control solubility with distinct periodic trends, but evidence for alkali control over speciation is ambiguous. Here we show that a simple Nb-POM, [Nb10O28]6– ({Nb10}), converts to oligomers of (HxNb24O72)(24–x)– ({Nb24}) upon adding only alkali chloride salts, even in buffered neutral solutions.

This dataset derived results are published in:

Manuscript title: Alkali-Driven Disassembly and Reassembly of Molecular Niobium Oxide in Water

Journal: J. Am. Chem. Soc.

DOI: 10.1021/jacs.8b05015

Al(x)Cr(y)_Keggin_oxos DOI: 10.19061/iochem-bd-1-23

This dataset derived results are published in:

Manuscript title: Crystallizing Elusive Chromium Polycations.

Journal: Chem

DOI: 10.1016/j.chempr.2016.11.006

A Metal-Free Synthesis of N-Aryl Carbamates under Ambient Conditions DOI: 10.19061/iochem-bd-1-3

This dataset derived results are published in:

Manuscript title: A Metal-Free Synthesis of N-Aryl Carbamates under Ambient Conditions

Journal: Angew. Chem. Int. Ed.

DOI: 10.1002/anie.201504956

Analysis of the interaction between Keplerate nanocapsules and their anionic ligands DOI: 10.19061/iochem-bd-1-33

This dataset derived results are published in:

Manuscript title: Anions coordinating anions: Analysis of the interaction between anionic Keplerate nanocapsules and their anionic ligands

Journal: PCCP

DOI: 10.1039/C6CP08511C

AnS2(2+)_cations DOI: 10.19061/iochem-bd-1-30

Actinide disulphide dications, AnS22+, were produced in the gas phase for An = Th and Np by reaction of An2+ cations with the sulfur-atom donor COS, in a sequential abstraction process of two sulfur atoms, as examined by FTICR mass spectrometry. For An = Pu and Am, An2+ ions were unreactive with COS and did not yield any sulphide species. High level multiconfigurational (CASPT2) calculations were performed to assess the structures and bonding of the new AnS22+ species obtained for An = Th, Np, as well as for An = Pu to examine trends along the An series, and for An = U to compare with a previous experimental study and DFT computational scrutiny of US22+. The CASPT2 results showed that, like in the case of uranium, the new AnS22+ ions have ground states with triangular geometries, corresponding to the presence of a persulphide in the case of thorium that formally leads to a stable ThIVS22+ species, while a supersulphide appears to be present in the case of U, Np and Pu, formally leading to a AnIIIS22+ species. The computations also revealed that linear thioactinyl structures are higher in energy, with a difference that increases fourfold upon moving from U to Pu, apparently indicating that it will be even more pronounced for Am.

This dataset derived results are published in:

Manuscript title: Synthesis, structure and bonding of actinide disulphide dications in the gas phase

Journal: PCCP

DOI: 10.1039/c7cp01446e

Aromatic_Amination_of_Lactones DOI: 10.19061/iochem-bd-1-21

This dataset derived results are published in:

Manuscript title: Metal-Free Synthesis of N-Aryl Amides using Organocatalytic Ring-Opening Aminolysis of Lactones

Journal: ChemSusChem

DOI: 10.1002/cssc.201700415

Cs+ contac ion-pairing between hexaniobates and hexatantalates DOI: 10.19061/iochem-bd-1-31

Computational studies ascertained more persistent Cs+–[Ta6O19] ion pairs than Cs+–[Nb6O19] ion pairs, and bond energy decomposition analyses determined relativistic effects to be the differentiating factor between the two. These distinctions are likely responsible for many of the unexplained differences between aqueous Nb and Ta chemistry, while they are so similar in the solid state.

This dataset derived results are published in:

Manuscript title: Cs+ contac ion-pairing between hexaniobates and hexatantalates

Journal: PCCP

DOI: 10.1039/C6CP08454K

Electronic Structure Studies on the Whole Keplerate Family DOI: 10.19061/iochem-bd-1-24

A comprehensive study on the electronic structure of nano-scale molecular oxide capsules of the type [{MVI(MVI)5O21}12{M'V2O2(μ-X)(μ-Y)(Ln- )}30](12+n)-, where M,M'=Mo,W, and the bridging ligands X,Y=O,S, carried out by means of density functional theory based methods.

This dataset derived results are published in:

Manuscript title: Electronic Structure Studies on the Whole Keplerate Family: Predicting New Members

Journal: Chem. Eur. J.

DOI: 10.1002/chem.201605981

Fe(III) Keggin structures DOI: 10.19061/iochem-bd-1-18

This dataset derived results are published in:

Manuscript title: Magneto-Structural Analysis of Iron(III) Keggin Polyoxometalates

Journal: J. Phys. Chem. A

DOI: 10.1021/acs.jpca.6b10763

Glycidol DOI: 10.19061/iochem-bd-1-58

No other publication derived

Hierarchical self-assembly of polyoxometalate-based hybrids driven by metal coordination and electrostatic interactions: from discrete supramolecular species to dense monodisperse nanoparticles. DOI: 10.19061/iochem-bd-1-5

This dataset derived results are published in:

Manuscript title: Hierarchical Self-Assembly of Polyoxometalate-Based Hybrids Driven by Metal Coordination and Electrostatic Interactions: From Discrete Supramolecular Species to Dense Monodisperse Nanoparticles

Journal: J. Am. Chem. Soc.

DOI: 10.1021/jacs.6b00972

Hydrogen_Evolution_Catalysis DOI: 10.19061/iochem-bd-1-99

No other publication derived

Kioto Project DOI: 10.19061/iochem-bd-1-56

No other publication derived

Master Thesis

No other publication derived

Mechanistic Insights into the Carbon Dioxide-Cyclohexene Oxide Copolymerization reaction DOI: 10.19061/iochem-bd-1-17

A detailed study on the mechanism for the alternating copolymerization of cyclohexene oxide (CHO) and CO2 mediated by a [Al{amino‐tri(phenolate)}]/NBu4I binary catalyst system has been carried out using density functional theory (DFT) based methods.

This dataset derived results are published in:

Manuscript title: Mechanistic Insights into the Carbon Dioxide-Cyclohexene Oxide Copolymerization reaction: Is one Metal Center enough?

Journal: ChemSusChem

DOI: 10.1002/cssc.20160152

Mechanistic Study on Limonene Oxide and Carbon Dioxide Copolymerisation

This dataset derived results are published in:

Manuscript title: AlIII-Catalysed Formation of Poly(limonene)carbonate: DFT Analysis of the Origin of Stereoregularity

Journal: Chem. Eur. J.

DOI: 10.1002/chem.201406334

Mo(I)_hydrogen_generation

No other publication derived

Molecular basis for the recognition of higher fullerenes into ureidopyrimidinonecyclotriveratrylene self-assembled capsules DOI: 10.19061/iochem-bd-1-7

This dataset derived results are published in:

Manuscript title: Molecular Basis for the Recognition of Higher Fullerenes into Ureidopyrimidinone–Cyclotriveratrylene Self-Assembled Capsules

Journal: Chem. Eur. J.

DOI: 10.1002/chem.201601690

Molecular Motion and Conformational Interconversion of IrI·COD Included in Rebek’s Self-Folding Octaamide Cavitand DOI: 10.19061/iochem-bd-1-2

This dataset derived results are published in:

Manuscript title: Molecular Motion and Conformational Interconversion of IrI·COD Included in Rebek’s Self-Folding Octaamide Cavitand

Journal: J. Am. Chem. Soc.

DOI: 10.1021/jacs.5b12646

Oxidative Carbon-Carbon Bond Cleavage by Vanadium Catalyst DOI: 10.19061/iochem-bd-1-53

The aerobic oxidative CC bond cleavage of vicinal diols catalyzed by vanadium aminotriphenolates is described. Our results show that CC bond cleavag e can be performed in different solvents,under an air or oxygen atmosphere, with a large variety of glycols (cyclic or linear, with aromati c or aliphaticsubstituents) affording the corresponding carbonyl derivatives with high chemoselectivity.Reactions can be performed with as little as 10 ppm of catalyst reaching TON up to 81,000 and TOFs of up to4150 h1. A reaction mechanism, rationalized by de nsity functional theory calculations, is also proposed.

This dataset derived results are published in:

Manuscript title: Efficient Vanadium-Catalyzed Aerobic CC Bond OxidativeCleavage of Vicinal Diols

Journal: Adv. Synth. Catal.

DOI: https://doi.org/10.1002/adsc.201800050

Photochromism and Dual-Color Fluorescence in a Polyoxometalate–Benzospiropyran Molecular Switch DOI: 10.19061/iochem-bd-1-27

This dataset derived results are published in:

Manuscript title: Photochromism and Dual-Color Fluorescence in a Polyoxometalate–Benzospiropyran Molecular Switch

Journal: Angew. Chem. Int. Ed.

POMS DOI: 10.19061/iochem-bd-1-60

No other publication derived

PrLn DOI: 10.19061/iochem-bd-1-64

No other publication derived

Raman spectra of species observed during the formation of [Mo 132] Keplerates DOI: 10.19061/iochem-bd-1-32

Infrared and Raman Spectra of MoxOy species

This dataset derived results are published in:

Manuscript title: Direct Observation of the Formation Pathway of [Mo 132] Keplerates

Journal: Inorg. Chem.

DOI: 10.1021/acs.inorgchem.5b02570

Regioselective Catalysis by the {Mo132} nanocapsule DOI: 10.19061/iochem-bd-1-54

This dataset derived results are published in:

Manuscript title: Regioselective Catalysis by the {Mo132} nanocapsule: A computational inspection.

Journal: Eur. J. Inorg. Chem.

DOI: 10.1002/ejic.201800155

Thermodynamic Stability of Heterodimetallic [LnLn’] Complexes DOI: 10.19061/iochem-bd-1-22

The solid state and solution configuration of the heterodimetallic complexes, (Hpy)[CeEr(HL)3(NO3)(py)(H2O)] (1), (Hpy)[PrSm(HL)3(NO3)(py)(H2O)] (2) and (Hpy)2[LaYb(HL)3(NO3)(H2O)](NO3) (3), where H3L is 6-(3-oxo-3-(2-hydroxyphenyl)propionyl)pyridine-2-carboxylic acid, are analysed experimentally and through DFT calculations. The theoretical study is also extended to the [LaCe], [LaLu] and [CeGd] analogues. The results are consistent with a remarkable selectivity of the metal distribution within the molecule while in the solid state, enhanced by the size difference of both metals. This selectivity is significantly reduced in solution.

This dataset derived results are published in:

Manuscript title: Thermodynamic Stability of Heterodimetallic [LnLn’] Complexes: Synthesis and DFT Studies

DOI: 10.1002/chem.201700095

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