Roger Bofill

Roger Bofill
Autonomous University of Barcelona | UAB · Department of Chemistry

About

55
Publications
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1,293
Citations

Publications

Publications (55)
Article
The development of organic-inorganic hybrid materials for redox catalysis is key to access new energy conversion schemes and the sustainable production of dihydrogen. Here on, bare and P-doped graphene arising...
Article
Full-text available
Covalent organic frameworks (COFs) are crystalline porous organic polymers built from covalent organic blocks that can be photochemically active when incorporating organic semicon-ducting units, such as triazine rings or diacetylene bridges. The bandgap, charge separation capacity , porosity, wettability, and chemical stability of COFs can be tuned...
Article
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A family of Cu-based complexes bearing dianionic bpy-amidate ligands have been prepared and characterized by spectroscopic and electrochemical techniques. The new complexes are capable of performing water oxidation catalysis at overpotentials between 557–830 mV pH 11.6. A detailed electrocatalytic study in combination with computational calculation...
Article
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Water oxidation to dioxygen is one of the key reactions that need to be mastered for the design of practical devices based on water splitting with sunlight. In this context, water oxidation catalysts based on first-row transition metal complexes are highly desirable due to their low cost and their synthetic versatility and tunability through ration...
Chapter
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Hydrogen production by a sustainable approach like proton reduction triggered by renewable energy sources is a high challenge. Ruthenium-based nanomaterials have recently gained a renewed interest as catalysts for this reaction, showing very promising performances. This Chapter summarizes the key factors ruling the catalytic activity of Ru metal/me...
Cover Page
Catal. Sci. Technol cover page featuring the article: The role of catalyst–support interactions in oxygen evolution anodes based on Co(OH)2 nanoparticles and carbon microfibers
Article
The performance of OER anodes based on supported nanocatalysts is highly dependent on the interactions taking place at the interface between the nanocatalyst and the employed conductive support. Herein, the versatility offered by the organometallic approach for the synthesis of metal-based nanostructures allowed preparing electrodes of tailored nan...
Article
Four different cathodes for the hydrogen evolution reaction (HER) have been developed by the decoration of commercial carbon microfibers with Ru nanoparticles (Ru NPs). Two types of carbon fibers have been used: pristine, as‐received, carbon fibers (pCF) and carbon fibers modified by an oxidative treatment that led to the functionalization of their...
Article
Both global warming and the limited fossil resources make the transition from fossil to solar fuels an urgent matter. In this regard, the splitting of water activated by sunlight is a sustainable and carbon-free new energy conversion scheme able to produce efficient technological devices. Having at disposal appropriate catalysts is essential for th...
Article
Metallothioneins are small Cys-rich peptides capable of coordinating metal ions, and proposed to be involved in radical stress. The four Zn(II)-GmMTs complexes of soybean (Glycine max) were recombinantly synthesised and exposed to oxidative (HO•) and reductive (H• atoms and eaq–) stress conditions. Gamma-irradiation was used to simulate the endogen...
Article
Cobalt nanoparticles (NPs) have been prepared by hydrogenation of the organometallic complex [Co(η3-C8H13)(η4-C8H12)] in 1-heptanol in the absence of any other stabilizer and then transformed into Co3O4 NPs using mild oxidative reaction conditions. After deposition onto glassy carbon rotating disk electrodes, the electrocatalytic performance of the...
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In this work we lay out design guidelines for catalytically more efficient organic photocathodes achieving stable hydrogen production in neutral pH. We propose an organic photocathode architecture employing a NiO hole selective layer, a PCDTBT:PCBM bulk heterojunction, a compact TiO2 electron selective contact and a RuO2 nanoparticle catalyst. The...
Article
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Electrochemical water reduction by employing first row transition metal nanoparticles (NPs) constitutes a sustainable way for the generation of H2. We have synthesized Co-based NPs from a molecular CoII/CoIII precursor after its reductive decomposition at -1.86 V vs. NHE in different organic solvents. These NPs are able to electrochemically reduce...
Article
Ruthenium complexes containing the pentapyridyl ligand 6,6′′-(methoxy(pyridin-2-yl)methylene)di-2,2′-bipyridine (L-OMe) of general formula trans-[RuII(X)(L-OMe-κ-N5)]n+ (X=Cl, n=1, trans-1+; X=H2O, n=2, trans-22+) have been isolated and characterized in solution (by NMR and UV/Vis spectroscopy) and in the solid state by XRD. Both complexes undergo...
Article
Ru complexes containing the pentapyridyl ligand 6,6''-(methoxy(pyridin-2-yl)methylene)di-2,2'-bipyridine (L-OMe) of general formula trans-[RuII(X)(L-OMe--N5)]n+ (X = Cl, n = 1, trans-1+; X = H2O, n = 2, trans-22+) have been isolated and characterized in solution (NMR, UV-Vis) and in the solid state by XRD. Both complexes suffer a series of substit...
Article
In this work, we describe the synthesis of a new N-heterocyclic carbene (NHC) ligand, derived from a hybrid pyrazole-imidazolium scaffold, namely 1-[2-(3,5-dimethylpyrazol-1-yl)ethyl]-3-((S)-1-phenylethyl)-3H-imidazol-2-ylidene (L). This ligand has been used as a stabilizer for the organometallic synthesis of palladium(0) nanoparticles (Pd NPs). L...
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Full-text available
A new CNNC carbene-phthalazine tetradentate ligand has been synthesised, which in the reaction with [Ru(T)Cl3] (T = trpy, tpm, bpea; trpy = 2,2';6',2''-terpyridine; tpm = tris(pyrazol-1-yl)methane; bpea = N,N-bis(pyridin-2-ylmethyl)ethanamine) in MeOH or iPrOH undergoes a C-N bond scission due to the nucleophilic attack of a solvent molecule, with...
Article
A Ru(II)-pentadentate polypyridyl complex [Ru(II)(κ-N(5)-bpy2PYMe)Cl](+) (1(+), bpy2PYMe = 1-(2-pyridyl)-1,1-bis(6-2,2'-bipyridyl)ethane) and its aqua derivative [Ru(II)(κ-N(5)-bpy2PYMe)(H2O)](2+) (2(2+)) were synthesized and characterized by experimental and computational methods. In MeOH, 1(+) exists as two isomers in different proportions, cis (...
Article
Four Metallothioneins (MTs) from soybean (Glycine max) were heterologously synthesized and comparatively analysed by Raman spectroscopy. The participation of protein donor groups (S-thiol and N-imidazol) in Zn(II) chelation, as well as the presence of secondary structure elements was comparatively analysed. Metal clusters with different geometry ca...
Article
Hydrogen release from the splitting of water by simply using sunlight as the only energy source is an old human dream that could finally become a reality. This process involves both the reduction and oxidation of water into hydrogen and oxygen, respectively. While the first process has been fairly overcome, the conversion of water into oxygen has b...
Article
A new bis-facial dinuclear ruthenium complex, {[Ru(II)(bpy)]2(μ-bimp)(μ-Cl)}(2+), 2(2+), containing a hexadentate pyrazolate-bridging ligand (Hbimp) and bpy as auxiliary ligands has been synthesized and fully characterized in solution by spectrometric, spectroscopic, and electrochemical techniques. The new compound has been tested with regard to it...
Article
Plant metallothioneins (MTs) constitute a family of small Cys-rich proteins capable of coordinating metal ions, significantly differing from microbial and animal MTs. They are divided into four subfamilies depending on the Cys pattern in their sequence. In this work, the MT system of the sunflower plant (Helianthus annuus) has been defined, with te...
Article
Full-text available
Metallothioneins (MTs) are a superfamily of Cys-rich, low-molecular weight metalloproteins that bind heavy metal ions. These cytosolic metallopeptides, which exist in most living organisms, are thought to be involved in metal homeostasis, metal detoxification, and oxidative stress protection. In this work, we characterise the Zn(II)- and Cd(II)-bin...
Chapter
The replacement of fossil fuels by hydrogen generated by water splitting with sunlight is a very attractive solution to today's energy problem. In order to develop a practical technology based on these elements, robust and efficient water oxidation catalysts need to be developed. The molecular complexity of this process is high and thus tailored tr...
Article
Full-text available
Chemical communication in the family Hesperiidae (Lepidoptera) is practically unstudied, even though this group includes approximately 4,000 species and represents a fifth of the world’s butterfly fauna.We present the first comparative morphological and chemical analysis of scent organs for nine species in the genus Pyrgus, the most species-rich he...
Article
One clean alternative to fossil fuels would be to split water using sunlight. However, to achieve this goal, researchers still need to fully understand and control several key chemical reactions. One of them is the catalytic oxidation of water to molecular oxygen, which also occurs at the oxygen evolving center of photosystem II in green plants and...
Article
A new family of Ru-Hbpp dinuclear complexes contg. the pos. charged terpyridine deriv. ligand 4-(-p-(pyridin-1-ylmethyl)phenyl)-2,2':6',2'-terpyridine of general formula {[Ru(L1+)]2(μ-bpp)(L-L)}m+ (L-L = μ-Cl, μ-acetato, or (H2O)2; m = 4 or 5) have been synthesized and fully characterized, both in the solid state (X-ray diffraction) and in soln. (1...
Chapter
The replacement of fossil fuels by hydrogen generated by water splitting with sunlight is a very attractive solution to today's energy problem. In order to develop a practical technology based on these elements, robust and efficient water oxidation catalysts (WOCs) need to be developed. The molecular complexity involved in water oxidation is such t...
Article
Full-text available
Much attention has been paid to heterocyclic N-containing ligands due to their applicability as bridging ligands in the synthesis of redox active dinuclear metal complexes. With this aim, we report the synthesis and full characterization of a novel phthalazine-triazole ligand (1,4-bis(1-methyl-1H-1,2,3-triazol-4-yl)phthalazine). Moreover, we show t...
Article
Full-text available
Metallothioneins (MTs) constitute a superfamily of ubiquitous metal-binding proteins of low molecular weight and high Cys content. They are involved in metal homeostasis and detoxification, amongst other proposed biological functions. Two MT isoforms (SpMTA and SpMTB) have been reported in the echinoderm Strongylocentrotus purpuratus (sea urchin),...
Article
A large diversity of transition-metal complexes bearing the dinucleating tetra-N-dentate ligand 3,5-bis(2-pyridyl)pyrazole (Hbpp) is described. Hbpp is a compartamental ligand and can allow the formation of both mononuclear and dinuclear complexes bridged by the pyrazolate unit of the Hbpp. Furthermore, a slightly related ligand even allows the pre...
Article
Metallothioneins (MTs) are a particular type of small metalloprotein that possess a significant amount of Cys residues, which confer upon them an extraordinary capacity for heavy metal binding. Now, more than 50 years after their discovery and after the publication of thousands of papers, it is generally agreed that they are involved in different b...
Article
Two metallothionein (MT) isoforms have been identified in the model nematode Caenorhabditis elegans: CeMT1 and CeMT2, comprising two polypeptides that are 75 and 63 residues in length, respectively. Both isoforms encompass a conserved cysteine pattern (19 in CeMT1 and 18 in CeMT2) and, most significantly, as a result of their coordinative potential...
Article
Full-text available
Data on the metal-binding behaviour of circa 20 recombinant metallothioneins (MTs) from evolutionary divergent organisms, gathered after years of systematic research, are here comprehensively analyzed. The consideration of four independent in vivo and in vitro metal-binding features reveals a gradation of the metal-binding character of the MTs cons...
Article
Full-text available
In contrast with the paradigmatic mammalian metallothioneins (MTs), mollusc MT systems consist at least of a high-cadmium induced form, possibly involved in detoxification, and another isoform either constitutive or regulated by essential metals and probably associated with housekeeping metabolism. With the aim of providing a deeper characterizatio...
Article
Tetrahymena pyriformis MT1 (TpyMT1) is a model among ciliate metallothioneins (MTs). Here, we report on the analytic (ICP-AES, GC-FPD), spectroscopic (CD, UV-Vis, Raman) and spectrometric (ESI-MS) characterization of its recombinant Cd(II)-, Zn(II)- and Cu(I)-complexes, and of those formed during in vitro Zn/Cd and Zn/Cu replacement. In the presenc...
Article
Protein engineering studies suggest that the transition state for the folding of ubiquitin is highly polarised towards the N-terminal part of the sequence and involves a nucleus of residues within the beta-hairpin (residues 1-17) and main alpha-helix (residues 23-34). In contrast, the observation of small phi-values for residues in the C-terminal p...
Article
Ein guter Dienst: Haarnadelschleifen sind eine wichtige Komponente von Proteinstrukturen und Ausgangspunkte für die β-Haarnadel-Faltung. Mit Ubiquitin als „Wirt“-System (siehe Struktur) wurden Protein-Engineering-Methoden verwendet, um den Energiebeitrag von Typ-I′-Haarnadelschleifen zur Stabilität von Proteinen zu bestimmen, wobei das Ziel war, da...
Article
(Figure Presented) One good turn: β-Turns are an important component of protein structure and nucleation sites for β-hairpin folding. With ubiquitin as a "host" system (see structure), protein engineering methods have been used to determine the energetic contribution of type I' β-turns to the stability of proteins, with a view to optimizing the rat...
Article
The N-terminal beta-hairpin sequence of ubiquitin has been implicated as a folding nucleation site. To extend and stabilise the ubiquitin folding nucleus, we have inserted an autonomously folding 14-residue peptide sequence beta4 which in isolation forms a highly populated beta-hairpin (>70%) stabilised by local interactions. NMR structural analysi...
Article
Substitution of trans-proline at three positions in ubiquitin (residues 19, 37 and 38) produces significant context-dependent effects on protein stability (both stabilizing and destabilizing) that reflect changes to a combination of parameters including backbone flexibility, hydrophobic interactions, solvent accessibility to polar groups and intrin...
Article
Haarig: Eine Methode zur Bestimmung der Stabilität einer β-Haarnadelstruktur wird beschrieben. Eine β-Haarnadel bildende Sequenz (β4) wird in natives Ubiquitin (siehe Struktur) eingebaut, wodurch der Protein stabilisierende Beitrag dieses Strukturmotivs abgeschätzt werden kann. Dieser Wert dient als Anhaltspunkt für die maximale Stabilität selbstst...
Article
Back to the fold: A new method to determining the stability of a β hairpin is described. A β hairpin forming sequence (β4) is introduced into native ubiquitin (see structure) enabling the contribution to protein stability of this structural motif to be estimated. This data provides both an upper limit on stability for autonomously folding β hairpin...
Article
Full-text available
We report the synthesis and characterization of a Homarus americanus MT-cDNA (MTH) through retrotranscription of MTH-mRNA from metal-injected lobsters. Heterologous Escherichia coli expression in zinc- and copper-supplemented medium was achieved for MTH, the two domains betabetaMTH and betaalphaMTH and three site-directed mutants, betabetaC9H, beta...
Article
We postulate that zinc(II) is a keystone in the structure of physiological mouse copper metallothionein 1 (Cu-MT 1). Only when Zn(II) is coordinated does the structure of the in vivo- and in vitro-conformed Cu-MT species consist of two additive domains. Therefore, the functionally active forms of the mammalian Cu-MT may rely upon a two-domain struc...
Article
Two Drosophila metallothioneins (MT) have been reported: MTN, a 40 residue peptide including 10 Cys, and MTO, a 43 residue peptide including 12 Cys. However, neither functional nor evolutionary analyses for either of the Drosophila MT are available. Here, heterologous expression of Mtn in Escherichia coli is reported. The metal binding abilities of...
Article
Full-text available
The β domain of mouse metallothionein 1 (βMT) was synthesized in Escherichia coli cells grown in the presence of copper or cadmium. Homogenous preparations of Cu–βMT and Cd–βMT were used to characterize the corresponding in vivo-conformed metal-clusters, and to compare them with the species obtained in vitro by metal replacement to a canonical Zn3–...
Article
The copper(I) and silver(I) binding properties of the beta fragment of recombinant mouse metallothionein I have been studied by electronic absorption and circular dichroism spectroscopy. When possible, the stoichiometry of the species formed was confirmed by electrospray mass spectrometry. The behaviour observed differs from that reported for the n...
Chapter
Heterologous expression in E.coli, coupled with spectroscopic analyses, has enabled the metal binding properties of the recombinant mouse Zn-MT, Zn-αMT and Zn-βMT to be characterized. Cd(II) binding properties of Zn7-MT and Zn4-αMT have shown that they behave like the native proteins and those of the Zn3-βMT fragment have been reported for the firs...

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Project
Tailored design of tunable molecular-material hybrids at the nanoscale for the cost-effective generation of H2 and liquid carbon-neutral fuels.