ORCID Profile
0000-0003-2480-3222
Current Organisation
University of Amsterdam
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Publisher: American Chemical Society (ACS)
Date: 22-12-2022
DOI: 10.1021/JACS.2C11310
Publisher: American Chemical Society (ACS)
Date: 28-06-2013
DOI: 10.1021/CM401593B
Publisher: Springer Science and Business Media LLC
Date: 02-02-2014
DOI: 10.1038/NCHEM.1861
Abstract: Dye-sensitized solar cells have gained widespread attention in recent years because of their low production costs, ease of fabrication and tunable optical properties, such as colour and transparency. Here, we report a molecularly engineered porphyrin dye, coded SM315, which features the prototypical structure of a donor-π-bridge-acceptor and both maximizes electrolyte compatibility and improves light-harvesting properties. Linear-response, time-dependent density functional theory was used to investigate the perturbations in the electronic structure that lead to improved light harvesting. Using SM315 with the cobalt(II/III) redox shuttle resulted in dye-sensitized solar cells that exhibit a high open-circuit voltage VOC of 0.91 V, short-circuit current density JSC of 18.1 mA cm(-2), fill factor of 0.78 and a power conversion efficiency of 13%.
Publisher: Royal Society of Chemistry (RSC)
Date: 2011
DOI: 10.1039/C1JM10993F
Publisher: Royal Society of Chemistry (RSC)
Date: 2017
DOI: 10.1039/C6TA09181D
Abstract: A controlled growth of nanometric defect-free polydopamine layers leads to its novel demonstration as a hydrogen selective material.
Publisher: Wiley
Date: 15-03-2023
Abstract: Coordination chemistry is a powerful method to synthesize supramolecular cages with distinct features that suit specific applications. This work demonstrates the synthesis of discrete, homochiral Fe II 2 L 3 cages via chirality‐driven self‐assembly. Specifically, the installation of chirality – at both the vertices and ligand backbones – allows the formation of discrete, homochiral Fe II 2 L 3 cages of different sizes via stereochemical control of the iron(II) centers. We observed that larger cages require multiple chiral centra (chiral ligands and vertices). In contrast, the formation of smaller cages is stereoselective with solely chiral ligands. The latter cages can also be formed from two chiral subcomponents, but only when they have matching chirality. Single‐crystal X‐ray diffraction of these smaller Fe II 2 L 3 cages revealed several non‐covalent interactions as a driving force for narcissistic chiral self‐sorting. This expected behavior was confirmed utilizing the shorter ligands in racemic form, yielding discrete, homochiral Fe II 2 L 3 cages formed in enantiomeric pairs.
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C8SE00495A
Abstract: The development of new redox couples provides a clear strategy to improve power conversion efficiency (PCE) in p-type dye-sensitized solar cells (p-DSSCs) through enabling improvements in open-circuit voltage ( V OC ).
Publisher: American Chemical Society (ACS)
Date: 30-09-2021
DOI: 10.1021/JACS.1C04924
Publisher: Wiley
Date: 20-06-2022
Abstract: Reversing the conventional site‐selectivity of C−H activation processes provides new retrosynthetic disconnections to otherwise unreactive bonds. Here, we report a new catalytic system based on palladium/norbornene and an S,O‐ligand for the meta ‐C−H arylation of aryl ethers that significantly outperforms previously reported systems. We demonstrate the unique ability of this system to employ alkoxyarene substrates bearing electron donating and withdrawing substituents. Additionally, ortho ‐substituted aryl ethers are well tolerated, overcoming the “ ortho constraint”, which is the necessity to have a meta ‐substituent on the alkoxyarene to achieve high reaction efficiency, by enlisting novel norbornene mediators. Remarkably, for the first time the monoarylation of alkoxyarenes is achieved efficiently enabling the subsequent introduction of a second, different aryl coupling partner to rapidly furnish unsymmetrical terphenyls. Further insight into the reaction mechanism was achieved by isolation and characterization of some Pd‐complexes—before and after meta C−H activation—prior to evaluation of their respective catalytic activities.
Publisher: Wiley
Date: 24-03-2022
Abstract: This work reports an aqueous dye‐sensitized photoelectrochemical cell (DSPEC) capable of oxidizing glycerol (an archetypical biobased compound) coupled with H 2 production. We employed a mesoporous TiO 2 photoanode sensitized with the high potential thienopyrroledione‐based dye AP11 , encased in an acetonitrile‐based redox‐gel that protects the photoanode from degradation by aqueous electrolytes. The use of the gel creates a biphasic system with an interface at the organic (gel) electrode and aqueous anolyte. Embedded in the acetonitrile gel is 2,2,6,6‐tetramethylpiperidine‐1‐oxyl ( TEMPO ), acting as both a redox‐mediator and a catalyst for oxidative transformations. Upon oxidation of TEMPO by the photoexcited dye, the in situ generated TEMPO + shuttles through the gel to the acetonitrile – aqueous interface, where it acts as an oxidant for the selective conversion of glycerol to glyceraldehyde. The introduction of the redox‐gel layer affords a 10‐fold increase in the conversion of glycerol compared to the purely aqueous system. Our redox‐gel protected photoanode yielded a stable photocurrent over 48 hours of continuous operation, demonstrating that this DSPEC is compatible with alkaline aqueous reactions.
Publisher: Springer Science and Business Media LLC
Date: 24-03-2022
DOI: 10.1038/S41557-022-00905-4
Abstract: Square-planar cobalt(II) systems have emerged as powerful carbene transfer catalysts for the synthesis of numerous (hetero)cyclic compounds via cobalt(III)-carbene radical intermediates. Spectroscopic detection and characterization of reactive carbene radical intermediates is limited to a few scattered experiments, centered around monosubstituted carbenes. Here, we reveal the formation of disubstituted cobalt(III)-carbene radicals derived from a cobalt(II)-tetraphenylporphyrin complex and acceptor-acceptor λ
Publisher: Wiley
Date: 04-07-2013
Publisher: Royal Society of Chemistry (RSC)
Date: 2020
DOI: 10.1039/D0SC03992F
Abstract: A molecular mechanics approach enables the accurate prediction of polyhedral topology for homoleptic and heteroleptic palladium M x L 2x coordination cages, allowing for new insight and design when considering endo- and exo-hedral functionalization.
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D2NR06509F
Abstract: Lead dioxide precursor as an efficient source of highly complexed iodoplumbates for the synthesis of 2D lead halide perovskite microplates.
Publisher: Research Square Platform LLC
Date: 14-02-2023
DOI: 10.21203/RS.3.RS-2384735/V1
Abstract: Selective formation of multicomponent structures via the self-assembly of numerous building blocks is ubiquitous in biological systems but challenging to emulate synthetically. The energy landscape for product formation broadens with increasing number of components, introducing kinetic intermediates with trap-state ability. Therefore, pathway engineering becomes an essential tool to navigate these complex kinetic landscapes and push self-assembly to greater limits. Here, we report an ex le of pathway engineering in the self-assembly of cuboctahedral M 12 L 24 nanospheres through pseudorotaxane formation to the exo -functionalized ligands. Without ring in solution for pseudorotaxane formation, a Pd x –L y polymer resting-state is rapidly formed. Solutions with ring exhibit rapid nanosphere formation from small Pd x –L y oligomers, with Pd x –L y polymer formation bypassed. The threading of ring to an exo -functionalized ligand therefore directs the self-assembly pathway toward nanosphere formation. As the process of pseudorotaxane formation increases rate of nanosphere formation, the ring effectively acts as a supramolecular catalyst for nanosphere self-assembly.
Publisher: American Chemical Society (ACS)
Date: 08-04-2019
Abstract: Porphyrins are attractive chromophores for application in dye-sensitized solar cells (DSCs), as judicious tuning of donor-acceptor properties can enable excellent near-infrared (NIR) absorption and exceptional device performance. Here, we report a porphyrin-based dye (SM85) conjugated to the planar strong electron donor, indolizine, designed to extend absorption further into the NIR region by inducing π-π interactions such as head-to-tail dye aggregation. The optoelectronic consequences of indolizine incorporation in SM85 include raising the ground-state oxidation potential and broadening and red-shifting ultraviolet-visible-NIR absorptions, along with increased molar absorptivity when compared to the dye SM315. Density functional theory (DFT) and time-dependent DFT (TD-DFT) calculations confirm the push-pull character of SM85, which features an overlap of frontier occupied and unoccupied orbitals. Steady-state spectrophotometric analyses reveal the presence of solution aggregates via absorption and emission spectroscopies. Aggregate modes were probed by DFT and TD-DFT analyses, and plausible models are presented. SM85-based DSC devices demonstrate a 5.7% power conversion efficiency (PCE) at full sun (7.4% PCE at 10% sun) with an exceptional improvement to the incident photon-to-current conversion onset at ∼850 nm. Current dynamics measurements, time-correlated single photon counting, and computational analyses are used to better understand device performances. This study puts forward a novel intramolecular charge-transfer porphyrin system with a dramatic shift into the NIR region, as is needed for nonprecious metal-based sensitizers, and provides an ex le of controlled, donor-acceptor-mediated aggregation as a complementary strategy to traditional donor-acceptor modifications to single-molecule π-systems in accessing enhancements in long wavelength light harvesting in molecular-based optoelectronic devices.
Publisher: American Chemical Society (ACS)
Date: 29-06-2011
DOI: 10.1021/JP2030208
Publisher: Springer Science and Business Media LLC
Date: 2009
Publisher: IEEE
Date: 02-2008
Publisher: American Chemical Society (ACS)
Date: 14-06-2008
DOI: 10.1021/JA801142K
Publisher: Elsevier BV
Date: 2012
Publisher: Springer Science and Business Media LLC
Date: 27-10-2022
DOI: 10.1038/S41557-022-01068-Y
Abstract: Molecular photoelectrochemical devices are h ered by electron-hole recombination after photoinduced electron transfer, causing losses in power conversion efficiency. Inspired by natural photosynthesis, we demonstrate the use of supramolecular machinery as a strategy to inhibit recombination through an organization of molecular components that enables unbinding of the final electron acceptor upon reduction. We show that preorganization of a macrocyclic electron acceptor to a dye yields a pseudorotaxane that undergoes a fast (completed within ~50 ps) 'ring-launching' event upon electron transfer from the dye to the macrocycle, releasing the anionic macrocycle and thus reducing charge recombination. Implementing this system into p-type dye-sensitized solar cells yielded a 16-fold and 5-fold increase in power conversion efficiency compared to devices based on the two control dyes that are unable to facilitate pseudorotaxane formation. The active repulsion of the anionic macrocycle with concomitant reformation of a neutral pseudorotaxane complex circumvents recombination at both the semiconductor-electrolyte and semiconductor-dye interfaces, enabling a threefold enhancement in hole lifetime.
Publisher: American Chemical Society (ACS)
Date: 22-11-2021
DOI: 10.1021/JACS.1C10927
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D3SC01086D
Abstract: Two fluorescent, stable Pt 2 L 4 nanocages are developed. Pt 2 L 4 have alternated cytotoxicity and display erse cell uptake in vivo making the versitale nanocages interesting candidates for further delivery and toxicity studies.
Publisher: Wiley
Date: 10-04-2018
Abstract: Two porous coordination polymers (PCPs) with different topologies (NTU-19: sql and NTU-20: dia) underwent finely controlled, stepwise crystal conversions to yield a common water-stable, flexible 2D framework (NTU-22: kgm). The crystal conversions occurred directly at higher temperature via the 3D intermediate (NTU-21: nbo), which could be observed at lower temperature. The successful isolation of the intermediate product of NTU-21, characterization with in situ PXRD and UV/Vis spectra were combined with DFT calculations to allow an understanding of the dynamic processes at the atomic level. Remarkably, breakthrough experiments demonstrate NTU-22 with integral structural properties allowed significant CO
Publisher: Royal Society of Chemistry (RSC)
Date: 2016
DOI: 10.1039/C5TA08728G
Abstract: A panchromatic ullazine–porphyrin dye was synthesized, characterized and applied as a light harvester in dye-sensitized solar cells.
Publisher: American Chemical Society (ACS)
Date: 18-04-2014
DOI: 10.1021/JP502447Y
Publisher: Wiley
Date: 21-06-2022
Abstract: Reversing the conventional site‐selectivity of C−H activation processes provides new retrosynthetic disconnections to otherwise unreactive bonds. Here, we report a new catalytic system based on palladium/norbornene and an S,O‐ligand for the meta ‐C−H arylation of aryl ethers that significantly outperforms previously reported systems. We demonstrate the unique ability of this system to employ alkoxyarene substrates bearing electron donating and withdrawing substituents. Additionally, ortho ‐substituted aryl ethers are well tolerated, overcoming the “ ortho constraint”, which is the necessity to have a meta ‐substituent on the alkoxyarene to achieve high reaction efficiency, by enlisting novel norbornene mediators. Remarkably, for the first time the monoarylation of alkoxyarenes is achieved efficiently enabling the subsequent introduction of a second, different aryl coupling partner to rapidly furnish unsymmetrical terphenyls. Further insight into the reaction mechanism was achieved by isolation and characterization of some Pd‐complexes—before and after meta C−H activation—prior to evaluation of their respective catalytic activities.
Publisher: IEEE
Date: 02-2008
Publisher: IEEE
Date: 02-2008
Publisher: Royal Society of Chemistry (RSC)
Date: 2023
DOI: 10.1039/D3SC03745B
Publisher: Wiley
Date: 24-03-2022
Abstract: This work reports an aqueous dye‐sensitized photoelectrochemical cell (DSPEC) capable of oxidizing glycerol (an archetypical biobased compound) coupled with H 2 production. We employed a mesoporous TiO 2 photoanode sensitized with the high potential thienopyrroledione‐based dye AP11 , encased in an acetonitrile‐based redox‐gel that protects the photoanode from degradation by aqueous electrolytes. The use of the gel creates a biphasic system with an interface at the organic (gel) electrode and aqueous anolyte. Embedded in the acetonitrile gel is 2,2,6,6‐tetramethylpiperidine‐1‐oxyl ( TEMPO ), acting as both a redox‐mediator and a catalyst for oxidative transformations. Upon oxidation of TEMPO by the photoexcited dye, the in situ generated TEMPO + shuttles through the gel to the acetonitrile – aqueous interface, where it acts as an oxidant for the selective conversion of glycerol to glyceraldehyde. The introduction of the redox‐gel layer affords a 10‐fold increase in the conversion of glycerol compared to the purely aqueous system. Our redox‐gel protected photoanode yielded a stable photocurrent over 48 hours of continuous operation, demonstrating that this DSPEC is compatible with alkaline aqueous reactions.
Publisher: Pan Stanford Publishing
Date: 12-01-2012
DOI: 10.1201/B11621-10
Publisher: American Chemical Society (ACS)
Date: 17-10-2022
Publisher: No publisher found
Date: 2012
Publisher: Wiley
Date: 18-12-2009
Publisher: Wiley
Date: 24-08-2023
Abstract: The thermal curing of industrial coatings (e.g., car painting and metal coil coatings) is accompanied by a substantial energy consumption due to the intrinsically high temperatures required during the curing process. Therefore, the development of new photochemical curing processes—preferably using visible light—is in high demand. This work describes new diazo‐based cross‐linkers that can be used to photocure acrylic coatings using blue light. This work demonstrates that the structure of the tethered diazo compounds influences the cross‐linking efficiency, finding that side reactions are suppressed upon engineering greater molecular flexibility. Importantly, this work shows that these diazo compounds can be employed as either thermal or photochemical cross‐linkers, exhibiting identical crosslinking performances. The performance of diazo‐cross‐linked coatings is evaluated to reveal excellent water resistance and demonstrably similar material properties to UV‐cured acrylates. These studies pave the way for further usage of diazo‐functionalized cross‐linkers in the curing of paints and coatings.
Publisher: World Scientific Pub Co Pte Ltd
Date: 07-05-2021
DOI: 10.1142/S1088424621500504
Abstract: A facile synthetic strategy was developed for the synthesis of meso -tetrakis(4-formyl-phenyl)porphyrin and meso -tetrakis(3-formylphenyl)porphyrin from commercially available starting materials. This method gives facile access to practical amounts of these synthons in high purity and good overall yield, without employing laborious chromatographic separations. The reduction of the respective carboxylic acid-functionalized porphyrins by LiAlH 4 afforded the tetra(benzylalcohol)porphyrin intermediates, subsequently utilized in a Parikh-Doering oxidation to selectively afford the desired tetraformylated products. The inherent ease of synthesis of these porphyrin building blocks provides a convenient pathway for the synthesis of various macromolecular and supramolecular architectures for applied chemical technologies.
Publisher: Royal Society of Chemistry (RSC)
Date: 2017
DOI: 10.1039/C6TC05640G
Abstract: Diffusion impediments of redox shuttles are major limitations in realizing high power conversion efficiencies (PCEs) in dye sensitized solar cells (DSCs) using cobalt complexes.
Publisher: Wiley
Date: 16-10-2020
Publisher: Royal Society of Chemistry (RSC)
Date: 2019
DOI: 10.1039/C9CC00901A
Abstract: Hydrogen as a renewable fuel is viable when produced sustainably via proton reduction catalysis (PRC). Encapsulation of a hydrogenase mimic in a supramolecular cage results in a 150 mV decrease of the catalytic overpotential in proton reduction catalysis.
Publisher: Royal Society of Chemistry (RSC)
Date: 2021
DOI: 10.1039/D1SE01275D
Abstract: Dye-sensitised photoelectrochemical cells (DSPECs) for light-driven oxidative organic reactions and simultaneous reductive hydrogen production are reported, using TEMPO as catalyst/mediator either in homogeneous phase or immobilized on the electrode.
Publisher: Wiley
Date: 10-12-2021
Publisher: American Chemical Society (ACS)
Date: 02-10-2013
DOI: 10.1021/NN403384K
Abstract: A hydrophobic gadolinium bis(naphthalocyanine) sandwich complex (GdSand) possessing several absorbances across visible and infrared wavelengths (up to 2500 nm) was solubilized in aqueous solution by uptake into a nascent mutant high-density lipoprotein (HDL) nanocarrier. The HDL nanocarrier was additionally functionalized with a trans-activator of transcription peptide sequence to promote efficient cell penetration of the drug delivery system (cpHDL). The dye-loaded nanocarrier (GdSand@cpHDL) exhibited photothermal heat generation properties upon irradiation with near-infrared (NIR) laser light, with controllable heat generation abilities as a function of the incident laser light power. Comparison of the photothermal behavior of the dyes GdSand and the well-explored molecular photothermal agent indocyanine green (ICG) in the cpHDL nanocarrier (i.e., ICG@cpHDL) revealed two significant advantages of GdSand@cpHDL: (1) the ability to maintain elevated temperatures upon light absorption for extended periods of time, with a reduced degree of self-destruction of the dye, and (2) exclusive photothermal heat generation with no detectable singlet oxygen production leading to improved integrity of the cpHDL nanocarrier after irradiation. Finally, GdSand@cpHDL was successfully subjected to an in vitro study against NCI-H460 human lung cancer cells, demonstrating the proof-of-principle utility of lanthanide sandwich complexes in photothermal therapeutic applications.
Publisher: American Chemical Society (ACS)
Date: 11-08-2017
DOI: 10.1021/JACS.7B05702
Abstract: The prevalence of the condensed phase, interpenetration, and fragility of mesoporous coordination polymers (meso-PCPs) featuring dense open metal sites (OMSs) place strict limitations on their preparation, as revealed by experimental and theoretical reticular chemistry investigations. Herein, we propose a rational design of stabilized high-porosity meso-PCPs, employing a low-symmetry ligand in combination with the shortest linker, formic acid. The resulting dimeric clusters (PCP-31 and PCP-32) exhibit high surface areas, ultrahigh porosities, and high OMS densities (3.76 and 3.29 mmol g
Publisher: American Chemical Society (ACS)
Date: 24-03-2023
Publisher: Wiley
Date: 26-11-2020
No related grants have been discovered for Simon Mathew.