4.6 Article

New insights into the mesophase transformation of ethane-bridged PMOs by the influence of different counterions under basic conditions

Journal

RSC ADVANCES
Volume 5, Issue 8, Pages 5553-5562

Publisher

ROYAL SOC CHEMISTRY
DOI: 10.1039/c4ra15849k

Keywords

-

Funding

  1. GOA-BOF
  2. University of Antwerp

Ask authors/readers for more resources

The counterions are of crucial importance in determining the mesostructure and morphology of ethanebridged PMO materials synthesized under basic conditions. By using CTABr as the surfactant, the final PMO materials show a 2-D hexagonal (p6mm) mesophase, while PMO materials with cubic (Pm (3) over barn ) mesostructure are obtained when CTACl or CTA(SO4)(1)/(2) are used. With gradually replacing CTABr by CTACl or CTA(SO4) (1)/(2) while keeping the total surfactant concentration constant, a clear p6mm to Pm (3) over barn 3n mesophase evolution process is observed. For a given gel composition, the mesophase of ethanebridged PMO materials can also be adjusted by the addition of different sodium salts. In short, the effect of the counterions on the mesophase can be attributed to the binding strength of the ions on the surfactant micelles, which follows the Hofmeister series (SO42- < Cl- < Br-< NO3- < SCN-). Furthermore, it is found that the hydrolysis and condensation rate of the organosilica precursor also plays an important role in the formation of the final mesostructure

Authors

I am an author on this paper
Click your name to claim this paper and add it to your profile.

Reviews

Primary Rating

4.6
Not enough ratings

Secondary Ratings

Novelty
-
Significance
-
Scientific rigor
-
Rate this paper

Recommended

Article Nanoscience & Nanotechnology

Ferroelectric Gating of Narrow Band-Gap Nanocrystal Arrays with Enhanced Light-Matter Coupling

Charlie Greboval, Audrey Chu, Debora Vale Magalhaes, Julien Ramade, Junling Qu, Prachi Rastogi, Adrien Khalili, Sang-Soo Chee, Herve Aubin, Gregory Vincent, Sara Bals, Christophe Delerue, Emmanuel Lhuillier

Summary: This paper discusses how field-effect transistors (FETs) can be compatible with low-temperature detection and proposes two key developments. By gating nanocrystal films from SrTiO3 and compatibility with a plasmonic resonator, high gate capacitance and broadband absorption are achieved.

ACS PHOTONICS (2021)

Review Chemistry, Multidisciplinary

Three-Dimensional Nanoparticle Transformations Captured by an Electron Microscope

Wiebke Albrecht, Sandra Van Aert, Sara Bals

Summary: The three-dimensional morphology and composition play a crucial role in governing the properties of nanopartides. In situ transmission electron microscopy is a promising tool for studying NP transformations under relevant conditions. By using specialized techniques like tomographic methods or atom counting, along with in situ holders, diffusion processes on a single nanoparticle level can be quantified. This provides valuable insights into the changes in plasmonic and catalytic properties of metal NPs in response to external stimuli.

ACCOUNTS OF CHEMICAL RESEARCH (2021)

Article Chemistry, Multidisciplinary

Understanding and Controlling the Crystallization Process in Reconfigurable Plasmonic Superlattices

Maciej Baginski, Adrian Pedrazo-Tardajos, Thomas Altantzis, Martyna Tupikowska, Andreas Vetter, Ewelina Tomczyk, Radius N. S. Suryadharma, Mateusz Pawlak, Aneta Andruszkiewicz, Ewa Gorecka, Damian Pociecha, Carsten Rockstuhl, Sara Bals, Wiktor Lewandowski

Summary: This study presents proof-of-principle experiments decoding the crystallization of reconfigurable assemblies of nanoparticles in solid state. By utilizing XRD, TEM, and other techniques, the study explores the dependence and correlation in the process of crystallization of nanoparticles, providing insightful information on the anisotropic and reversibly reconfigurable assemblies of NPs.

ACS NANO (2021)

Article Biochemistry & Molecular Biology

On the Track of Long-Range Electron Transfer in B-Type Dye-Decolorizing Peroxidases: Identification of a Tyrosyl Radical by Computational Prediction and Electron Paramagnetic Resonance Spectroscopy

Kevin Nys, Paul Georg Furtmueller, Christian Obinger, Sabine Van Doorslaer, Vera Pfanzagl

Summary: This study investigates the formation of tyrosine radicals in B-type dye-decolorizing peroxidase (KpDyP) and identifies the unique interaction between Y247 and Y92 specific to enterobacterial species. This provides evidence for the existence of long-range electron transfer pathways in B-type DyPs.

BIOCHEMISTRY (2021)

Article Physics, Atomic, Molecular & Chemical

Pitfalls in Sample Preparation of Metalloproteins for Low-Temperature EPR: The Example of Alkaline Myoglobin

Ilenia Serra, Ines Garcia Rubio, Sabine Van Doorslaer

Summary: This study systematically investigates the impact of various factors on the EPR spectrum of myoglobin, focusing on the use of high-pH buffers to induce alkaline transition. The findings show that specific pairs of buffers and cryoprotectants can significantly alter the sample's pH, with ethylene glycol being more effective than glycerol as a cryoprotectant. Additionally, the effect of experimental factors is enhanced at cryogenic temperatures, highlighting the importance of careful selection in EPR studies of metalloproteins.

APPLIED MAGNETIC RESONANCE (2022)

Article Construction & Building Technology

Exploring the oxidative mechanisms of bitumen after laboratory short- and long-term ageing

Georgios Pipintakos, Hilde Soenen, H. Y. Vincent Ching, Christophe Vande Velde, Sabine Van Doorslaer, Filip Lemiere, Aikaterini Varveri, Wim Van den Bergh

Summary: This study focused on identifying the intermediate and final oxygenated products of binders from different crude sources after short- and long-term laboratory ageing. Analyzing the results from FTIR, EPR, H-1 NMR, and TOF-SIMS, it was found that the increase of sulfoxide and carbonyl functional groups, as well as organic carbon-centered radicals, were related to the ageing process and binder characteristics.

CONSTRUCTION AND BUILDING MATERIALS (2021)

Article Chemistry, Inorganic & Nuclear

Copper(II) Complexes of Sulfonated Salan Ligands: Thermodynamic and Spectroscopic Features and Applications for Catalysis of the Henry Reaction

Szilvia Bunda, Nora May, Dora Bonczidai-Kelemen, Antal Udvardy, H. Y. Vincent Ching, Kevin Nys, Mohammad Samanipour, Sabine Van Doorslaer, Ferenc Joo, Norbert Lihi

Summary: Copper(II) complexes formed with sulfonated salan ligands exhibit excellent binding ability and stability, especially when introducing a cyclohexyl moiety. The complexes also show moderate catalytic activity in the Henry reaction, with the best yield achieved by complexes of PrHSS and BuHSS. Despite lower metal binding ability compared to cyclohexyl counterparts, these complexes possess larger spin density on the nitrogen nuclei, affecting their catalytic activity.

INORGANIC CHEMISTRY (2021)

Article Chemistry, Physical

ZnAl layered double hydroxide based catalysts (with Cu, Mn, Ti) used as noble metal-free three-way catalysts

Tim Van Everbroeck, Jianxiong Wu, Daniel Arenas-Esteban, Radu-George Ciocarlan, Myrjam Mertens, Sara Bals, Christophe Dujardin, Pascal Granger, Elena M. Seftel, Pegie Cool

Summary: This research presents a novel approach for developing noble metal-free three-way catalysts using ZnAl layered double hydroxide (LDH) co-precipitated with Mn and Ti. The addition of Cu during the co-precipitation step and a post-synthesis method using the LDH memory effect were explored. The results showed that smaller CuO particle size resulted in better performance for oxidation reactions. The addition of Mn had a positive effect on the general performance of the catalysts, while the presence of Ti mainly improved the NO conversion. The developed materials showed good stability in consecutive catalytic testing cycles and even showed some NO conversion under stoichiometric conditions.

APPLIED CLAY SCIENCE (2022)

Article Chemistry, Multidisciplinary

Direct Solar Energy-Mediated Synthesis of Tertiary Benzylic Alcohols Using a Metal-Free Heterogeneous Photocatalyst

Yu Zhang, Shaowei Qin, Nathalie Claes, Waldemar Schilling, Prakash Kumar Sahoo, H. Y. Vincent Ching, Aleksander Jaworski, Filip Lemiere, Adam Slabon, Sabine Van Doorslaer, Sara Bals, Shoubhik Das

Summary: In this study, a metal-free heterogeneous photocatalyst was developed for the direct hydroxylation of tertiary benzylic C(sp(3))-H bonds using oxygen as the key reagent. The gram-scale reaction was achieved with high product yield using direct solar energy. The high stability of the catalyst was proven through catalyst recycling and spectroscopic analyses, and a possible mechanism was proposed based on experimental evidence.

ACS SUSTAINABLE CHEMISTRY & ENGINEERING (2022)

Correction Electrochemistry

A Versatile In-Situ Electron Paramagnetic Resonance Spectro-electrochemical Approach for Electrocatalyst Research (vol 7, pg 4578, 2020)

Sander Neukermans, Mohammad Samanipour, H. Y. Vincent Ching, Jonas Hereijgers, Sabine Van Doorslaer, Annick Hubin, Tom Breugelmans

CHEMELECTROCHEM (2022)

Article Chemistry, Analytical

Correlation between the Fluorination Degree of Perfluorinated Zinc Phthalocyanines, Their Singlet Oxygen Generation Ability, and Their Photoelectrochemical Response for Phenol Sensing

Liselotte Neven, Hanan Barich, H. Y. Vincent Ching, Shahid U. Khan, Christopher Colomier, Hemantbhai H. Patel, Sergiu M. Gorun, Sammy Verbruggen, Sabine Van Doorslaer, Karolien De Wael

Summary: Electron-withdrawing perfluoroalkyl peripheral groups grafted on phthalocyanine macrocycles improve their properties for catalytic applications, with a high degree of fluorination enhancing reducibility and potentially altering singlet oxygen photoproduction. The use of a specific solvent mixture was found to dissolve perfluorinated complexes and minimize aggregation, while solid-state studies showed potential for developing efficient sensors based on these complexes. The most efficient generator of singlet oxygen was determined to be F52PcZn, highlighting the importance of the value of n and structural features in their applications.

ANALYTICAL CHEMISTRY (2022)

Review Chemistry, Physical

Engineering Heterostructures of Layered Double Hydroxides and Metal Nanoparticles for Plasmon-Enhanced Catalysis

Diana Gilea, Radu G. Ciocarlan, Elena M. Seftel, Pegie Cool, Gabriela Carja

Summary: Artificially designed heterostructures formed by close conjunctions of plasmonic metal nanoparticles and non-plasmonic lamellar nanostructures are of great interest. These heterostructures exhibit localized surface plasmon resonance in the specific environment of the light-absorbing matrix, impacting their potential in plasmon-enhanced catalysis. Layered double hydroxides, with their unique 2D-layered structure and advantages in optical absorption, preparation ease, composition diversity, and high surface area, have emerged as promising candidates for versatile and robust catalysts.

CATALYSTS (2022)

Article Biochemistry & Molecular Biology

Compound I Formation and Reactivity in Dimeric Chlorite Dismutase: Impact of pH and the Dynamics of the Catalytic Arginine

Daniel Schmidt, Nikolaus Falb, Ilenia Serra, Marzia Bellei, Vera Pfanzagl, Stefan Hofbauer, Sabine Van Doorslaer, Gianantonio Battistuzzi, Paul G. Furtmuller, Christian Obinger

BIOCHEMISTRY (2023)

Article Chemistry, Inorganic & Nuclear

Interaction of nitrite with ferric protoglobin from Methanosarcina acetivorans - an interesting model for spectroscopic studies of the haem-ligand interaction

Roberta Sgammato, Niels Van Brempt, Roy Aerts, Sabine Van Doorslaer, Sylvia Dewilde, Wouter Herrebout, Christian Johannessen

Summary: Protoglobin from Methanosarcina acetivorans (MaPgb) is a dimeric globin belonging to the same lineage as globin-coupled sensors. It has a putative role in scavenging reactive nitrogen and oxygen species. Through various spectroscopic techniques, the unusual reaction of ferric MaPgb with nitrite was revealed. Unlike other globins, nitrite did not induce the formation of a nitriglobin form in MaPgb. Instead, it led to the formation of a stable nitric-oxide ligated ferric form of the protein (MaPgb-NO) in mildly acidic pH. The changes in the optical and vibrational properties of MaPgb upon nitric-oxide ligation provide insights into its gas-binding mechanism.

DALTON TRANSACTIONS (2023)

Article Biochemistry & Molecular Biology

Structured LDH/Bentonite Composites for Chromium Removal and Recovery from Aqueous Solutions

Mitra De Geest, Bart Michielsen, Radu-G. Ciocarlan, Pegie Cool, Elena M. Seftel

Summary: This study focuses on the removal of chromium using structured calcined layered double hydroxide (LDH) (MgAl)-bentonite composites through adsorption and ion exchange. The powders were structured into granulates to overcome the limitations of working with powders in real-life applications, and the regeneration of the composites was optimized for multi-cycling operation. The optimized LDH/bentonite ratio showed excellent performance for the removal of Cr3+ and Cr6+ species, and the desorption process was optimized using a 2 M NaCl solution without pH modification.

MOLECULES (2023)

No Data Available