Article
Environmental Sciences
Nicole A. DiBlasi, Agost G. Tasi, Xavier Gaona, David Fellhauer, Kathy Dardenne, Joerg Rothe, Donald T. Reed, Amy E. Hixon, Marcus Altmaier
Summary: The impact of calcium on the Pu(IV)-EDTA system was investigated, revealing the formation of a quaternary complex CaPu(OH)4(EDTA)2- in the presence of calcium, significantly enhancing plutonium solubility.
SCIENCE OF THE TOTAL ENVIRONMENT
(2021)
Article
Geochemistry & Geophysics
Neha Mehta, Delphine Vantelon, Juliette Gaetan, Alejandro Fernandez-Martinez, Ludovic Delbes, Cynthia Travert, Karim Benzerara
Summary: The short-range order of bacterial intracellular amorphous calcium carbonates (ACC) remains largely unexplored. In this study, X-ray absorption near-edge structure (XANES) and extended X-ray absorption fine structure (EXAFS) spectroscopies were used to investigate the calcium speciation and coordination environment in intact cells of diverse ACC-forming cyanobacteria. The findings reveal that XANES is effective in detecting ACC in intact cells and that the short-range order of cyanobacterial ACC is different from eukaryotic ACC, resembling monohydrocalcite. These results provide insights into the fate of cyanobacterial ACC and the role of ACC-forming cyanobacteria in the biogeochemical cycle of calcium.
Article
Engineering, Environmental
Alain Manceau, Anne-Claire Gaillot, Pieter Glatzel, Yves Cherel, Paco Bustamante
Summary: The study confirms that mercury toxicity may be underestimated when the molar ratio of selenium to mercury is relatively high, as mercury binds extensively to selenoproteins, reducing the storage of bioavailable selenium for detoxifying MeHg. Additionally, the research shows that Hg(Sec)4 could severely deplete the bioavailable selenium in muscle tissue, potentially causing harm from mercury toxicity in terrestrial animals.
ENVIRONMENTAL SCIENCE & TECHNOLOGY
(2021)
Article
Environmental Sciences
Chengke Fu, Yichao He, Chengyun Yang, Jieyu He, Luna Sun, Yixin Pan, Liping Deng, Rui Huang, Manli Li, Kaikai Chang
Summary: In this study, FeS nanoparticles were anchored onto biochar (BC) to remove Se(IV) from simulated wastewater. The FeS-BC nanomaterials showed excellent performance in removing Se(IV) at pH 3.0, with a maximum removal capacity of 174.96 mg/g. The removal process involved adsorption by surface complexation and reductive precipitation of Se(IV) into Se-0. The FeS-BC nanomaterial exhibited great potential for the remediation of Se(IV).
ECOTOXICOLOGY AND ENVIRONMENTAL SAFETY
(2023)
Article
Chemistry, Physical
Jisheng Kou, Xiangyue Wei, Hui Wu, Wensheng Linghu, Guodong Sheng, Yixin Pan
Summary: The study investigated the removal of U(VI) and Se(IV) from aqueous solutions using FeS@h-BN nanocomposite and characterized the process using spectroscopy techniques. Results showed that the FeS@h-BN nanocomposite had a large surface area and potential, leading to excellent decontamination performance. The adsorption of U(VI) and Se(IV) on FeS@h-BN was mainly driven by chemical interaction. The pH of the solution played a significant role in the adsorption process due to its influence on the surface potential and speciation of U(VI) and Se(IV).
JOURNAL OF MOLECULAR LIQUIDS
(2022)
Article
Chemistry, Physical
Xiangyue Wei, Yixin Pan, Jisheng Kou, Rui Huang
Summary: The study focuses on the removal of selenium (IV) from aqueous solutions using a new type of composite adsorbent called FeS@h-BN nanocomposite. SEM, FTIR, XRD, and XPS analyses were conducted to investigate the surface properties of the coated layer. The effectiveness of different adsorbent materials in removing Se(IV) in dynamic water was examined using the Adams-Bohart, Thomas, and Yoon-Nelson models.
SURFACES AND INTERFACES
(2023)
Article
Chemistry, Physical
Hui Wu, Junjie Chen, Lingxia Xu, Xiaojie Guo, Ping Fang, Kui Du, Chao Shen, Guodong Sheng
Summary: The study found that FeS/MOFs effectively decontaminate Cr (VI) and Se (IV) through an adsorption process, with the pseudo-second order kinetics model fitting the best. The adsorption of Cr (VI) and Se (IV) is influenced by medium pH, adsorption dosage, and temperature, and the Langmuir model best describes their adsorption isotherm on FeS/MOFs. XPS analysis revealed that both surface adsorption and reduction play a role in the decontamination of Cr (VI) and Se (IV) using FeS/MOFs, suggesting the potential of FeS/MOFs nanocomposite as a cost-effective and environmentally friendly adsorbent for wastewater treatment.
COLLOIDS AND SURFACES A-PHYSICOCHEMICAL AND ENGINEERING ASPECTS
(2021)
Article
Chemistry, Physical
S. Kanthal, P. Manna, Md A. Ahmed, A. Banerjee, S. Adhikary, S. Kanungo, A. K. Yadav, S. N. Jha, D. Bhattacharyya, S. Bandyopadhyay
Summary: The study demonstrated that doping rare earth (RE)-Nd based cuprate francisite with cobalt significantly enhances magnetic properties, including magnetic hysteresis and magnetic field induced metamagnetic transition. First principle theoretical calculations and local structural studies help explain these phenomena and detect unexpected trends in magnetism with increasing cobalt doping.
APPLIED SURFACE SCIENCE
(2021)
Article
Automation & Control Systems
Xi Jie Zhang, Feng Li, Ye Wang, Zi Yu Chen
Summary: This study introduces a new method called staggered extrusion (SE) to solve the bottleneck in traditional curvature product manufacturing processes. The key to this method is quantitatively controlling the curvature of extruded products. The research findings show that the staggered distance has a significant impact on curvature, with an increase in staggered distance leading to an increase in curvature.
INTERNATIONAL JOURNAL OF ADVANCED MANUFACTURING TECHNOLOGY
(2022)
Article
Chemistry, Physical
Guokai Huang, Teng Li, Xian Zhang, Lingyu Wang, Daqing Cui, Miao Yang
Summary: This study investigated the corrosion behavior of 304 stainless steel in simulated groundwater and found that corrosion products effectively reduced the dissolution of Se.
Article
Engineering, Chemical
Maarten Houlleberghs, Loes Verheyden, Filip Voorspoels, C. Vinod Chandran, Karel Duerinckx, Sambhu Radhakrishnan, Johan A. Martens, Eric Breynaert
Summary: Magnetohydrodynamic mixing was evaluated as an alternative method to conventional high shear mixing for preparing carbomer hydrogels. Results showed that magnetohydrodynamic mixing can adjust the viscosity of the hydrogel and achieve higher concentrations of TEA.
Article
Chemistry, Analytical
Hannah Vanderschaeghe, Maarten Houlleberghs, Loes Verheyden, Dirk Dom, C. Vinod Chandran, Sambhu Radhakrishnan, Johan A. Martens, Eric Breynaert
Summary: Porous silica is commonly used to enhance the bioavailability of poorly soluble compounds in drug delivery. Traditional methods for residual solvent quantification in drug formations are tedious and involve extraction and capillary gas chromatography. This study presents a new method using magic-angle spinning nuclear magnetic resonance spectroscopy, originally developed for water quantification in zeolites. The results show that the initial water content of the silica carrier can impact the residual solvent concentration in drug-loaded materials.
ANALYTICAL CHEMISTRY
(2023)
Article
Chemistry, Multidisciplinary
Karel Asselman, Mohamed Haouas, Maarten Houlleberghs, Sambhu Radhakrishnan, Wauter Wangermez, Christine E. A. Kirschhock, Eric Breynaert
Summary: Recently discovered zeolite precursors, hydrated silicate ionic liquids (HSIL), simplify the study of zeolite crystallization by minimizing the correlation of synthesis variables and elucidating the role of water. By conducting hydrothermal treatment of Al-doped potassium HSIL, porous merlinoite (MER) zeolite is formed when H2O/KOH exceeds 4, while dense, anhydrous megakalsilite is formed when H2O/KOH is lower. The selectivity of phase formation is determined by cation hydration, water activity, and affinity to coordinate with aluminosilicate or water.
CRYSTAL GROWTH & DESIGN
(2023)
Article
Chemistry, Multidisciplinary
Ewoud Vaneeckhaute, Jean-Max Tyburn, James G. Kempf, Johan A. Martens, Eric Breynaert
Summary: Amino acids and ammonia are essential metabolic markers for nitrogen metabolism and cellular regulation. This study demonstrates a high-field approach using NMR to investigate these metabolic pathways, providing a valuable alternative to existing techniques. By designing a specialized catalyst, spin order can be transferred from p-H-2 to N-15, allowing for reversible hyperpolarization of alanine and ammonia under ambient conditions. The stereochemistry and kinetics of these catalyst complexes are determined using isotopological fingerprinting and 2D-ZQ-NMR.
Review
Chemistry, Multidisciplinary
Karel Asselman, Christine Kirschhock, Eric Breynaert
Summary: Since the 1940s, researchers have been aiming to rationally design zeolites by controlling their synthesis to obtain desired properties. However, the fundamental processes of zeolite synthesis have remained largely unknown. This Account presents recent progress in crystallizing zeolites using hydrated silicate ionic liquids as synthesis media, allowing for the evaluation of the individual impacts of synthesis parameters on zeolite nucleation, growth, and phase selection. The relationship between the characteristics of the synthesis medium and the properties and structure of the crystalline product is elucidated.
ACCOUNTS OF CHEMICAL RESEARCH
(2023)
Article
Nanoscience & Nanotechnology
Maarten Debruyne, Sander Borgmans, Sambhu Radhakrishnan, Eric Breynaert, Henk Vrielinck, Karen Leus, Andreas Laemont, Juul De Vos, Kuber Singh Rawat, Siebe Vanlommel, Hannes Rijckaert, Hadi Salemi, Jonas Everaert, Flore Vanden Bussche, Dirk Poelman, Rino Morent, Nathalie De Geyter, Pascal Van Der Voort, Veronique Van Speybroeck, Christian V. Stevens
Summary: Covalent organic frameworks (COFs) are a new type of photoactive organic semiconductors with ordered structures and high surface areas. The band gaps of COFs can be tuned by the choice of building blocks and linkages, making them tailor-made for specific (photocatalytic) applications. However, there are still many unexplored building blocks for COFs as photocatalytic moieties, and the scope of photocatalyzed reactions by COFs is limited.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Multidisciplinary
Hannelore Geerts-Claes, Gina Vanbutsele, Sreeprasanth Pulinthanathu Sree, Sambhu Radhakrishnan, C. Vinod Chandran, Eric Breynaert, Johan A. Martens, Sam Smet
Summary: RHO zeolites with different Si/Al ratios and particle morphologies were successfully synthesized by adding crown ether and adjusting the sodium content. The zeolites showed exceptional stability even at low Si/Al ratios, which can be attributed to the double eight-ring framework.
CRYSTAL GROWTH & DESIGN
(2023)
Article
Biochemistry & Molecular Biology
Sambhu Radhakrishnan, Sam Smet, C. Vinod Chandran, Sreeprasanth Pulinthanathu Sree, Karel Duerinckx, Gina Vanbutsele, Johan A. Martens, Eric Breynaert
Summary: Selective catalytic reduction (SCR) is a major technology for reducing emissions from diesel engines, and variable temperature NMR can be used to predict the activity of Cu-zeolite SCR catalysts.
Article
Multidisciplinary Sciences
Emile Jules Beckwee, Geert Watson, Maarten Houlleberghs, Daniel Arenas Esteban, Sara Bals, Pascal Van Der Voort, Eric Breynaert, Johan Martens, Gino Baron, Joeri F. M. Denayer
Summary: This study reports a new type of periodic mesoporous organosilica (PMO) nanotubes, referred to as hollow ring PMO (HR-PMO), capable of promoting methane clathrate hydrate formation under mild working conditions and at high water loading. The HR-PMO nanotubes exhibit a steep single-stepped isotherm and a noticeably high methane storage capacity. Supported by ex situ cryo-electron tomography and x-ray diffraction, the findings suggest that HR-PMO nanotubes promote clathrate hydrate nucleation and growth by distributing and confining water in the mesopores of their outer wall, central channels, and external surface. These results highlight the potential application of organosilica materials for pressure-based storage of biomethane in confined clathrate hydrates.
Article
Chemistry, Multidisciplinary
Sambhu Radhakrishnan, Charlotte Lejaegere, Karel Duerinckx, Wei-Shang Lo, Alysson F. F. Morais, Dirk Dom, C. Vinod Chandran, Ive Hermans, Johan A. A. Martens, Eric Breynaert
Summary: During the liquid phase adsorption of C-1-C-5 primary alcohols on high silica MFI zeolites, the concentration of adsorbed molecules exceeds the traditional adsorption sites. This additional adsorption is driven by hydrogen bonding between the alcohol function and the zeolite siloxane bridges, while chemi- and physi-sorption on traditional sites also occur simultaneously.
MATERIALS HORIZONS
(2023)
Article
Chemistry, Physical
Geert Watson, Nithin B. Kummamuru, Sammy W. Verbruggen, Patrice Perreault, Maarten Houlleberghs, Johan Martens, Eric Breynaert, Pascal van der Voort
Summary: This study explores the use of hydrophobic periodic organosilica nanoparticles for hydrogen storage as clathrate hydrates. The surface decoration with promoter agents enhances the formation and growth kinetics of clathrate hydrates, resulting in an increase in hydrogen storage capacity. These findings are of significant importance for the development of hydrogen clathrates in industrial applications.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)
Article
Chemistry, Multidisciplinary
Alysson F. Morais, Ivan G. N. Silva, Bruno J. Ferreira, Alexandre C. Teixeira, Sreeprasanth P. Sree, Huayna Terraschke, Fernando A. Garcia, Eric Breynaert, Danilo Mustafa
Summary: The photoluminescence properties of Eu3+ in layered double hydroxides enable calibrationless quantification of anions in the interlayers. This concept can be used as a remote optical sensor to detect anion intrusion.
CHEMICAL COMMUNICATIONS
(2023)
Article
Chemistry, Physical
Andreas Hoffmann, Michiel De Prins, Sreeprasanth Pulinthanathu Sree, Gina Vanbutsele, Sam Smet, C. Vinod Chandran, Sambhu Radhakrishnan, Eric Breynaert, Johan A. Martens
Summary: This paper investigates the synthesis of LEV type zeolites and their conversion to copper loaded NH3-SCR catalysts. It is found that the synthesis recipe affects the distribution of aluminum in the zeolite, and hydrothermal stability is related to factors such as silanol concentration and crystal morphology. Catalytic activity is dependent on the positioning of aluminum in the double 6-rings.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Nick Pellens, Nikolaus Doppelhammer, Karel Asselman, Barbara Thijs, Bernhard Jakoby, Erwin K. Reichel, Francis Taulelle, Johan Martens, Eric Breynaert, C. E. A. Kirschhock
Summary: This study investigated zeolite crystallization from single phasic hydrated silicate ionic liquids (HSiL) using a specifically designed conductivity measurement set-up, providing access to the crystallization kinetics. A crystallization model based on a surface growth mechanism was proposed, showing that zeolite crystallization from highly ionic media proceeds via a multi-step mechanism involving reversible surface condensation and incorporation of growth units into the crystal. The agreement between experiment and theory suggests that the crystallization process is governed by liquid phase concentration, surface energy, and cation mobility.
FARADAY DISCUSSIONS
(2022)
Article
Chemistry, Multidisciplinary
Maarten Houlleberghs, Loes Verheyden, Filip Voorspoels, C. Vinod Chandran, Karel Duerinckx, Sambhu Radhakrishnan, Johan A. Martens, Eric Breynaert
Summary: Mixing dry carbomer powder with water using magneto-hydrodynamic mixing resulted in carbomer dispersions with higher viscosity and increased storage modulus compared to conventional high shear mixing. This was caused by a different water distribution, lower ionization, and higher degradation of the polymer in the case of high shear mixing.
