Article
Chemistry, Physical
Silvio Dantas, Katie Cychosz Struckhoff, Matthias Thommes, Alexander V. Neimark
Summary: The study introduces a new method for evaluating pore structures in carbon materials, using high-pressure CO2 adsorption isotherms to determine the pore size distribution in both micro- and mesopores. By utilizing Monte Carlo simulations and meso-canonical ensemble methods, capillary condensation transitions in mesopores were successfully predicted, demonstrating the feasibility of the technique in micro-mesoporous carbon materials.
Article
Chemistry, Multidisciplinary
Anthony Griffin, Genwei Chen, Mark Robertson, Kun Wang, Yizhi Xiang, Zhe Qiang
Summary: Conventional ordered mesoporous carbon (OMC) production requires long processing times, but this work demonstrates accelerated synthesis of OMCs using dielectric barrier discharge plasma, achieving carbonization within 15 minutes. The use of plasma enables faster production rates and does not require additional substrates within the OMC precursor systems.
Article
Green & Sustainable Science & Technology
E. Maruccia, M. A. O. Lourenco, T. Priamushko, M. Bartoli, S. Bocchini, F. C. Pirri, G. Saracco, F. Kleitz, C. Gerbaldi
Summary: D-glucosamine was used as a non-toxic and sustainable C/N source to synthesize nitrogen-containing CMK-8 ordered mesoporous carbons. The resulting NOMCs exhibited large surface area and excellent pore ordering, with high CO2 adsorption capacity and selectivity under various conditions. The combination of a suitable C/N precursor and hard templating synthetic route proved effective in obtaining high-performing, sustainable, and reusable selective CO2 sorbents.
MATERIALS TODAY SUSTAINABILITY
(2022)
Article
Chemistry, Multidisciplinary
Jinsong Shi, Hongmin Cui, Jianguo Xu, Nanfu Yan, Shengyong You
Summary: The influences of porous carbon's physicochemical properties on CO2 adsorption at different pressures were investigated in this study. N-doped hierarchically ordered micro-mesoporous carbons (NHOMCs) were synthesized and their characteristics and CO2 uptake were analyzed. The results showed that NHOMCs exhibited high CO2 adsorption capacity and the adsorption performance was correlated with the physicochemical properties of the materials.
JOURNAL OF CO2 UTILIZATION
(2022)
Article
Chemistry, Multidisciplinary
Uiseok Jeong, HyeonJi Kim, Sreerangappa Ramesh, Nesibe A. Dogan, Sirinapa Wongwilawan, Sungsu Kang, Jungwon Park, Eun Seon Cho, Cafer T. Yavuz
Summary: A new and rapid synthetic route for N-doped ordered mesoporous carbon structure was reported by preferential heating of iron oxide nanoparticles by microwaves. The well-defined cubic mesoporous carbon structure showed remarkable improvement in hydrogen desorption kinetics as a host scaffold for NaAlH4, attributed to their ordered pore structure and N-doping effect.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Nanoscience & Nanotechnology
Felix Markus, Charlotte Vogler, Johanna R. Bruckner, Stefan Naumann
Summary: By using an organocatalytic polymerization method, well-defined amphiphilic block copolyethers can be prepared and applied as structure-directing agents in a standard soft templating process to deliver ordered mesoporous carbons with monomodal and narrowly distributed pore diameters. Selective tuning of pore diameters in the range of 6-18 nm is achievable by judiciously choosing the properties of the structure-directing agents, potentially reducing the effort required to obtain systematically altered materials.
ACS APPLIED NANO MATERIALS
(2021)
Article
Engineering, Environmental
Xiaoning Liu, Junyan Fu, Yiwei Tang, Richard L. Smith, Xinhua Qi
Summary: MgO-doped ordered mesoporous carbon (OMC-MgO) was successfully synthesized using biomass-derived gallic acid, metal ion Mg2+, and F127 as a template through evaporation-induced self-assembly (EISA). The resulting material showed high specific surface area, orderly mesoporous structure, and efficient phosphorus removal capacity, making it a promising candidate for wastewater treatment and catalysis applications.
CHEMICAL ENGINEERING JOURNAL
(2021)
Article
Energy & Fuels
Nilesh Mohan Khalse, Mahuya De
Summary: This study investigated the effect of nitrogen doping on the adsorptive removal of sulfur compounds from model fuel. Nitrogen doping improved the surface area and pore volume of templated carbon, thereby enhancing the adsorption capacity of sulfur compounds. The adsorption-regeneration cycles showed that the removal efficiency was only lowered by 4-10% after five cycles.
Article
Chemistry, Applied
Enrique Garcia-Diez, Alberto Castro-Muniz, Juan Ignacio Paredes, M. Mercedes Maroto-Valer, Fabian Suarez-Garcia, Susana Garcia
Summary: Activated ordered mesoporous carbon (AOMC) sorbents have been synthesized, characterized, and evaluated for CO2 capture. Both physical and chemical activation processes were applied, with the best chemical activated AOMC achieved at 850℃ with a KOH: carbon ratio of 4:1, and the best physical activated AOMC obtained after 48 hours with a burn-off degree of 48%. The ordered mesoporous structure was found to facilitate CO2 diffusion into the micropores of the porous carbons, with performance remaining constant over multiple adsorption-desorption cycles.
MICROPOROUS AND MESOPOROUS MATERIALS
(2021)
Article
Engineering, Environmental
Xu Liu, Fei-Feng Mao, Zhang-Min Li, Zhao-Hui Xu, Xue-Jun Shu, Jin-Peng Mi, Yan Zhou, Duan-Jian Tao
Summary: N-functionalized ordered mesoporous carbons were prepared through a solvent-free self-assembly strategy for selective capture and separation of sulfur dioxide. These materials exhibit high capture capacity and stability.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Chemistry, Physical
Yaqian Lin, Zeyu Hu, Ying Shao, Zhi Chen, Xiangru Wei, Zhangxiong Wu
Summary: N/S-doped carbon materials show great promise for the oxygen reduction reaction (ORR), and the key to enhancing their performance lies in constructing uniform doping with desirable configurations and engineering the pore structure. A single-precursor design and a solvent-free nanocasting approach were utilized to synthesize N/S/O-doped ordered mesoporous carbons with high surface areas, large pore volumes, and excellent ORR performance.
Article
Engineering, Environmental
Xiaobo Lei, Lunguang Yao, Qiyu Lian, Xu Zhang, Tiejun Wang, William Holmes, Guoyu Ding, Daniel Dianchen Gang, Mark E. Zappi
Summary: The study found that ordered mesoporous carbons with lower oxygen content showed better adsorption efficiency and faster adsorption rate for PFOA. Multi-layer adsorption of PFOA onto mesoporous carbons was proposed, with background salts having a positive effect on adsorption and humic acid competing for adsorption sites.
JOURNAL OF HAZARDOUS MATERIALS
(2022)
Article
Biochemistry & Molecular Biology
Barbara Szczesniak, Sylwia Glowniak, Jakub Wozniak, Stanislaw Popiel, Jerzy Choma, Mietek Jaroniec
Summary: A facile mechanochemical method was used to synthesize ordered mesoporous carbons with well-dispersed metal nanoparticles. The as-prepared carbons exhibited hexagonally ordered cylindrical mesopores with narrow pore size distributions, and the uniform decoration of carbons with small-sized metal particles was essential for high hydrogen storage capacities. This synthesis strategy has great potential in applications such as adsorption and catalysis.
Article
Chemistry, Multidisciplinary
Junyan Fu, Chang Chen, Richard Lee Smith Jr, Xinhua Qi
Summary: The alcohol-soluble fraction of humins can be directly transformed into ordered mesoporous carbons (OMCs) using the solvent evaporation-induced self-assembly (EISA) method. The resulting OMCs have well-defined mesoporous structures and high adsorption capacity for macromolecular organic pollutants.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Chemistry, Multidisciplinary
Xinyu Li, Hiroki Yoshikawa, Kaito Ishihara, Koji Miyake, Yoshiaki Uchida, Norikazu Nishiyama
Summary: Incorporation of magnesium nitrate into the precursors during the synthesis of ordered mesoporous carbons improved pore uniformity and volume. The addition of magnesium nitrate lowered the melting point of resorcinol, increased diffusivity, and promoted self-assembly. It resulted in a modification of the pore structure and prevented shrinkage under high-temperature conditions, enhancing uniformity and mesopore volume. This novel method also significantly increased the capacity of electric double-layer capacitors.
Article
Chemistry, Organic
Jonas Everaert, Maarten Debruyne, Flore Vanden Bussche, Kristof Van Hecke, Thomas S. A. Heugebaert, Pascal Van der Voort, Veronique Van Speybroeck, Christian Stevens
Summary: This paper presents the synthesis of new nitrile-functionalized N-heterocyclic ligands, which vary in the extent of the aromatic system and denticity. These ligands can be used for rational design of enhanced support materials in catalysis.
SYNTHESIS-STUTTGART
(2023)
Article
Thermodynamics
Kevin De Ras, Marvin Kusenberg, Joris W. Thybaut, Kevin M. Van Geem
Summary: Oxymethylene ethers (OMEs) are synthetic compounds that can replace fossil fuels and contribute to a circular carbon economy. However, little is known about their thermal decomposition behavior. In this study, new insights into the pyrolysis chemistry of oxymethylene ether-2 (OME-2) and the role of carbenes were obtained through high-temperature experiments. The major products of OME-2 pyrolysis included dimethoxymethane, formaldehyde, methyl formate, methane, CO2, CO, and H2. A kinetic model was developed to simulate the experimental results and predict the major product trends.
PROCEEDINGS OF THE COMBUSTION INSTITUTE
(2023)
Article
Chemistry, Physical
Evert Dhaene, Simon Coppenolle, Loren Deblock, Klaartje De Buysser, Jonathan De Roo
Summary: We introduced monoalkyl phosphinic acids as ligands for nanocrystal (NC) synthesis, which show interesting reactivity differences compared to other ligands and provide a cleaner work-up in comparison to phosphonates. In this study, we investigated the binding affinity of monoalkyl phosphinate ligands with respect to other ligands through competitive ligand exchange reactions on the surface of NCs. Our results showed that carboxylate ligands can be easily exchanged with monoalkyl phosphinic acids, while an equilibrium is reached between monoalkyl phosphinates and phosphonates, slightly favoring phosphonate. These findings enable the sophisticated use of monoalkyl phosphinic acids for NC synthesis and post-synthetic surface engineering.
CHEMISTRY OF MATERIALS
(2023)
Article
Engineering, Electrical & Electronic
Hannes Rijckaert, Klaartje De Buysser, Isabel Van Driessche
Summary: Chemical solution deposition (CSD) approach was used to simplify and optimize the trifluoracetic based MTiO3 precursor solution, resulting in high shelf-life and purity. The growth of MTO solutions on (100) LaAlO3 single-crystal substrates produced (h00) oriented and dense MTO buffer layers. However, the roughness of MTO films and the lattice mismatch between MTO buffer layer and superconducting YBa2Cu3O7-delta film are crucial for film formation.
IEEE TRANSACTIONS ON APPLIED SUPERCONDUCTIVITY
(2023)
Article
Engineering, Chemical
Sebastien Siradze, Jeroen Poissonnier, Ana Costa R. da Cruz, Joris W. Thybaut
Summary: This article proposes a top-down methodology for kinetic model construction, which includes regression against experimental data. Methane steam reforming (MSR) and water-gas shift (WGS) reactions on a nickel catalyst at 923 K are used as a case study. The level of detail in the reaction mechanism and corresponding model is gradually enhanced, ranging from a simple power law to a microkinetic model. The transient solution of the reactor equations overcomes the numerical challenges faced in steady-state solutions, especially for microkinetic models. The best balance between detail accounted for and parameter significance is achieved using a Langmuir-Hinshelwood-Hougen-Watson (LHHW) mechanism, with CO formation and COOH formation as rate-determining steps for MSR and WGS, respectively.
Article
Engineering, Environmental
Bram Van Wettere, Joris W. Thybaut, Erhin de Werd, Saleh Aghakhani, Jeroen Lauwaert
Summary: An elementary-step kinetic model is developed for the synthesis of ethyl acetate using a silica supported silicotungstic acid catalyst. The model accurately predicts the effects of various conditions on conversions and selectivities. It also identifies two physicochemical phenomena that need to be considered for a better fit between experimental and predicted values. The model provides insights that are crucial for optimizing and innovating production plants.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Francis Bru, Sofie M. P. Vanden Broeck, Gianmarco Pisano, Klaartje De Buysser, Catherine S. J. Cazin
Summary: This article describes the implementation of a laboratory exercise in an undergraduate chemistry course where students compare three different synthetic methods for [Cu(Cl)(IPr)]-complexes. The exercise introduces students to the concepts of continuous improvement in reactions using green chemistry and mechanochemistry as a synthetic methodology. By directly comparing the three methods, students learn about green chemistry metrics and are challenged to question the use of solvents in chemical syntheses.
JOURNAL OF CHEMICAL EDUCATION
(2023)
Article
Nanoscience & Nanotechnology
Laurens Bourda, Anna M. Kaczmarek, Min Peng, Sonali Mohanty, Hannes Rijckaert, Pascal Van Der Voort, Kristof Van Hecke
Summary: In this study, hybrid crystalline lanthanide-containing 3D covalent organic framework (Ln@3D COF) materials were developed for temperature sensing applications. Different approaches were tested to obtain these hybrid materials and their material quality and thermometric properties were compared. Luminescent materials derived from these approaches were tested as ratiometric temperature sensors, showing excellent temperature sensing properties. The findings of this study open up a new pathway for potential multifunctional materials combining thermometry with other modalities in just one nanocomposite material.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Materials Science, Ceramics
Bianca Swanckaert, Olivier Verschatse, Eva Loccufier, Klaartje De Buysser, Lode Daelemans, Karen De Clerck
Summary: This study reveals that electrospun silica nanofiber membranes have great potential in environmental applications, but their mechanical performance is not well known. Compared to conventional nanofiber membranes, silica nanofiber membranes exhibit a completely different deformation behavior due to their unique chemical and physical properties. Additionally, storing the membranes at room temperature results in significant changes in failure mechanisms, which can be accelerated through thermal treatment. These findings demonstrate the possibility of mechanical tunability in silica nanofiber membranes by adjusting the storage or treatment conditions.
CERAMICS INTERNATIONAL
(2023)
Article
Thermodynamics
Kevin De Ras, Thomas Panaget, Yann Fenard, Jeroen Aerssens, Laure Pillier, Joris W. Thybaut, Guillaume Vanhove, Kevin M. Van Geem
Summary: Oxymethylene ethers have attracted attention as a potential alternative to fossil fuels. This study investigated the low-temperature oxidation chemistry of oxymethylene ether-2 through experiments and kinetic modeling. Experimental data obtained from stabilized cool flames revealed the formation of various reaction products. A detailed kinetic model was developed, which accurately predicted the experimental observations and ignition delay times.
COMBUSTION AND FLAME
(2023)
Article
Materials Science, Multidisciplinary
Ewout Picavet, Hannes Rijckaert, Eduardo Solano, Oier Bikondoa, Edgar Gutierrez Fernandez, Petriina Paturi, Laura Van Bossele, Henk Vrielinck, Jeroen Beeckman, Klaartje De Buysser
Summary: The integration of ferroelectric thin films on silicon or silicon nitride platforms plays a crucial role in miniaturizing electronic and photonic components. However, the current integration processes are slow, complex, and expensive. To overcome this, a high-throughput method using an ultrathin La2O2CO3 template film to integrate fiber textured ferroelectric thin films has been investigated. The results show that the La2O2CO3 thin film enables the integration of highly textured ferroelectric thin films on Si or SiN-based platforms, offering potential for large-scale miniaturization of photonic or electronic devices.
JOURNAL OF MATERIALS CHEMISTRY C
(2023)
Article
Chemistry, Multidisciplinary
Amrita Chatterjee, Linyang Wang, Pascal Van Der Voort
Summary: There is an urgent need for cleaner production processes in the chemical field. Heterogeneous photocatalysis, which converts (visible) light into chemical energy, shows promise as an efficient alternative. Metal-organic frameworks (MOFs) have emerged as a favorable material for photocatalysis due to their large surface area, tunable properties, versatile functionality, and ability to form composites. Research is focusing on constructing Z-scheme heterojunctions in MOFs to enhance light harvesting capacity and improve the redox ability of photocatalysts.
CHEMICAL COMMUNICATIONS
(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, Physical
Linyang Wang, Jiamin Sun, Maojun Deng, Chunhui Liu, Servet Ataberk Cayan, Korneel Molkens, Pieter Geiregat, Rino Morent, Nathalie De Geyter, Jeet Chakraborty, Pascal Van Der Voort
Summary: This study introduces two benzothiadiazole-based COFs with tunable electronic structures and electron affinities for photocatalytic H2O2 production. The triazine-containing TAPT-BT-COF exhibits outstanding charge separation and achieves high H2O2 production rate in pure water.
CATALYSIS SCIENCE & TECHNOLOGY
(2023)
Review
Chemistry, Physical
Jiamin Sun, Jeet Chakraborty, Maojun Deng, Andreas Laemont, Xiao Feng, Ying-Ya Liu, Pascal van der Voort
Summary: This review provides a comprehensive overview of the intrinsic characteristics of MOFs and COFs, focusing on strategies to enhance light harvesting, charge separation, charge mobility, and the associated oxidation and reduction reactions. By addressing current limitations, it explores H2O2 production mechanisms and outlines future directions for improved photocatalytic performance.
JOURNAL OF MATERIALS CHEMISTRY A
(2023)