Article
Chemistry, Multidisciplinary
Riki Kadokawa, Takatsugu Endo, Yoshiro Yasaka, Kazuaki Ninomiya, Kenji Takahashi, Kosuke Kuroda
Summary: The study found that ionic liquids were selected as the solvent because the solvent-polysaccharide interaction can be precisely regulated by bulky cations, allowing for the dissolution of cellulose but not xylan. The difference in dissolution behavior was attributed to diffusivity for cellulose and a combination of cation bulkiness and diffusivity for xylan. Molecular dynamics simulations showed that polysaccharides cannot form the most stable state in bulky ionic liquids due to the disorder of hydrogen bonds, supporting the difference in dissolution behavior.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2021)
Article
Biochemistry & Molecular Biology
Huan Zhang, Andreea Ionita, Pilar F. Serinan, Maria Luisa Ferrer, Maria A. Rodriguez, Aitana Tamayo, Fausto Rubio Alons, Francisco del Monte, Maria C. Gutierrez
Summary: Ionic liquids and deep eutectic solvents are widely used neoteric solvents. By adding acetic acid to 1-Ethyl-3-methylimidazolium chloride, the transition from the original ionic liquid to a eutectic mixture of EMIMCl and AcOH can be promoted. The study investigated the effects of this transition on cellulose regeneration and EMIMCl recovery, and demonstrated the potential application for obtaining highly acetylated cellulose.
Article
Agricultural Engineering
Mindaugas Bulota, Darius Ciuzas, Edvinas Krugly, Ingrida Pauliukaityte, Odeta Baniukaitiene, Dainius Martuzevicius
Summary: A new method was developed in this study for preparing lightweight fiber-reinforced composites, which combined cellulose dissolution, fiber production through electrospinning, and composite preparation. The use of ionic liquid BMIMAc in the electrospinning process effectively prevented fiber fusion, resulting in strong, tough fiber-reinforced composites.
INDUSTRIAL CROPS AND PRODUCTS
(2022)
Article
Materials Science, Multidisciplinary
Rose J. Miller, Vanessa M. Smith, Stacy A. Love, Sarah M. Byron, David Salas-de la Cruz, Kevin M. Miller
Summary: By functionalizing cellulose with 1,2,3-triazolium groups, derivatives were obtained with observed T-g values inversely related to the size of the counteranions, indicating dependence on anion basicity and hydration for thermal and ionic conductivity properties.
ACS APPLIED POLYMER MATERIALS
(2021)
Article
Polymer Science
Daisuke Sawada, Yoshiharu Nishiyama, Thomas Roeder, Lionel Porcar, Hilda Zahra, Mikaela Trogen, Herbert Sixta, Michael Hummel
Summary: The nanometric internal structure of polymeric fibres plays a vital role in their mechanical properties. This study examined the correlation between structural parameters and mechanical properties of regenerated cellulose fibres prepared using various spinning technologies, finding a high correlation in the former group but lower correlation in the latter group. These structural parameters serve as a basis for understanding the structure-property relationship and optimizing fibre production based on spinning types and conditions.
Article
Materials Science, Paper & Wood
Ashley Victoria, Peter John Hine, Keeran Ward, Michael Edward Ries
Summary: In this study, statistical design of experiments (DoE) was used to optimize all cellulose composites (ACCs) made from cotton textile and interleaf films. The optimized samples showed improved mechanical properties and density, highlighting the potential of DoE for understanding and optimizing ACC processes.
Article
Chemistry, Applied
Yunhao Liang, Michael E. Ries, Peter J. Hine
Summary: This study establishes three methods to explore the dissolution kinetics of cellulosic fibers in a specific ionic liquid. By analyzing the microscopic images of processed samples and comparing the temperature, it is found that the dissolution follows an Arrhenius behavior. The study also develops a new method to determine the swelling ratio and water content in different regions of the processed samples.
CARBOHYDRATE POLYMERS
(2022)
Article
Biochemistry & Molecular Biology
Changli Ma, Taisen Zuo, Zehua Han, Yuqing Li, Sabrina Gartner, Huaican Chen, Wen Yin, Charles C. Han, He Cheng
Summary: The atomic picture of cellulose dissolution in alkali/urea aqueous solution is investigated using trehalose as the model molecule and total scattering as the main tool. The study reveals that the hydration shell of trehalose has a layered structure, with smaller alkali ions penetrating glucose rings and larger urea molecules interacting with hydroxide groups to form complexations. The solubility of alkali aqueous solution for cellulose decreases with the alkali cation radius. These findings are important for the design of greener solvents for cellulose.
Article
Materials Science, Paper & Wood
Lorena Villar, Marta Pita, Javier Paez, Pablo B. Sanchez
Summary: In this study, a image-assisted technique based on luminance evolution was applied to investigate the kinetics of cellulose dissolution under different experimental conditions. The validity of this protocol was confirmed by directly determining the dissolved cellulose. The effects of solvent properties were studied using three ionic liquids, and the viscosity of the solvent was identified as a key factor influencing the dissolution process.
Article
Nanoscience & Nanotechnology
John P. Elliott, Naresh C. Osti, Madhusudan Tyagi, Eugene Mamontov, Lifeng Liu, Joel M. Serrano, Ke Cao, Guoliang Liu
Summary: This study investigates the confinement of ionic liquids in block copolymer-based porous carbon fibers (PCFs). It is found that the ion diffusion in PCFs is 7-fold faster than in the bulk, suggesting the exceptional potential of PCFs in electrochemical catalysis, energy conversion, and storage.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Polymer Science
Junmeng Zhao, Wenjiao Ge, Jianbo Shuai, Xiangli Gao, Fengshan Zhang, Xiaohui Wang
Summary: Cellulose is a promising feedstock for sustainable materials, and efficient cellulose solvents are essential for its full utilization. Ten superbase amino acid ionic liquids (SAAILs) were synthesized in this study and their properties varied with their cation and anion structures. The ability of the SAAILs to dissolve cellulose is related to their Kamlet-Taft parameters, especially hydrogen bond basicity (beta). Four SAAILs composed of specific cations and anions were identified as promising solvents for preparing regenerated cellulose films (RCFs) with high tensile strength, high Young's modulus, good transparency, and a smooth surface morphology. These halogen- and metal-free SAAILs offer a new avenue for cellulose processing.
MACROMOLECULAR RAPID COMMUNICATIONS
(2023)
Article
Materials Science, Paper & Wood
Fatimah A. Albarakati, Peter J. Hine, Michael E. Ries
Summary: This study investigated the dissolution rate of flax fibers in the ionic liquid [C2mim][OAc] with the addition of water. The addition of even small amounts of water was found to significantly decrease the speed of dissolution. The measurement of the activation energy for the dissolution of flax fiber showed that the hypothetical dry ionic liquid could dissolve cellulose 23% faster than the ionic liquid as received.
Article
Chemistry, Multidisciplinary
Bart-Jan Niebuur, Leonardo Chiappisi, Florian A. Jung, Xiaohan Zhang, Alfons Schulte, Christine M. Papadakis
Summary: The identification and control of the disintegration mechanism of polymer nanoparticles, particularly poly(N-isopropylacrylamide) (PNIPAM) mesoglobules, are crucial for their applications in transport and release systems. By inducing phase separation through fast pressure jumps, two disintegration mechanisms were observed: the release of single polymers from the surface of mesoglobules leading to size reduction, and the swelling of mesoglobules by water causing the chains to become more loosely associated.
Article
Thermodynamics
Monia A. R. Martins, Filipe H. B. Sosa, Ilkka Kilpelainen, Joao A. P. Coutinho
Summary: This study aims to characterize the physicochemical properties of binary systems of water and two superbase-based ionic liquids, and to experimentally screen potential extractants for the recovery of the ILs. The results show that butanol has a certain extraction efficiency for [mTBDH][OAc].
FLUID PHASE EQUILIBRIA
(2022)
Article
Materials Science, Paper & Wood
Yunhao Liang, James E. Hawkins, Michael E. Ries, Peter J. Hine
Summary: This study investigated the dissolution of cotton fibres in the ionic liquid [C2mim][OAc], showing that the resulting coagulated fraction had a crystal structure predominantly of cellulose II. Despite differences in growth patterns of the coagulated fraction for three distinct fibre arrangements, all could be shifted to form master curves using Time-Temperature Superposition, with very similar activation energies determined.
Article
Chemistry, Physical
Guang Wang, Christopher J. Garvey, Senlin Gu, Weimin Gao, Luke A. O'Dell, Anwen M. Krause-Heuer, Tamim A. Darwish, Alexander Zhigunov, Xin Tong, Lingxue Kong
Summary: Introducing polymerizable monomers into a hexagonal lyotropic liquid crystalline (LLC) template can retain the nanostructure but decrease intra-and inter aggregate interactions. The system with a proper volume ratio of PEGDA/HEMA (1/4) shows excellent homogeneity, higher dimensional stability, and lower dynamic property, resulting in robust, free-standing, transparent membranes after photo-polymerization. The unique property of the system includes a lower order-disorder transition temperature facilitating mesochannel reorientation.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2022)
Article
Nanoscience & Nanotechnology
Claire Buchanan, Ljiljana Puskar, Christopher J. Garvey, Adam Mechler
Summary: Amidation can introduce a third hydrogen bond pair and create a new self-assembly motif, providing a new and easy-to-synthesize helical nanorod self-assembly motif.
Article
Chemistry, Multidisciplinary
Youngju Kim, Jacopo Valsecchi, Ohsung Oh, Jongyul Kim, Seung Wook Lee, Francois Boue, Evelyne Lutton, Matteo Busi, Christopher Garvey, Markus Strobl
Summary: Scattering studies of milk and milk products are important for understanding the microscopic structural differences between dairy samples, which determine the physical properties and consumer experience. This study explores the potential of small-angle neutron scattering and neutron dark-field imaging to investigate the structures of fat globules and milk gel.
APPLIED SCIENCES-BASEL
(2022)
Article
Chemistry, Physical
M. Golub, J. Gaetcke, S. Subramanian, A. Koelsch, T. Darwish, J. K. Howard, A. Feoktystov, O. Matsarskaia, A. Martel, L. Porcar, A. Zouni, J. Pieper
Summary: Small-angle neutron scattering (SANS) provides structural information on PSI and PSII in solution under nearly physiological conditions without the need for crystallization or temperature decrease. Proper contrast matching of the detergent belt surrounding the protein is crucial for the reliability of the solution structure, with specifically deuterated detergents showing promise in this regard. Differences in temperature and solution state compared to high-resolution structures suggest the presence of a manifold of conformational substates accessible by protein dynamics under physiological conditions.
JOURNAL OF PHYSICAL CHEMISTRY B
(2022)
Article
Chemistry, Applied
Michael Moir, Nageshwar Rao Yepuri, David L. Marshall, Stephen J. Blanksby, Tamim A. Darwish
Summary: This article reports a method for the synthesis of perdeuterated linoleic acid-d(31), starting from saturated fatty acids obtained by metal catalysed hydrogen-deuterium exchange. The synthesis involves direct utilization of fatty acids through decarboxylative coupling, copper catalysed coupling, and reduction using P-2 nickel. The subsequent synthesis of tail-deuterated phospholipid, PLPC-d(62), is also described, and its regioisomeric purity is characterised by mass spectrometry techniques.
ADVANCED SYNTHESIS & CATALYSIS
(2022)
Article
Chemistry, Analytical
Dong Hao Wang, Dragoslav Vidovic, Alasdair I. McKay, Tamim Darwish, Hui Gyu Park, Secilia Martinez Garza, Samuel W. Shields, Jennifer S. Brodbelt, Zhen Wang, R. J. Scott Lacombe, Vadim V. Shmanai, Ivan L. Lysenko, Andrei V. Bekish, Karsten Schmidt, Christina Redfield, J. Thomas Brenna, Mikhail S. Shchepinov
Summary: This article describes the deuteration of highly unsaturated fatty acid ethyl esters through Ru-based catalysis and characterizes the extent and kinetics of deuteration using NMR and mass spectrometry analysis.
ANALYTICAL CHEMISTRY
(2022)
Article
Nanoscience & Nanotechnology
Nicolo Paracini, Philipp Gutfreund, Rebecca Welbourn, Juan Francisco Gonzalez-Martinez, Kexin Zhu, Yansong Miao, Nageshwar Yepuri, Tamim A. . Darwish, Christopher Garvey, Sarah Waldie, Johan Larsson, Max Wolff, Marite Cardenas
Summary: Arrays of nanoparticle-supported lipid bilayers (nanoSLB) are lipid-coated nanopatterned interfaces that provide a platform to study curved model biological membranes using surface-sensitive techniques. We investigated the structure of lipid bilayers formed on nanoparticle arrays through vesicle fusion using scattering techniques and direct imaging. The presence of both flat and curved supported lipid bilayers on the same substrate, combined with the accuracy of grazing incidence neutron scattering, offers a promising approach to studying curvature-dependent membrane phenomena.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Chemistry, Physical
Christopher J. Garvey, Saffron J. Bryant, Aaron Elbourne, Taavi Hunt, Ben Kent, Martin Kreuzer, Markus Strobl, Roland Steitz, Gary Bryant
Summary: The maintenance of plasma membrane structure is crucial for cell viability. However, the macroscopic phase separation observed during dehydration and freezing can lead to cell death. Previous studies have shown that POPC can function as a line-active component in lipid vesicles, inhibiting macroscopic phase separation and stabilizing membrane microdomains. However, our research found that under reduced hydration, POPC cannot stabilize microdomains in various model membrane systems.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2023)
Article
Chemistry, Physical
Marzieh Mirzamani, Arnab Dawn, Christopher J. Garvey, Lilin He, Hilmar Koerner, Harshita Kumari
Summary: This article presents a study on the process of supramolecular assembly. By using a slow-evolving urea-based gel, the authors were able to observe and analyze the different stages of self-assembly in real time. The results of this study provide a thorough understanding of the self-assembly process and its potential applications in industries such as cosmetics, 3D printing ink, and paint.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Multidisciplinary
Simon M. Clark, Vili Grigorova, Bruno Colas, Tamim A. Darwish, Kathleen Wood, Joerg Neuefeind, Dorrit E. Jacob
Summary: Magnesium doped Amorphous Calcium Carbonate can be synthesized by adjusting the Mg/Ca ratio in the precursor solution. The resultant Amorphous Calcium Carbonate crystallizes as aragonite, with no Mg present. Changes in the Mg to Ca ratio have minimal effect on nucleation rates but strongly impact crystal growth rates, suggesting a dissolution-reprecipitation model for aragonite formation via an Amorphous Calcium Carbonate intermediate.
Article
Polymer Science
Jordan T. Lovegrove, Ben A. Humphreys, Chin Ken Wong, Liliana de Campo, Anna Wang, Christopher J. Garvey, Martina H. Stenzel
Summary: This article investigates a synthetic pathway to produce biologically compatible, crosslinked, multicompartment worms (MCWs) in aqueous solution by incorporating thermoresponsive poly-N-isopropylacrylamide (PNIPAM) to direct assembly above the lower critical solution temperature (LCST). The self-assembly process and mechanism of MCWs starting from primary micelles were observed and controlled by adjusting the temperature.
Article
Polymer Science
Jordan Thomas Lovegrove, Radhika Raveendran, Patrick Spicer, Stephan Foerster, Christopher J. Garvey, Martina H. Stenzel
Summary: Margination refers to the movement of particles towards the endothelial wall within blood vessels. This study focused on 2D platelet particles as a potential drug delivery system and quantified their margination propensity. The results showed that 2D platelet particles exhibited increased margination compared to spherical particles, with higher margination observed at higher shear rates.
Article
Polymer Science
Dominik M. Schwaiger, Wiebke Lohstroh, Marcell Wolf, Christopher J. Garvey, Peter Mueller-Buschbaum
Summary: Blending PTB7 and PCBM films with binary solvent additive DIO:DPE accelerates the degradation of the films, but the removal of the additives at higher annealing temperature can restore the stability to the level of the pristine blend films, which is promising for photovoltaic applications.
JOURNAL OF POLYMER SCIENCE
(2023)
Article
Nanoscience & Nanotechnology
Tiexin Li, Chandramalika R. Peiris, Albert C. Aragones, Carlos Hurtado, Anthony Kicic, Simone Ciampi, Melanie MacGregor, Tamim Darwish, Nadim Darwish
Summary: In recent years, the hybrid silicon-molecular electronics technology has gained attention for various applications. It has been found that replacing hydrogen with deuterium can significantly enhance the resistance of Si-D surfaces to oxidation and improve their stability in terms of current-voltage characteristics.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Engineering, Environmental
Jingjing Mai, Christopher J. Garvey, Clement Matthew Chan, Steven Pratt, Bronwyn Laycock
Summary: Polyhydroxyalkanoates (PHAs) are attractive alternatives to petroleum-derived plastics, as they are derived from bacteria, thermoprocessible, and truly biodegradable. However, the common short chain length PHAs, such as poly(3-hydroxybutyrate) (P3HB) and poly(3-hydroxybutyrate-co-3-hydroxyvalerate) (PHBV), are relatively stiff and brittle. This study demonstrates the synthesis and characterization of novel high molecular weight PHBV-b-PHBV-b-PHBV block copolymers, which show significantly improved mechanical properties compared to the starting materials. This approach offers an attractive platform for the production of biodegradable PHA materials for various applications.
CHEMICAL ENGINEERING JOURNAL
(2023)
