Article
Polymer Science
Douglas J. Grzetic, Kris T. Delaney, Glenn H. Fredrickson
Summary: Microphase separation in a binary blend of oppositely charged polymers can be stabilized electrostatically, providing a route to control microstructure. The phase behavior is affected by differences in charge density and dielectric constant of the polymers, and specific ordered phases can be stabilized when the minority component has a higher dielectric constant. This system suggests a possible route to large-unit-cell complex-sphere phases.
Article
Polymer Science
Chongrui Zhang, Yinmin Cai, Qiang Zhao
Summary: In this study, a positively charged poly(ionic liquid) with benzene rings in repeating units was designed to form fluidic coacervates when mixed with a like-charge poly(ionic liquid). The effects of polymer concentration, temperature, and ionic strength on the coacervate were investigated, and it was confirmed that the coacervate formation benefited from the cation-pi interaction. This work provides principles and understandings for designing coacervates derived from like-charge poly(ionic liquids) with high charge density.
MACROMOLECULAR RAPID COMMUNICATIONS
(2022)
Article
Engineering, Chemical
Francesco Galiano, Raffaella Mancuso, Lorenzo Guazzelli, Michele Mauri, Cinzia Chiappe, Roberto Simonutti, Adele Brunetti, Christian S. Pomelli, Giuseppe Barbieri, Bartolo Gabriele, Alberto Figoli
Summary: This study developed novel polymeric membranes based on polymerized ionic liquids for CO2 separation, which showed a preference towards CO2 permeation in wet conditions and some membranes exceeded the Robeson upper bound for the CO2/H2 gas pair.
JOURNAL OF MEMBRANE SCIENCE
(2021)
Article
Engineering, Electrical & Electronic
Shuhang Shen, Qiang Liu, Zhongdong Wang
Summary: The experimental study focused on analyzing the spatial characteristics of Mach-cone shaped shockwaves generated by streamers in mineral oil and synthetic ester. The results showed that the appearance of Mach-cone shaped shockwave is an effective indicator of actively propagating streamer channel. Voltage levels did not have a significant impact on the observed shockwave parameters.
IEEE TRANSACTIONS ON DIELECTRICS AND ELECTRICAL INSULATION
(2021)
Article
Materials Science, Multidisciplinary
Wen-Xin Zhang, Yi-Ru Gao, Rong Xue, William Nguyen, Wei Chen, Jian-Hua Wang, Yang Shu
Summary: Ionic liquids have unique properties and great potential in biomedical applications. They can be used in various aspects of liquid formulations to meet specific application scenarios. Recent research has focused on the applications of ionic liquid-based microemulsions, micelles, vesicles, and solvents in the biomedical field.
MATERIALS TODAY PHYSICS
(2023)
Review
Chemistry, Physical
Xiao Tang, Shuyao Lv, Kun Jiang, Guohui Zhou, Xiaomin Liu
Summary: Ionic liquid-based electrolytes have been developed in lithium-ion batteries to enhance safety and performance. This review summarizes the recent progress in the physiochemical properties, interphase formation ability, and electrochemical performance of ionic liquids and ionic liquid-based electrolytes. The applications of different types of ionic liquid-based electrolytes are discussed in detail. The challenges and perspectives for further development of ionic liquid-based electrolytes in lithium-ion batteries are also presented.
JOURNAL OF POWER SOURCES
(2022)
Article
Chemistry, Physical
Tim Peppel, Martin Koeckerling
Summary: A series of new low-melting triply charged homoleptic Cr(III)-based ionic liquids and sixteen new Reineckate related salts with large imidazolium cations are reported. The compounds with [Cr(NCS)(6)](3-) anion have relatively low melting points and are stable up to 200 K above their melting points, while those with [Cr(NCS)(4)L-2](-) anion start to decompose at the melting point.
Article
Multidisciplinary Sciences
Matthew A. Harris, Thomas Kinsey, Durgesh Wagle, Gary A. Baker, Joshua Sangoro
Summary: A liquid-liquid transition (LLT) is a transformation from one liquid to another through a first-order transition, fundamental to understanding the liquid state. While LLT has been reported in some materials, experimental evidence for its existence in many molecular liquids remains controversial. Studying the local order and structural dynamics across an LLT provides unprecedented possibilities for understanding the nature of the liquid state.
PROCEEDINGS OF THE NATIONAL ACADEMY OF SCIENCES OF THE UNITED STATES OF AMERICA
(2021)
Article
Chemistry, Physical
Chao Sun, Yanli Zhang, Yasen Dai, Jiafu Xing, Yajuan Qu, Yinglong Wang, Jun Gao
Summary: Ionic liquids are used as extractants to efficiently and environmentally separate the azeotrope of ethyl acetate and ethanol. Through mechanism analysis, four ILs are selected as extractants and their separation performance is verified through experiments.
JOURNAL OF MOLECULAR LIQUIDS
(2023)
Article
Engineering, Chemical
Julia Sommer, Birgit Bromberger, Christian Robben, Roland Kalb, Peter Rossmanith, Patrick-Julian Mester
Summary: This study investigated the use of ionic liquids for the extraction of viral particles, identifying several liquids with good extraction properties and demonstrating the best results at a neutral pH of 7.5.
SEPARATION AND PURIFICATION TECHNOLOGY
(2021)
Article
Polymer Science
Fan Yang, Meng Zhao, Darren Smith, Peggy Cebe, Sam Lucisano, Thomas Allston, Thomas W. Smith
Summary: This study describes the synthesis, polymerization, and ion exchange of 1-butyl-2,3-dimethyl-4-vinylimidazolium triflate to produce a series of 1-butyl-2,3-dimethyl-4-vinylimidazolium polymers. Regardless of the anion's nature, substitution at the 2-position of the imidazolium moiety significantly increases the distance between the anion and cation.
Article
Polymer Science
David Domingo Huguet, Aitor Gual, Ricard Garcia-Valls, Adrianna Nogalska
Summary: This study demonstrates the potential of improving CO2 capture capabilities by supporting ionic liquids (ILs) on a polymeric matrix. The internal morphology and surface characteristics of the membrane were found to influence the ILs sorption capacity and CO2 solubility.
Article
Chemistry, Applied
Chaoting Deng, Yaping Liu, Donglin Yang, Xiaoyu Cao, Hengjun Gai, Meng Xiao, Tingting Huang, Quanhong Zhu, Hongbing Song
Summary: In this study, the adsorption properties of m-cresol in aqueous phase were regulated by preparing poly(ionic liquid)s (PILs). The PILs showed high adsorption capacity and the adsorption kinetics followed pseudo-second-order kinetics. The adsorption thermodynamics were described well by the Langmuir model. The adsorbent could be separated and recycled, maintaining stable removal efficiency.
MICROPOROUS AND MESOPOROUS MATERIALS
(2023)
Review
Chemistry, Multidisciplinary
Jaemin Min, Dipankar Barpuzary, Hyeonseong Ham, Gyeong-Chan Kang, Moon Jeong Park
Summary: Charged block copolymers with well-ordered structures can effectively control self-assembly and ion diffusion behavior for enhanced ionic conductivity. By tuning the nanostructures and ionic interactions, interconnected ionic channels are promoted to create efficient ion conduction pathways in various morphologies, leading to high-performance materials for next-generation electrochemical devices and soft robotics.
ACCOUNTS OF CHEMICAL RESEARCH
(2021)
Article
Chemistry, Physical
Xumin Wu, Jimin Wu, Jun Gao, Dongmei Xu, Lianzheng Zhang, Yixin Ma, Yinglong Wang
Summary: 2,2-difluoroethanol (DFE) is an important fine chemical in the chemical industry, but its regeneration from aqueous solution is challenging due to the formation of azeotropic mixture with water. This study investigated the use of hydrophobic imidazole-based ionic liquids as extraction agents to regenerate DFE from its aqueous mixture, showing promising results in terms of separating power and interaction energies.
JOURNAL OF MOLECULAR LIQUIDS
(2022)
Review
Chemistry, Physical
Carlos Larriba-Andaluz, James S. Prell
INTERNATIONAL REVIEWS IN PHYSICAL CHEMISTRY
(2020)
Article
Engineering, Chemical
Carlos Larriba-Andaluz, Francesco Carbone
Summary: Electrical Mobility is crucial for the classification of aerosol particles and ions, with the Stokes-Millikan correlation being a widely used analytical expression. However, this correlation has limitations, such as the need for modifications to predict non-spherical entities' mobility. The transition from diffuse to specular reemission in the free molecular regime for smaller ions poses challenges for existing models.
JOURNAL OF AEROSOL SCIENCE
(2021)
Article
Chemistry, Multidisciplinary
Cristian Vicent, Victor Martinez-Agramunt, Viraj Gandhi, Carlos Larriba-Andaluz, Dmitry G. Gusev, Eduardo Peris
Summary: The study investigated the encapsulation of tetracationic palladium metallosquare with four pyrene-bis-imidazolylidene ligands using ESI TWIM-MS and determined Collision Cross Sections (CCS). The host exhibited expansion when fullerenes or polycyclic aromatic hydrocarbons were encapsulated, with expansions ranging from 13 to 49 angstrom(2). DFT calculations were used to obtain energy-minimized structures of the complexes in the gas phase.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2021)
Article
Chemistry, Analytical
Pei Su, Xi Chen, Andrew J. Smith, Michael F. Espenship, Hugo Y. Samayoa Oviedo, Solita M. Wilson, Habib Gholipour-Ranjbar, Carlos Larriba-Andaluz, Julia Laskin
Summary: In this study, an efficient approach to multiplex electrospray ionization sources for applications in analytical and preparative mass spectrometry is reported. By implementing up to four orthogonal injection inlets on the opposite sides of an electrodynamic ion funnel interface, the total ion current transmitted through the mass spectrometer and the signal-to-noise ratio increase significantly. The results demonstrate the potential for proportional increase in ion current with the number of ESI inlets, presenting exciting opportunities for the development of bright ion sources in mass spectrometry applications.
ANALYTICAL CHEMISTRY
(2021)
Article
Chemistry, Analytical
Viraj D. Gandhi, Carlos Larriba-Andaluz
Summary: High-resolution mobility devices such as FAIMS and DMS use strong electric fields to separate ions in the gas phase based on the gas concentration ratio E/N. However, the relation between mobility K and E/N shows non-linear, ion-dependent behavior that is difficult to characterize. By utilizing a two-temperature theory, it is possible to closely follow the K - E/N behavior numerically, and optimizing the Lennard-Jones potentials can improve the accuracy of calculations.
ANALYTICA CHIMICA ACTA
(2021)
Article
Chemistry, Analytical
Christopher P. Harrilal, Viraj D. Gandhi, Gabe Nagy, Xi Chen, Michael G. Buchanan, Roza Wojcik, Christopher R. Conant, Micah T. Donor, Yehia M. Ibrahim, Sandilya V. B. Garimella, Richard D. Smith, Carlos Larriba-Andaluz
Summary: The recent discovery of the ability to separate isotopomers in ultra-high resolution ion mobility spectrometry (IMS) measurements has raised questions about the physical basis for this separation. A study comparing IMS separations for two isotopomer sets, along with theory and simulations accounting for ion rotational effects, has provided the first-ever prediction of rotation-mediated shifts. The simulations show observable mobility shifts due to differences in gas-ion collision frequency and translational-to-rotational energy transfer, providing a new foundation for refining IMS theory and obtaining additional structural insights.
ANALYTICAL CHEMISTRY
(2021)
Article
Physics, Atomic, Molecular & Chemical
Carlos Larriba-Andaluz
Summary: Ion Mobility Spectrometry (IMS) is widely used as an analytical technique, requiring suitable theory to explain observed differences and reliable empirical data to improve existing theory. This study explores useful theoretical approaches and proposes a new labeling system for mobility.
INTERNATIONAL JOURNAL OF MASS SPECTROMETRY
(2021)
Article
Chemistry, Analytical
Xi Chen, Mohsen Latif, Viraj D. Gandhi, Xuemeng Chen, Leyan Hua, Nobuhiko Fukushima, Carlos Larriba-Andaluz
Summary: A linearly decreasing electric field in a varying field drift tube (VFDT) system has been proven to be effective for correcting ions' diffusion and improving resolving power. However, the theoretical predictions of resolving power were higher than the experimental observations. The discrepancy was identified as the difference between spatial resolving power (theoretical) and time resolving power (experimental). To match the high spatial resolving power observed experimentally, a secondary high voltage pulse (HVP) was used to increase ions' drift velocity and time-resolving power. Numerical simulations and experimental tests were conducted to support the theoretical findings. The HVP-VFDT atmospheric pressure portable system achieved unprecedented resolving power of 250 in just 21 cm length and 7 kV voltage.
ANALYTICAL CHEMISTRY
(2022)
Article
Biochemical Research Methods
Mohsen Latif, Xi Chen, Viraj D. Gandhi, Carlos Larriba-Andaluz, Gerardo Gamez
Summary: In this work, a field-switching technique combined with a flowing atmospheric pressure afterglow source was used to enhance drift tube ion mobility spectrometry. By substituting the Bradbury-Nielsen gate with a tip-repeller electrode, the performance of the ion mobility spectra was optimized and the limit of detection was significantly improved. Various operating conditions were optimized and compared with literature results.
JOURNAL OF THE AMERICAN SOCIETY FOR MASS SPECTROMETRY
(2022)
Article
Chemistry, Physical
Xi Chen, G. Asher Newsome, Michael Buchanan, Jeremy Glasper, Leyan Hua, Mohsen Latif, Viraj Gandhi, Xintong Li, Carlos Larriba-Andaluz
Summary: Thermal gas jet probes, a type of sampling technique in ambient mass spectrometry, have not been studied using computational fluid dynamics (CFD) models. In this study, two systems were constructed: a heated nitrogen jet probe and a CFD model. The results showed that the transmission efficiency of desorbed particles was less than 10% in the tested physical model, but improved when the system was close to the sample surface. The use of a baffle to increase pressure in the sample region led to a transmission efficiency of almost 100% according to a Lagrangian particle tracking approach.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Article
Chemistry, Analytical
Viraj D. Gandhi, Jihyeon Lee, Leyan Hua, Mohsen Latif, Christopher J. Hogan, Carlos Larriba-Andaluz
Summary: To improve ion separation techniques, a differential mobility analyzer (DMA) has been combined with field asymmetric waveform ion mobility spectrometry (FAIMS). The DMA's filtering effect allows for individual ion selection based on low-field mobility, and these ions can then be studied in FAIMS at different electric field strengths to achieve two-dimensional mobility separations. Comparisons with theoretical predictions show excellent results, although deviations occur beyond 100 Td due to ion heating and collisions with the nitrogen gas. A newly developed implicit equation is used to predict dispersion plots, overcoming issues associated with the more complex Buryakov equation. The results demonstrate that the DMA-FAIMS coupling provides comprehensive information on ion mobility and can predict spectra based on ion structures and gas properties.
ANALYTICAL CHEMISTRY
(2023)
Article
Engineering, Chemical
Viraj D. Gandhi, Kyle Short, Leyan Hua, Ivan Rodriguez, Carlos Larriba-Andaluz
Summary: In an effort to calculate electrical mobilities in the free molecular regime using non-negligible electrical fields, researchers have developed and tested an algorithm based on collision integrals and the two-temperature theory. The algorithm calculates mobility based on the ion's effective temperature using a 4-6-12 potential interaction, with or without an ion-quadrupole potential in the case of nitrogen gas. The algorithm has been successfully parallelized and tested against experimental results for small ions in light gases, as well as mid-sized analytes in nitrogen at room temperature and 100K.
JOURNAL OF AEROSOL SCIENCE
(2023)
Article
Chemistry, Physical
Christopher P. Harrilal, Sandilya V. B. Garimella, Jaehun Chun, Nikhil Devanathan, Xueyun Zheng, Yehia M. Ibrahim, Carlos Larriba-Andaluz, Gregory Schenter, Richard D. Smith
Summary: The role of ion rotation in determining ion mobilities is explored using ion mobility spectrometry (IMS) measurements of isotopomer ions. Differences in ion mass distributions between isotopomer ions result in subtle ion mobility shifts which can be measured with high precision. The study investigates the rotational dependence of ion mobility shifts and finds that differences in rotational energy transfer during ion-molecule collisions contribute significantly to the separation of isotopomer ions. These findings demonstrate the potential of combining high-resolution IMS measurements with theory and computation for studying subtle structural differences between ions.
JOURNAL OF PHYSICAL CHEMISTRY A
(2023)
Review
Chemistry, Analytical
Viraj D. Gandhi, Leyan Hua, Xuemeng Chen, Mohsen Latif, Carlos Larriba-Andaluz
Summary: Ion mobility has become a widely used tool in Analytical Chemistry for separating compounds in the gas phase. This manuscript aims to explain the physics of ion-gas collisions at high fields using the two-temperature approximation. It provides a concise description and rigorous mathematical arguments to predict the ion's drift velocity, as well as a detailed procedure for obtaining higher-order mobility approximations. The comparison between different models and experimental results shows good agreement and convergence.
Correction
Chemistry, Physical
Carlos Larriba-Andaluz, James S. Prell
INTERNATIONAL REVIEWS IN PHYSICAL CHEMISTRY
(2021)