Article
Polymer Science
Andrew Selkirk, Nadezda Prochukhan, Ross Lundy, Cian Cummins, Riley Gatensby, Rachel Kilbride, Andrew Parnell, Jhonattan Baez Vasquez, Michael Morris, Parvaneh Mokarian-Tabari
Summary: This study overcomes the kinetic challenges in the self-assembly of UHMW BCPs through precision solvent annealing, resulting in highly ordered large-period lamellar domains. The research reveals that film thickness and solvent concentration significantly affect the domain morphology.
Article
Chemistry, Multidisciplinary
Yi Wang, Jun Chen, Chenhui Zhu, Baixu Zhu, Soojin Jeong, Yi Yi, Yang Liu, Joshua Fiadorwu, Peng He, Xingchen Ye
Summary: Polymer-inorganic nanocomposites based on polymer-grafted nanocrystals (PGNCs) are being used in technologically relevant applications due to their unique physical, chemical, and mechanical properties. This study demonstrates a kinetically controlled assembly of binary superstructures from a homogeneous disordered PGNC mixture using solvent vapor annealing (SVA), providing insight into the multistep crystallization pathway of PGNCs. By varying the solvent vapor pressure during SVA, exquisite control of the rate and extent of PGNC assembly is achieved, allowing for the synthesis of multicomponent PGNC superstructures with multifunctionalities and emergent properties.
Article
Chemistry, Physical
Hong Zhao, Le Wang, Yufei Wang, Wenyan Su, Dongxu Lin, Wanzhu Cai, Jian Qing, Zibang Zhang, Jingang Zhong, Lintao Hou
Summary: The simplified one-step spraying of OSCs can be achieved successfully with the assistance of solvent vapor annealing (SVA), making it attractive for future photovoltaic module manufacturing while maintaining high photovoltaic performance. The sprayed self-assembly interfacial molecules can enhance charge separation and transport capability, comparable to conventional two-step spraying OSCs.
ACS APPLIED ENERGY MATERIALS
(2021)
Article
Nanoscience & Nanotechnology
Jing Zhou, Vikram Thapar, Yu Chen, Bi-Xian Wu, Gordon S. W. Craig, Paul F. Nealey, Su-Mi Hur, Tzu-Hsuan Chang, Shisheng Xiong
Summary: The study investigates the self-aligned assembly of a triblock copolymer on neutral graphene nanoribbons through solvent vapor annealing, showing long-range ordered alignment and overcoming the lithography resolution restriction required for traditional DSA.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Polymer Science
Iulia Babutan, Otto Todor-Boer, Leonard Ionut Atanase, Adriana Vulpoi, Ioan Botiz
Summary: In this study, we utilized solvent vapor annealing as a polymer processing method to condense a large amount of solvent vapors onto thin films of block copolymers, promoting their self-assembly into ordered nanostructures. Atomic force microscopy revealed the successful generation of a periodic lamellar morphology of poly(2-vinylpyridine)-b-polybutadiene and an ordered morphology comprised of hexagonally-packed structures made of poly(2-vinylpyridine)-b-poly(cyclohexyl methacrylate) on solid substrates.
Article
Nanoscience & Nanotechnology
Gayashani Ginige, Youngdong Song, Brian C. Olsen, Erik J. Luber, Cafer T. Yavuz, Jillian M. Buriak
Summary: Self-assembly of block copolymers promises high resolution and density multiplication with lower costs. However, the defectivity of resulting nanopatterns remains high due to small variations of processing parameters. A solvent vapor annealing (SVA) flow-controlled system combined with design of experiments (DOE) and machine learning (ML) approaches enables precise optimization of self-assembly conditions and characterization of defects, leading to a faster route toward low-defectivity BCP dot arrays for electronic microfabrication.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Article
Chemistry, Multidisciplinary
Hongjun Jin, Ziyan Wu, Weilin Lin, Yinye Chen, Jingran Zhang, Ruyi Zheng, Haibing Wei, Qinghua Chen, Qingrong Qian, Jianbin Huang, Jie Zhang, Yun Yan
Summary: In this study, size-controllable tetragonal nanoprisms were formed through crystallization-directed ionic self-assembly (CDISA) by evaporating a micellar solution on solid substrates. The length and width of the nanoprisms can be easily tuned by varying the initial concentration. This precise size-control strategy is expected to provide new possibilities for designing advanced materials with size-controllable anisotropic nanostructures.
Article
Polymer Science
Athmen Zenati, Ashish Pokhrel
Summary: Two sets of liquid crystalline diblock copolymers (DBCs) and triblock copolymers (TBCs) composed of hard and soft blocks were prepared with high control over their molecular masses, dispersities (M-w/M-n = D <= 1.38), and compositions using reversible addition-fragmentation chain transfer polymerization. The structures and properties of the block copolymers were characterized using various techniques, and their morphologies in a mixed solvent system varied depending on the volume fractions of the blocks and the solvent interactions.
JOURNAL OF POLYMER SCIENCE
(2023)
Article
Polymer Science
Melisa Trejo-Maldonado, Aisha Womiloju, Steffi Stumpf, Stephanie Hoeppener, Ulrich S. Schubert, Luis E. Elizalde, Carlos Guerrero-Sanchez
Summary: This study reports the synthesis of poly(styrene-block-lactic acid) copolymers with triazole rings as a junction between blocks. The self-assembly behavior and morphological changes induced by different techniques were observed. The synthetic approach showed effectiveness in obtaining copolymer structures with specific self-assembly properties.
Article
Polymer Science
Shuwen Cheng, Yu Hu, Xuanhong Wu, Wei Li, Jingshan Mu
Summary: A series of different shaped semi-crystalline triblock copolymers were prepared and studied for their self-assembly behavior during solvent vapor annealing. The dumbbell-shaped polymer showed plasticization effects on the PE midblock, affecting chain folding and reducing crystallinity. The hierarchical self-assembly process was influenced by both PE crystallization and copolymer topological structures.
MACROMOLECULAR CHEMISTRY AND PHYSICS
(2021)
Article
Materials Science, Multidisciplinary
Sajan Singh, Tandra Ghoshal, Nadezda Prochukhan, Alberto Alvarez Fernandez, Jhonattan Frank Baez Vasquez, Pravind Yadav, Sibu C. Padmanabhan, Michael A. Morris
Summary: In this study, we demonstrated the formation of oxide porous and nanodot structures from the same block copolymer (BCP) through the phase inversion of a BCP template. The effect of solvent annealing time on the ordering of the BCP was investigated. Metal ions were infiltrated into the BCP templates and oxidized to their oxides. The resulting structures were analyzed through various methods, confirming the complete elimination of the BCP template and the presence of metal oxides.
ACS APPLIED POLYMER MATERIALS
(2023)
Article
Chemistry, Physical
Tae-Yi Kim, Su-Mi Hur, Abelardo Ramirez-Hernandez
Summary: This study used dissipative particle dynamics to investigate the solution self-assembly of symmetric ABCBA linear pentablock polymers in a selective solvent and examined the effect of block sequence, composition, and polymer concentration on the final morphology and polymer conformations. The results confirmed that block sequence affects the self-assembled morphology and has a strong influence on polymer conformations, leading to the formation of physical gels for the sequence where the solvophilic block is located in the middle of the macromolecule. Our findings are summarized in morphology diagrams in the composition concentration parameter space.
JOURNAL OF PHYSICAL CHEMISTRY B
(2023)
Article
Polymer Science
Ling-Ying Shi, Zhixiong Fei, Qian Wang, Lin Weng, Chenxiao Yin, Jinrui Sun, Zhihao Shen
Summary: Bottlebrush block copolymers (BBCPs) are intriguing architectural polymers that can produce various anisotropic nanostructures. This study presents a method for creating ordered silicon oxide patterns and particles on substrates using solvent vapor induced thin film self-assembly of BBCPs containing polydimethylsiloxane (PDMS) and polystyrene (PS) side chains. Different morphologies, including cylindrical or stripes-like, spherical, and ordered porous structures, as well as Janus particle-like structures, were achieved through solvent vapor annealing. The Janus particle-like structures were further transformed into meso-to-macroporous silicon oxide bowls after oxygen plasma etching. The study also discussed the effects of solvent vapor and backbone length on the self-assembly behavior of the thin film.
Article
Engineering, Environmental
Ming Zhu, Tao Yang, Liting Wang, Mengyuan Xiong, Wenjun He, Yaowei Chen, Weili Deng, Xiaoyan Li
Summary: This study presents a superstretchable fiber membrane with good electromechanical performance, stable electrical conductivity, and underwater working capability. The membrane shows promising potential in the field of human motion monitoring.
CHEMICAL ENGINEERING JOURNAL
(2022)
Article
Nanoscience & Nanotechnology
Kshitij Sharma, Aman Agrawal, Ali Masud, Sushil K. Satija, John F. Ankner, Jack F. Douglas, Alamgir Karim
Summary: The kinetics and morphology of block copolymer films are influenced by the processing pathway, which affects the enthalpic and entropic forces driving the ordering processes. Understanding the free energy landscape and how processing procedures can move the system through this landscape is important for controlling the variability of block copolymer morphology. The authors demonstrate a method where a target low-energy structure can be quickly achieved by subjecting as-cast films to initial solvent annealing followed by a short period of thermal annealing.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Electrochemistry
Varada Menon Palakkal, Matthew L. Jordan, Deepra Bhattacharya, Yupo J. Lin, Christopher G. Arges
Summary: In this study, ionomer coated nylon mesh nets were used to address spacer channel resistances in MCDI, resulting in lower cell voltage rise during deionization, improved energy recovery, and increased energy normalized adsorbed salt values. This allowed for an increase in current density without exceeding the upper bound set for mitigating parasitic reactions, potentially reducing the capital costs of MCDI units.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
Deepra Bhattacharya, Subarna Kole, Orhan Kizilkaya, Joseph Strzalka, Polyxeni P. Angelopoulou, Georgios Sakellariou, Dongmei Cao, Christopher G. Arges
Summary: This study reports the use of self-assembled block copolymers as templates for fabricating nanostructured platinum and iridium oxide electrocatalysts, with experiments showing that electrocatalysts prepared from alkylated block copolymer templates exhibit higher mass activities. Evaluations conducted in the study demonstrate that the mesostructure of nanostructured electrocatalysts has a significant impact on reactivity.
Article
Chemistry, Multidisciplinary
Sushant P. Sahu, Subarna Kole, Christopher G. Arges, Manas Ranjan Gartia
Summary: This study reports an electrochemical sensor with a selective perfluorinated anion exchange ionomer (PFAEI) coating for direct sensing of a type of PFAS called perfluorooctanoic acid (PFOA). The sensor operates without redox probes and has a low detection limit.
Article
Engineering, Chemical
Luis A. Briceno-Mena, Jose A. Romagnoli, Christopher G. Arges
Summary: This study combines knowledge-based modeling and data-driven modeling to improve the accuracy of performance prediction for high-temperature electrochemical systems by implementing a few-shot learning approach. The knowledge-based model generates simulated data and is pre-trained, then target models are trained using experimental datasets, achieving high accuracy in predicting unseen data.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2022)
Article
Electrochemistry
Matthew L. Jordan, Tanmay Kulkarni, Dodangodage Ishara Senadheera, Revati Kumar, Yupo J. Lin, Christopher G. Arges
Summary: This study investigates the use of tethered benzyl 1-methyl imidazolium cations in polysulfone anion exchange membranes (AEMs) for ionic separations. The results demonstrate that these alternative cation moieties significantly enhance lactate conductivity and anion flux compared to traditional quaternary benzyl ammonium AEMs. Molecular dynamics and NMR experiments suggest that the closer binding of lactate anions to the imidazolium cations is responsible for the improved flux values.
JOURNAL OF THE ELECTROCHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Gokul Venugopalan, Deepra Bhattacharya, Evan Andrews, Luis Briceno-Mena, Jose Romagnoli, John Flake, Christopher G. Arges
Summary: In this study, a high-temperature PEM EHP demonstrated successful purification of hydrogen from gas mixtures with high CO content, achieving high recovery rates and minimal performance loss. This presents a possibility for a simplified hydrogen separation and compression technology.
ACS ENERGY LETTERS
(2022)
Editorial Material
Electrochemistry
Christopher G. Arges
ELECTROCHEMICAL SOCIETY INTERFACE
(2022)
Article
Chemistry, Multidisciplinary
Matthew L. Jordan, Grzegorz Kokoszka, Hishara Keshani Gallage Dona, Dodangodage Ishara Senadheera, Revati Kumar, Yupo J. Lin, Christopher G. Arges
Summary: In this study, a new membrane wafer assembly (MWA) was developed for the separation of p-coumaric acid in electrodeionization (EDI) process. The MWA showed improved capture efficiency for p-coumaric acid and reduced energy consumption and cost.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2023)
Article
Engineering, Chemical
Hishara Keshani Gallage Dona, Teslim Olayiwola, Luis A. Briceno-Mena, Christopher G. Arges, Revati Kumar, Jose A. Romagnoli
Summary: This study establishes a framework that combines molecular dynamics and machine learning to predict the activity coefficients of ions in ion-exchange membranes. By using small-scale experimental data, polymer structure information, and molecular attributes describing the solvation of ions and polymers, two machine learning models were developed to estimate the molecular attributes and ion activity coefficients. The best model achieved an average mean absolute error of less than 7% for solvation descriptors and 10% for ion activity coefficients. This approach allows for the estimation of ion activity coefficients in ion-exchange membranes without the need for time-consuming molecular dynamics simulations and experiments.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2023)
Article
Engineering, Environmental
Tanmay Kulkarni, Aliya Muhammad Al Dhamen, Deepra Bhattacharya, Christopher G. G. Arges
Summary: This study introduces the selective ionic separation method based on bipolar membrane (BPM) capacitive deionization. By utilizing Pourbaix diagrams and acid-base equilibrium principles, selective separations of multicomponent ionic species mixtures were achieved. The study found that the location of the BPM in the electrochemical cell determines whether alkaline or acidic process streams are generated. The effects of cell voltage, residence time, and feed concentration on effluent stream pH were investigated. The BPM-MCDI showed significantly higher removal percentages for copper ions compared to sodium ions from brine mixtures, and also showed improved removal rates for copper ions and itaconic acid from brine mixtures compared to a traditional flow-by-MCDI setup.
ACS ES&T ENGINEERING
(2023)
Editorial Material
Electrochemistry
Christopher G. Arges, Darrell Velegol, Matthew L. Jordan
Summary: This article disseminates the experience of teaching senior chemical engineering students the core principles of electrochemical engineering in a single class period for designing an electrolytic caustic soda process. It discusses how key concepts in chemical engineering are related to electrochemical engineering principles and explores alternative process designs for caustic soda production.
ELECTROCHEMICAL SOCIETY INTERFACE
(2023)
Article
Chemistry, Multidisciplinary
Deepra Bhattacharya, Ke Wang, Guang-Peng Wu, Christopher Arges
Summary: Reducing platinum-group metal (PGM) loadings in fuel cells and electrolyzers is essential for cost reductions and the scale-up of hydrogen for decarbonization. This study reports the development of binder-free thin-film platinum electrocatalysts with tunable nanoscale morphology and periodic spacing. The electrocatalysts exhibit high performance and stability, surpassing commercial catalysts, and the use of block copolymer (BCP) templating allows for the fabrication of stable and tunable catalyst geometries.
Article
Materials Science, Multidisciplinary
Mario. V. V. Ramos-Garces, Dodangodage Ishara Senadheera, Karthik Arunagiri, Polyxeni. P. P. Angelopoulou, Georgios Sakellariou, Ke Li, Bryan. D. D. Vogt, Revati Kumar, Christopher. G. G. Arges
Summary: Ion-exchange membranes (IEMs) are widely used in various applications in electrochemical systems. The chemical composition and macromolecular architecture of ion-conducting polymers play a crucial role in ion and water transport. This study focuses on the preparation of different microphase separated block copolymer electrolytes (BCEs) with distinct side chain chemistries. The results show that the more hydrophobic alkyl side chains exhibit significantly higher ionic conductivity compared to alkoxy and zwitterionic side chains.
MATERIALS ADVANCES
(2023)
Article
Computer Science, Artificial Intelligence
Luis A. Briceno-Mena, Gokul Venugopalan, Jose A. Romagnoli, Christopher G. Arges
Summary: High-temperature polymer electrolyte membrane fuel cells (HT-PEMFCs) are a promising energy conversion technology using low-cost hydrogen from methane, but require improvement in power density. Machine Learning tools have been shown to efficiently explore large search spaces and guide activities to enhance HT-PEMFC power density. Support vector regression analysis and data analysis frameworks were used to analyze existing datasets and generate insights to achieve power density above 1 W cm(-2) in HT-PEMFCs.
Article
Materials Science, Multidisciplinary
Gokul Venugopalan, Deepra Bhattacharya, Subarna Kole, Cameron Ysidron, Polyxeni P. Angelopoulou, Georgios Sakellariou, Christopher G. Arges
Summary: Ionomer electrode binders are crucial for PEM fuel cells and electrolyzers, impacting cell performance significantly. The use of two different types of high-temperature ionomers as thin films on IDE platforms with nanoscale platinum electrocatalysts showed comparable reaction kinetics to electrochemical hydrogen pumps. The application of these ionomers in membrane electrode assemblies demonstrated promising results for HT-PEM electrochemical hydrogen pumps.
MATERIALS ADVANCES
(2021)
