Article
Chemistry, Multidisciplinary
Mizhi Xu, McKinley K. Paul, Krista K. Bullard, Christopher DuPre, Will R. Gutekunst
Summary: This study demonstrates that the geometry and reactivity of twisted amide scaffolds can be significantly modulated by remote substituent effects. The electron-donating ability of the substituent shows a strong positive correlation with the distortion of the amide bond, impacting the rates of nucleophilic substitution. The nature of the substituent determines the rate-limiting step of the cascade sequence, while solvent polarity and halide ion also play a role in reaction pathway and efficiency.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Polymer Science
Devavrat Sathe, Hanlin Chen, Junpeng Wang
Summary: By investigating the effects of different substituents on cyclobutane on the polymers, this study reveals their impact on polymerization conversion and thermal properties. These findings are important for designing the next generation of chemically recyclable polymers.
MACROMOLECULAR RAPID COMMUNICATIONS
(2023)
Article
Multidisciplinary Sciences
Mohamed Barakat Zakaria Hegazy, Karim Harrath, David Tetzlaff, Mathias Smialkowski, Daniel Siegmund, Jun Li, Rui Cao, Ulf -Peter Apfel
Summary: In this study, the synthesis of heterotrimetallic pentlandite-type material Fe3Co3Ni3S8 (FCNS) in the presence of suitable phosphorus and nitrogen donors for electrochemical water splitting was reported. The preferential incorporation of N into the FCNS lattice was observed, while the addition of phosphorus led to metal-phosphate-FCNS composites. The doped FCNS materials showed improved performance in oxygen evolution reaction (OER) and hydrogen evolution reaction (HER) compared to the pristine FCNS.
Article
Polymer Science
Fengbiao Chen, Fei Gao, Xinru Guo, Liang Shen, Yangju Lin
Summary: This study demonstrates the fabrication of enamine-one vitrimers through an amino-yne click reaction using secondary amine substrates, and shows that the activation energy of the exchange reaction and the properties of the vitrimer networks can be tuned by modulating the substituents of the secondary amine. Interestingly, piperidine exhibits reactivities comparable to that of primary amines. This research enriches the scope of amine substrates for vitrimer fabrication and provides a convenient means to tune the network dynamics.
Article
Nanoscience & Nanotechnology
Ita Rahmawati, Indriyati, Fitri A. Permatasari, Muhammad A. Irham, Mohamad I. Nugraha, Thomas D. Anthopoulos, Ferry Iskandar
Summary: Carbon dots (CDs) are a new family of carbon nanomaterials that show potential for solar water evaporation due to their cost-effectiveness, non-toxicity, high solubility, and tunable optical properties. However, CDs mainly absorb ultraviolet light, limiting their functionality in generating steam from solar energy. In this study, we demonstrate that the optical and photothermal properties of CDs can be controlled by varying their surface stoichiometry through adjusting precursor molar ratios. Using CDs as photothermal materials in a solar evaporator, we achieve a remarkable evaporation efficiency and rate, along with excellent durability and stability.
ACS APPLIED NANO MATERIALS
(2023)
Article
Chemistry, Physical
Rui Dong, Anquan Zhu, Pengfei Tan, Yong Liu, Min Jiang, Lu Yang, Jianping Xie, Jun Pan
Summary: This study successfully synthesized oxygen-doped cobalt phosphide arrays with efficient bifunctional catalytic active sites, achieved by adjusting the P/O atomic ratio through controlling the phosphating time to affect the electronic environment of cobalt active sites, leading to excellent electrocatalytic water decomposition performance.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2022)
Article
Polymer Science
Marcel G. Martins, Thamiris F. Paiva, Juliana S. Goulart, Claudio R. A. Abreu, Priscilla Finotelli, Helen C. Ferraz
Summary: In this study, curcumin was incorporated into a polymer matrix via bulk polymerization to enhance its photostability. The extraction of curcumin from turmeric extract using the precursor monomer MMA was found to reduce degradation of the fluorescent species during polymerization. The addition of AA as a comonomer further improved the photochemical stability and promoted the bathochromic effect of the turmeric extract.
Article
Polymer Science
Yuanhao Zhong, Baoli Wang, Dongmei Cui
Summary: This study demonstrates the successful coordination terpolymerization of polar ortho-alkoxystyrene (oAOS), isoprene (IP), and butadiene (BD), showing the ability to tune the concentration of monomers in the resulting polymers by changing the feed ratios. This results in varying microstructures of the poly(oAOS-IP-BD) copolymers.
Article
Chemistry, Multidisciplinary
Kang Li, Jia-Min Hu, Wei-Min Qin, Jing Guo, Yue-Peng Cai
Summary: This study demonstrates a method of transforming hydrophobic molecular scaffolds into hydrophilic ones, enhancing solubility and facilitating self-assembly by N/O heteroatom doping. The Hansen solubility parameters and hydrogen bonding solubility parameter provide evidence of the influence of N/O doping species and positions on the solubility.
COMMUNICATIONS CHEMISTRY
(2022)
Article
Polymer Science
Saeid Tajbakhsh, Faezeh Hajiali, Milan Maric
Summary: The study focused on nitroxide mediated polymerization of methacryloisobutyl POSS (POSSMA) and bio-sourced monomers, achieving high molecular weight polymers with high efficiency. The addition of POSSMA was shown to enhance the thermal stability of bio-based polymers, indicating significant potential for practical applications.
JOURNAL OF APPLIED POLYMER SCIENCE
(2021)
Article
Polymer Science
Yi Zhang, Hua Lu
Summary: Ring-opening copolymerization is an important method to combine the properties of different monomers and adjust polymer properties. However, the copolymerization of two different monomers with full recyclability is rare. In this study, we successfully copolymerized rigid 4-hydroxyproline-derived thiolactone with various lipoic acid derivatives with flexible backbones to prepare poly(thioester-co-disulfide) copolymers with tunable thermal and mechanical properties. The resulting copolymers can be depolymerized to high monomer yields for full recycling. This research provides a detailed understanding of the kinetics and controllability of the thiolactone and 1,2-dithiolane copolymerization system, which may contribute to the design, modification, and strengthening of new recyclable polymer materials in the future.
Article
Polymer Science
Yongfei Zhu, Peilin Li, Runsheng Lin, Junming Su
Summary: By introducing PG-FA and PG-A as catalysts, the ROP temperature of P-DDM can be decreased, while the thermal stability of PP-DDM can be enhanced. This is mainly manifested by an increase in the total amount of hydrogen bonds and a decrease in the proportion of specific hydrogen bonds.
Article
Polymer Science
Marco Paolino, Mario Saletti, Annalisa Reale, Vincenzo Razzano, Germano Giuliani, Alessandro Donati, Claudia Bonechi, Gianluca Giorgi, Giuseppa Mercorillo, Filippo Samperi, Wojciech Mroz, Chiara Botta, Andrea Cappelli
Summary: Two benzofulvene derivatives with a 4-pyridylacetylene substituent in different positions (2 and 6) were synthesized and found to spontaneously polymerize in the absence of catalysts or initiators. NMR and MALDI-TOF studies confirmed the polymeric nature of the materials and revealed that the derivative with the substituent in position 6 exhibited higher structural homogeneity compared to the one with the substituent in position 2. The most homogeneous polybenzofulvene derivative demonstrated outstanding hole mobility, making it a promising material for FET device applications.
EUROPEAN POLYMER JOURNAL
(2023)
Article
Chemistry, Multidisciplinary
Han Wang, Gaojie Yan, Mengke Li, Haifeng Ji, Yi Feng, Jingjing Shi, Xiaojie Zhang
Summary: This study developed a simple quasi-click reaction to synthesize a sulfhydryl polymer for coating carbon nanotubes as a cathode material in lithium-sulfur batteries. The experimental results demonstrated that the sulfhydryl polymer effectively inhibits the shuttle effect and improves the capacity retention and cycle stability of the batteries.
ACS SUSTAINABLE CHEMISTRY & ENGINEERING
(2022)
Article
Biochemistry & Molecular Biology
Ruonan Sun, Junxiang Zhu, Hao Wu, Shiqing Wang, Wenxiang Li, Qingjie Sun
Summary: By adjusting the surface charge density of TOCNs, the properties and stability of the film can be improved. The TOCNs in sodium alginate/chitosan multilayer film form a compact and uniform interlayer structure through strong electrostatic interactions and hydrogen bonding. The addition of TOCNs can also enhance the mechanical properties, thermal stability, hydrophobicity, and barrier properties of the multilayer film.
INTERNATIONAL JOURNAL OF BIOLOGICAL MACROMOLECULES
(2021)
Article
Nanoscience & Nanotechnology
Shunrui Luo, Kostiantyn Turcheniuk, Lihua Chen, Ah-Young Song, Wenqiang Hu, Xiaolei Ren, Zifei Sun, Rampi Ramprasad, Gleb Yushin
Summary: We report a new synthesis pathway for Mg n-propoxide nanowires from Mg ethoxide nanoparticles. The morphology transformation from nanoparticles to nanowires was studied using characterization techniques such as SEM, FTIR, and NMR spectroscopy. The ligand exchange and increased fraction of OH groups greatly enhanced Mg alkoxide bonding and facilitated the formation and growth of the Mg n-propoxide nanowires.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Physical
R. Datta, R. Ramprasad, S. Venkatram
Summary: This study utilizes a deep neural network to rapidly and accurately predict the conductivity of ionic liquids (ILs) and identifies key chemical structural characteristics that correlate with the ionic conductivity. The findings provide guidance for the design and synthesis of new highly conductive ILs.
JOURNAL OF CHEMICAL PHYSICS
(2022)
Article
Chemistry, Physical
Harikrishna Sahu, Kuan-Hsuan Shen, Joseph H. Montoya, Huan Tran, Rampi Ramprasad
Summary: Researchers have developed a Python toolkit called PSP for generating polymer models based on SMILES strings. Users can adjust parameters to manage the quality and scale of models, with output structures and forcefield parameter files available for downstream simulations. The PSP package also includes a Colab notebook for user interaction and learning.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2022)
Article
Chemistry, Physical
Huan Tran, Aubrey Toland, Kellie Stellmach, McKinley K. Paul, Will Gutekunst, Rampi Ramprasad
Summary: This study developed a first-principles computational scheme for accurately calculating the enthalpy of ring-opening polymerization (Delta H-ROP). The scheme demonstrated a smaller root-mean-square error compared to conventional approaches when validated on a diverse benchmark set. This development opens up new pathways for building a high-quality database of Delta H-ROP and accelerating the design of depolymerizable polymers.
JOURNAL OF PHYSICAL CHEMISTRY LETTERS
(2022)
Article
Engineering, Chemical
Shubham Jamdade, Rishi Gurnani, Hanjun Fang, Salah Eddine Boulfelfel, Rampi Ramprasad, David S. Sholl
Summary: We developed a computational approach to screen MOFs for oxygen-helium separation at low temperatures. Through molecular simulations and stability evaluation, we identified high-performance materials for this separation process. This method can also be applied to selecting adsorbents for other gas separations.
INDUSTRIAL & ENGINEERING CHEMISTRY RESEARCH
(2023)
Article
Chemistry, Physical
Huan Tran, Kuan-Hsuan Shen, Shivank Shukla, Ha-Kyung Kwon, Rampi Ramprasad
Summary: Modern fuel cell technologies use Nafion for proton-exchange membrane and as the binding material for the catalyst layers. This study proposes an informatics-based scheme to search large polymer chemical spaces and identifies 60 new polymer candidates for various applications in fuel cells.
JOURNAL OF PHYSICAL CHEMISTRY C
(2023)
Article
Chemistry, Physical
Rishi Gurnani, Christopher Kuenneth, Aubrey Toland, Rampi Ramprasad
Summary: Artificial intelligence-based methods are effective in screening polymer libraries for experimental inquiry. Our approach uses machine learning to extract important features from polymer repeat units, speeding up feature extraction by 1-2 orders of magnitude without compromising model accuracy. This approach will enable more sophisticated and large-scale screening technologies in polymer informatics.
CHEMISTRY OF MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Yong-Liang Su, Liang Yue, Huan Tran, Mizhi Xu, Anthony Engler, Rampi Ramprasad, H. Jerry Qi, Will R. R. Gutekunst
Summary: In this study, a chemically recyclable polythioether system based on nucleophilic aromatic substitution (SNAr) was developed. The system demonstrated chain-growth ring-opening polymerization through SNAr reactions, with fast reaction rates and efficient polymerization and depolymerization cycles. The resulting polythioether materials showed comparable performance to commercial thermoplastics, and could be depolymerized to the original monomers in high yields.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Physical
Pranav Shetty, Arunkumar Chitteth Rajan, Chris Kuenneth, Sonakshi Gupta, Lakshmi Prerana Panchumarti, Lauren Holm, Chao Zhang, Rampi Ramprasad
Summary: This study used natural language processing methods to extract material property data from polymer literature abstracts. By training the MaterialsBERT language model, we obtained around 300,000 material property records for analysis in various applications such as fuel cells, supercapacitors, and polymer solar cells.
NPJ COMPUTATIONAL MATERIALS
(2023)
Article
Materials Science, Multidisciplinary
Huan Tran, Tuoc N. Vu
Summary: First-principles computations have been instrumental in discovering hydride-based superconductors, especially under high pressures, in the last decade. Machine-learning (ML) approaches show promise in further accelerating future discoveries if their reliability can be improved. This paper demonstrates the sustainable and reliable prediction of superconductivity at any pressure from atomic structures. ML models were trained to predict electron-phonon interaction parameters, from which the critical temperature Tc can be computed. Two possible superconductors with Tc close to 10-15 K at zero pressure were identified, and it was found that they have been previously synthesized and studied. In summary, this ML approach enables the direct transfer of knowledge from high-pressure atomic-level details to zero pressure, contributing to the discovery of new superconductors.
PHYSICAL REVIEW MATERIALS
(2023)
Review
Materials Science, Multidisciplinary
Janhavi Nistane, Lihua Chen, Youngjoo Lee, Ryan Lively, Rampi Ramprasad
Summary: This study presents a machine learning model that can instantly predict the temperature-dependent Flory-Huggins interaction parameter for polymer-solvent mixtures. The model has been trained using a large dataset of experimental data and demonstrates high accuracy and generality.
MRS COMMUNICATIONS
(2022)
Article
Chemistry, Multidisciplinary
Abdullah Alamri, Chao Wu, Shamima Nasreen, Huan Tran, Omer Yassin, Ryan Gentile, Deepak Kamal, Rampi Ramprasad, Yang Cao, Gregory Sotzing
Summary: Polymer dielectrics with ultra-high charge-discharge rates are significant for advanced electrical and electronic systems. Incorporating metal into the polymer matrix can improve the dielectric constant while maintaining high breakdown strength.
