Article
Polymer Science
David R. O. Hewitt, Robert B. Grubbs
Summary: Polymerization of ethyl glyoxylate can be initiated from alcohols or thiols by activation with triethylamine, resulting in poly(ethyl glyoxylate) with controllable molecular weights and relatively low dispersities. Stabilization against depolymerization by chain-capping with benzyl chloroformate can proceed without side reactions observed from chain-capping with tolyl isocyanate.
Article
Multidisciplinary Sciences
Xiaoyu Zhao, Ye Zhao, Ming-De Li, Zhong'an Li, Haiyan Peng, Tao Xie, Xiaolin Xie
Summary: Photopolymerization-based 3D printing can achieve customized manufacturing, but the compromise between print speed and resolution remains challenging. A new approach using photooxidation of ketocoumarin as photosensitizer demonstrates high print speed and resolution on a common 3D printer.
NATURE COMMUNICATIONS
(2021)
Article
Chemistry, Physical
Weiqi Zhang, Qi Jin, Junpeng Xiao, Jing Yao, Xitian Zhang
Summary: In this study, an efficient functional V2CTx/CNT framework was constructed and employed as a modified layer of the separator to improve the performance of Li-S batteries. The battery with V2CTx/CNT separator exhibited outstanding rate performance and low capacity decay.
JOURNAL OF ALLOYS AND COMPOUNDS
(2022)
Article
Polymer Science
Zihnil A. I. Mazrad, May Lai, Thomas P. Davis, Joseph A. Nicolazzo, Kristofer J. Thurecht, Meike N. Leiske, Kristian Kempe
Summary: This study explores the application of a new initiator in polymer synthesis. The results show that this initiator can achieve a higher degree of control over the polymerization process under irradiation, resulting in well-defined polymers. In addition, tailored amine-based polymers can be prepared by using different terminating agents.
Article
Polymer Science
Ahmad Arar, Lilian Wisson, Jacques Lalevee
Summary: The study introduces a pure organic and peroxide-free redox initiating system for polymerization, which enables full control of work time and high reactivity under mild conditions.
Article
Engineering, Chemical
Feng Sun, Jinren Lu, Yuhong Wang, Jie Xiong, Congjie Gao, Jia Xu
Summary: By controlling the self-polymerisation of polydopamine in a reducing environment, a thin polydopamine coating with small particles was formed on the MCE membrane skeleton, resulting in excellent water transport performance and organic foulant removal efficiency.
FRONTIERS OF CHEMICAL SCIENCE AND ENGINEERING
(2021)
Article
Chemistry, Physical
Natalia Voronina, Hee Jae Kim, Minyoung Shin, Seung-Taek Myung
Summary: The study found that Ti substitution can improve the performance of sodium-ion battery cathode materials, including increasing initial capacity and capacity retention, as well as reducing volume changes. By pairing with a hard-carbon anode, Na[(Mn0.4Fe0.3Ni0.3)(0.9)Ti-0.1]O-2 achieved excellent cyclability and capacity retention for 300 cycles.
JOURNAL OF POWER SOURCES
(2021)
Article
Biochemistry & Molecular Biology
Alexis Barrat, Frederic Simon, Jerome Mazajczyk, Bruno Charriere, Stephane Fouquay, Jacques Lalevee
Summary: Under mild conditions, redox free radical polymerization has been recognized as an effective method for polymerizing (meth)acrylate monomers. Recently, there has been growing interest in developing new redox initiating systems due to concerns over toxicity and stability issues of existing systems. This study presents a new, low-toxicity redox initiating system based on thiophenium salt as the oxidant species, and investigates its reactivity and stability, as well as reports the synthesis of new thiophenium salts.
Article
Chemistry, Physical
Pongkarn Chakthranont, Sakvarit Nitrathorn, Sutarat Thongratkaew, Pongtanawat Khemthong, Hideki Nakajima, Ratchadaporn Supruangnet, Teera Butburee, Noriaki Sano, Kajornsak Faungnawakij
Summary: This study presents highly active and selective 2e(-) O-2 reduction catalysts based on doped carbon nanohorns, synthesized by the gas-injected arc-in-water method. The selectivity of the catalyst may be more sensitive to changes in N dopant than O dopant, and regulating both O and N dopants is an effective design strategy for efficient carbon catalysts.
ACS APPLIED ENERGY MATERIALS
(2021)
Article
Chemistry, Analytical
Yu Luo, Ruizhi Lin, Yimei Zuo, Ziyi Zhang, Yi Zhuo, Ming Lu, Shu Chen, Hui Gu
Summary: In this study, an electrochemical microsensor was designed for the selective and accurate measurement of hydrogen peroxide (H2O2) in the living brain. By tuning the structure of the probe and using a stable internal reference material, the sensor was able to track the concentration of H2O2 in real-time. The sensor was successfully applied to measure H2O2 in the Parkinson's disease mouse brain. This research provides insights into the role and impact of H2O2 in Parkinson's disease.
ANALYTICAL CHEMISTRY
(2022)
Article
Chemistry, Physical
Jun Yang, Panrun Shao, Xinran Zhao, Yunhong Liao, Chao Yan
Summary: In this study, homogeneous dispersed quinone-amine polymer nanospheres (PQANS) were synthesized to address the challenges in aqueous proton batteries (APBs) related to the solubility, capacity, and cycle life of small organic molecules. The obtained PQANS exhibited improved reversible capacity and cycling stability as an anode material. The superior proton storage mechanism and the principle of binding protons with functional groups in PQANS were elucidated through various measurements and theoretical calculations. Furthermore, a PQANS anode-based aqueous proton full battery was constructed to demonstrate its potential application.
JOURNAL OF COLLOID AND INTERFACE SCIENCE
(2023)
Review
Chemistry, Multidisciplinary
Chenyu Wu, Nathaniel Corrigan, Chern-Hooi Lim, Wenjian Liu, Garret Miyake, Cyrille Boyer
Summary: The use of photocatalysts in controlled polymerization has provided new opportunities for sophisticated macromolecular synthesis. The rational design of photocatalysts based on the knowledge of structure-property-performance relationships allows for rapid and economic tuning of the performance and functionality of polymerization systems, thus advancing polymer science.
Article
Chemistry, Multidisciplinary
Zhiquan Jin, Sijia Jin, Xiaofeng Tang, Wenxian Tan, Da Wang, Shuang Song, Haiyan Zhang, Tao Zeng
Summary: This study presents the design of conjugated acetylenic polymers (CAPs) with different spatial arrangements and intramolecular spacers for efficient photocatalytic hydrogen peroxide (H2O2) production. The linear configuration of diacetylene moieties in CAPs enhances charge carrier mobility compared to cross-linked networks. Optimizing the intramolecular spacer between diacetylene moieties leads to a downshifted valence band and thermodynamically feasible H2O2 production. The optimized CAPs with a linear configuration exhibit superior H2O2 yield rate, apparent quantum efficiency, and solar-to-chemical energy conversion efficiency compared to previous conjugated polymers.
Article
Biochemistry & Molecular Biology
Tom E. Forshaw, Julie A. Reisz, Kimberly J. Nelson, Rajesh Gumpena, J. Reed Lawson, Thomas J. Jonsson, Hanzhi Wu, Jill E. Clodfelter, Lynnette C. Johnson, Cristina M. Furdui, W. Todd Lowther
Summary: Human peroxiredoxins (Prx) are involved in various cellular functions and diseases, and can be repaired by human sulfiredoxin (Srx), hydrogen sulfide (H2S), and glutathione (GSH) after being hyperoxidized. Studying engineered Prx2 and Prx3 dimers, it was found that loss of the active site interface can make variants more resistant to repair, and it was revealed for the first time potential cooperation between Prx isoforms and GSH and H2S in supporting Srx activity.
Review
Energy & Fuels
Dunyu Liu, Kailong Xu, Jingjing Mae, Qiuqi Liu, Yunpei Fan, Chaoran Wang, Xudong Wang, Jing Jin, Huancong Shi
Summary: This paper reviews the rational design methods for transition metal-based, SCR-based, precious metal-based, and fly ash-based catalysts, focusing on the selection of active sites, promoters, and supports. The characteristics of adsorption, oxidation, and desorption sites for Hg0 are discussed, along with the choice of appropriate supports. The design considerations for incorporating gases such as NO, H2S, CO, H2, and SO2 are also addressed. The work contributes to the development of efficient catalysts for Hg0 removal.
Article
Polymer Science
Jasmine Sinha, Shafer Soars, Christopher N. Bowman
Summary: This article describes an efficient enamine organocatalyzed thiol-Michael click reaction and its broad application in cross-linking polymerizations. The nucleophilicity of the enamines used is crucial for the reaction efficiency and overall yields, with in situ formation of an enamine via photo-deprotection of an amine showing promising results in facilitating thiol-Michael reactions and improving functional group conversion rates.
Article
Nanoscience & Nanotechnology
Sudheendran Mavila, Jasmine Sinha, Yunfeng Hu, Maciej Podgorski, Parag K. Shah, Christopher N. Bowman
Summary: This study presents a scalable method for synthesizing high refractive index, optically transparent photopolymers using low-viscosity multifunctional thiol and alkyne monomers through thiol-yne click reactions. These reactions create sulfide linkages, allowing for the production of cross-linked high optical quality photopolymers compared to thiol-ene systems.
ACS APPLIED MATERIALS & INTERFACES
(2021)
Review
Chemistry, Multidisciplinary
Benjamin D. Fairbanks, Laura J. Macdougall, Sudheendran Mavila, Jasmine Sinha, Bruce E. Kirkpatrick, Kristi S. Anseth, Christopher N. Bowman
Summary: Photoclick chemistry involves a collection of click reactions performed with the application of light, offering spatiotemporal control, high selectivity, and excellent product yields. Different photoclick reactions have their own advantages and disadvantages, and a broader understanding of their physical and chemical characteristics is essential for realizing the full potential of this chemistry.
Article
Chemistry, Physical
Samantha L. Millican, Jacob M. Clary, Charles B. Musgrave, Stephan Lany
Summary: This study investigates the redox mediating defect mechanism of solar thermochemical hydrogen production candidate material Hercynite using first-principles calculations. The results show the importance of defect interactions and suggest that oxygen defect entropy can positively influence the expansion of the thermodynamic window. This study is significant for guiding the discovery and design of suitable oxides.
CHEMISTRY OF MATERIALS
(2022)
Article
Chemistry, Physical
Samantha L. Millican, Ann M. Deml, Meagan Papac, Andriy Zakutayev, Ryan O'Hayre, Aaron M. Holder, Charles B. Musgrave, Vladan Stevanovic
Summary: This paper presents a new method for accurately predicting defect concentrations in complex oxides, taking into account atomic and magnetic disorder as well as effects beyond the dilute defect limit. Using this method, the predicted defect concentrations are in good agreement with experimental values.
CHEMISTRY OF MATERIALS
(2022)
Article
Chemistry, Physical
Jacob K. Kenny, Samuel Breske, Nicholas R. Singstock
Summary: It is demonstrated that FCEVs are economically competitive as RHAVs and expected price reductions can make them the most profitable technology, while also catalyzing the development of local hydrogen infrastructure.
INTERNATIONAL JOURNAL OF HYDROGEN ENERGY
(2022)
Article
Materials Science, Multidisciplinary
Sarah K. Bull, Theodore Champ, Sai Raj, Alan W. Weimer, Charles B. Musgrave
Summary: Density functional theory was used to screen refractory materials as high-temperature hydrogen permeation barriers. The study calculated activation energies and analyzed the properties of diffusing hydrogen atoms in the materials. Experimental evaluation confirmed the resistance of some nitride materials to nitrogen loss at high temperatures. This research provides theoretical support for effective hydrogen barriers at high temperatures.
JOURNAL OF NUCLEAR MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Karin U. D. Calvinho, Abdulaziz W. Alherz, Kyra M. K. Yap, Anders B. Laursen, Shinjae Hwang, Zachary J. L. Bare, Zachary Clifford, Charles B. Musgrave, G. Charles Dismukes
Summary: The development of efficient electrocatalysts for the CO2 reduction reaction to produce multicarbon products has been limited by high overpotentials and poor selectivity. By introducing iron phosphide as a catalyst, carbon product selectivity can be tuned by increasing negative bias.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Chemistry, Multidisciplinary
Zachary-L Bare, Ryan N. Morelock, Charles B. Musgrave
Summary: A high-throughput computational framework is used to identify novel multinary perovskite redox mediators, specifically Gd-containing perovskite oxide compositions that split water. The framework employs empirical approaches to evaluate material stabilities, electronic properties, and oxygen vacancy thermodynamics. By applying this computational scheme, 83 promising Gd-containing perovskite oxides are discovered, with three exhibiting catalytic activity in splitting water.
ADVANCED FUNCTIONAL MATERIALS
(2022)
Article
Chemistry, Physical
Ryan J. Morelock, Zachary J. L. Bare, Charles B. Musgrave
Summary: In this study, a parameterization framework based on the bond-valence method (BVM) was developed, which captures the relative stabilities computed by density functional theory (DFT) using the BVM global instability index (GII). The framework was tested against a dataset of 188 experimentally observed perovskite oxides and showed improved accuracy in identifying the ground state structures.
JOURNAL OF CHEMICAL THEORY AND COMPUTATION
(2022)
Article
Chemistry, Multidisciplinary
Nicholas R. Singstock, Charles B. Musgrave
Summary: By simulating the nitrogen reduction reaction mechanism on Fe2Mo6S8, the reasons for its high activity and selectivity are revealed, and new principles for designing stable multinary electrocatalysts for other reactions are proposed.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2022)
Article
Chemistry, Physical
Paige Brimley, Hussain Almajed, Yousef Alsunni, Abdulaziz W. Alherz, Zachary J. L. Bare, Wilson A. Smith, Charles B. Musgrave
Summary: This study uses Grand Canonical Density Functional Theory (GC-DFT) to model the electrochemical CO2 reduction process over metal-and nitrogen-doped graphene catalysts (MNCs) and includes the effects of the applied potential. The results predict effective catalysis of CO2R by Sc, Ti, Co, Cu, and Zn-N4Cs at moderate to large reducing potentials. The GC-DFT-computed density of states analysis demonstrates the critical role of adsorbed *CO2- anion in CO2R activation.
Article
Chemistry, Physical
Zhiming Liang, Yangyang Wang, Ben Pei, Seoung-Bum Son, Martin Nguyen, Nicholas R. Singstock, Shaofeng Huang, Michael Mo, Jianlin Li, M. Stanley Whittingham, Chunmei Ban
Summary: By using a conductive framework made of commercial micro-sized carbon fibers (Cfs), the energy density of lithium-ion batteries (LIBs) can be increased and the manufacturing costs can be lowered. This approach addresses challenges in manufacturing, rate performance, and cycling stability. The Cfs-integrated electrodes have high mass loading and exhibit high areal capacity, rate performance, and a lengthy cycling lifetime. Practical LIBs fabricated using this method have shown promising results in terms of energy density and cycling stability.
ADVANCED ENERGY MATERIALS
(2023)
Article
Chemistry, Physical
Forrest P. Hyler, Brian A. Wuille Bille, Jessica C. Ortiz-Rodriguez, Ana Sanz-Matias, Subhayan Roychoudhury, Joseph T. Perryman, Christopher J. Patridge, Nicholas R. Singstock, Charles B. Musgrave, David Prendergast, Jesus M. Velazquez
Summary: The electronic structure and local coordination of binary and ternary Chevrel Phases were investigated. The effect of compositional and structural modification on the electronic structure was quantified, and the expansion, contraction, and anisotropy of Mo-6 clusters in the Chevrel Phase frameworks were analyzed. The results showed that metal-to-cluster charge transfer upon intercalation is dominated by the chalcogen acceptors, highlighting the importance of chalcogen compositions in the electronic and local structure of Chevrel Phases.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)