Correction
Chemistry, Physical
Rassmus Andersson, Guiomar Hernandez, Jonas Mindemark
Summary: This correction provides a more accurate and reliable quantification of the ion coordination strength in polymer electrolytes. The errors in the original study have been addressed and corrected.
PHYSICAL CHEMISTRY CHEMICAL PHYSICS
(2022)
Article
Chemistry, Multidisciplinary
Jia Zhou, Xiao Wang, Jifang Fu, Liya Chen, Xiangrong Wei, Rongrong Jia, Liyi Shi
Summary: This study presents a 3D cross-linked metal-organic framework (MOF)-derived polymer solid electrolyte with good mechanical and ionic conductive properties, capable of inhibiting lithium dendrite growth. The MOF with optimized pore size and strong imidazole cation sites controls the migration of anions, resulting in a uniform Li+ flux and high lithium-ion transference number. The lithium symmetric batteries assembled with this electrolyte exhibit excellent long-cycle stability and cycle reversibility.
Article
Chemistry, Multidisciplinary
Ziyong Li, Ji-Rui Zhang, Xu-Ke Tian, Shuren Yang, Si Chen, Hui Zhou, Xiao-Gang Yang
Summary: Fluorescent dithienylethene-based photochromic molecule BFBDTE exhibits visible light-controlled fluorescence and thermally activated delayed fluorescence (TADF) switching, as well as rapid and repeatable cyclization and cycloreversion reactions in PMMA. It also demonstrates a remarkable on-off photoelectronic response between the open- and closed-form and holds promise for applications in photoswitchable molecular devices and optical memory storage systems.
Article
Chemistry, Physical
Florian Gebert, Jonathan Knott, Robert Gorkin, Shu-Lei Chou, Shi-Xue Dou
Summary: The paper reviews the development of solid-polymer and gel-polymer electrolytes for sodium-ion batteries as a way to enhance competitiveness. It discusses the targeted manipulation of these electrolytes and their significance for practical applications, as well as the interdependence of various electrochemical and mechanical properties. Additionally, a quantitative comparison of reported values across different polymer classes is conducted for the first time.
ENERGY STORAGE MATERIALS
(2021)
Article
Chemistry, Multidisciplinary
Pan-Pan Jiang, Haili Qin, Jing Dai, Shu-Hong Yu, Huai-Ping Cong
Summary: This article presents an extremely stretchable and self-healing conductor material that combines hard and soft tactics to achieve high stretchability and self-repair capability. By sandwiching the conductor with a newly developed dielectric, an ultrahigh stretchable and omni-healable capacitive strain sensor is demonstrated for the first time, showing great potentials in the field of wearable electronics and soft robotics.
Article
Polymer Science
Aidan E. Izuagbe, Vinh X. Truong, Bryan T. Tuten, Peter W. Roesky, Christopher Barner-Kowollik
Summary: We introduce a single-chain nanoparticle system that can dynamically adjust its internal structure using visible light. The system consists of linear polymer chains and variable photoresponsive azobenzene units, allowing reversible isomerization. The reversible compaction and isomerization can be observed by changing the light wavelength.
Review
Polymer Science
Jayeeta Chattopadhyay, Tara Sankar Pathak, Diogo M. F. Santos
Summary: This review summarizes the applications and advantages of polymer electrolytes in lithium-ion batteries, and discusses the ion transport mechanisms, preparation methods, and recent advancements in specific battery systems. Moreover, it proposes strategies for developing novel polymer electrolytes for high-performance lithium-ion batteries.
Article
Chemistry, Multidisciplinary
Chongyang Liu, Shi Wang, Xinyi Wu, Shijun Xiao, Chao Liu, Henan Cai, Wen-Yong Lai
Summary: Inspired by the unique mesh geometry of fishing nets and knotted fiber structures, new crosslinkers and elastic components are introduced into polyzwitterionic electrolytes to construct high-strength and ultra-flexible fishing-net-like structure electrolytes. The crosslinkers rich in -NH form chemical and physical crosslinking points, resulting in high strength, while the elastic segments provide super flexibility. The collective regulation of anions and Li+ by the polymer backbone enables stable Li+ deposition and suppresses the growth of lithium dendrites. This work presents a new perspective for constructing polymer electrolytes with synergistic cation-anion regulation functions for high safety and high energy density solid-state lithium batteries.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Polymer Science
Yu Tan, Huan Chen, Wenbing Kang, Xu Wang
Summary: This study presents a light-mediated strategy for synthesizing dry ion-conducting elastomers with dynamic bottlebrush network structures. The optimized materials exhibit high ionic conductivity, good elasticity, outstanding healing ability, excellent interfacial adhesiveness, flame retardancy, and strain and temperature dual sensitivity.
Article
Chemistry, Physical
Canhui Ling, Tuoya Naren, Xinsheng Liu, Jixu Yang, Pengfei Xiao, Weifeng Wei, Xiaobo Ji, Gui-Chao Kuang, Libao Chen
Summary: In this study, a novel self-healable polymer electrolyte (SHPE) was developed by in-situ polymerizing a mixture of butyl acrylate and 2-ureido-4-pyrimidinone (UPy) with plastic crystal succinonitrile (SN) and lithium bis(trifuoromethanesulfonyl) imide (LiTFSI). The SHPE exhibited high ionic conductivity and mechanical strength, addressing the limitations of traditional polymer electrolytes and improving the practical performance of lithium metal batteries.
MATERIALS TODAY ENERGY
(2023)
Article
Chemistry, Multidisciplinary
Liwei Zhao, Ming Gong, Jian Yang, Jinlou Gu
Summary: By integrating multistimuli-response molecules into the framework of NU-1000, a light-induced and pH-modulated artificial nanochannel with ion-switchable characteristics is prepared. The reversible changes in redox peak currents of model cations and anions under different light and pH signal combinations are achieved, indicating the potential applications in electronic devices and life sciences.
Article
Chemistry, Multidisciplinary
Jing Chen, Xuetian Deng, Yiyang Gao, Yuanjun Zhao, Xiangpeng Kong, Qiang Rong, Junqiao Xiong, Demei Yu, Shujiang Ding
Summary: An integrated cathode/polymer electrolyte has been developed to address the electrolyte-electrodes interfacial issues in all-solid-state lithium metal batteries, resulting in improved electrochemical performance and mechanical properties.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2023)
Article
Nanoscience & Nanotechnology
Gerrit Michael Overhoff, Md Yusuf Ali, Jan-Paul Brinkmann, Peter Lennartz, Hans Orthner, Mohaned Hammad, Hartmut Wiggers, Martin Winter, Gunther Brunklaus
Summary: Researchers have developed a ceramic-polymer hybrid electrolyte to enhance the performance of rechargeable lithium metal batteries. The hybrid electrolyte, featuring an oxide-rich layer, stabilizes the interface between lithium metal and the electrolyte, reducing polarization and lithium dendrite growth. Experimental results show that the hybrid electrolyte enables long-term single-side lithium deposition at high current densities and exhibits high ionic conductivities. In LiNi0.6Co0.2Mn0.2O2||Li metal cells, the electrolyte demonstrates impressive capacity retention.
ACS APPLIED MATERIALS & INTERFACES
(2022)
Article
Chemistry, Physical
Priyadarshini Mirmira, Claire Fuschi, Walker Gillett, Peiyuan Ma, Jin Zheng, Zachary D. Hood, Chibueze V. Amanchukwu
Summary: Hybrid ceramic-polymer solid state electrolytes show promise for high energy-density lithium metal batteries. Our work demonstrates that using nonconductive, nonreactive polymers in hybrid electrolytes can improve conductivity and enable longer term lithium cycling.
ACS APPLIED ENERGY MATERIALS
(2022)
Article
Chemistry, Multidisciplinary
Sangyeop Lee, Im Kyung Han, Na Gyeong Jeon, Yubin Lee, Hye Bin Son, Dong-Yeob Han, Seoha Nam, Taehun Chung, Myung-Jun Kwak, Youn Soo Kim, Soojin Park
Summary: A gel electrolyte based on zwitterionic polymer has been proposed for advanced aqueous zinc metal batteries. By controlling the concentration of dissolved salt, electrochemical behaviors can be modified, improving the reversibility of the zinc anode and extending the cycle life.
Article
Chemistry, Multidisciplinary
Robert D. Murphy, Ronnie V. Garcia, Seung J. Oh, Tanner J. Wood, Kyoo D. Jo, Javier Read de Alaniz, Ed Perkins, Craig J. Hawker
Summary: Describes the synthesis of functional hydrogels from 3-arm diblock copolypeptide stars, which achieve mechanical stability and biological activity through physical and photo-crosslinking, enabling direct ink writing of 3D objects with high precision and biological viability.
ADVANCED MATERIALS
(2023)
Article
Materials Science, Composites
Younghoon Kwon, Soyoung E. Seo, Jaejun Lee, Szabolcs Berezvai, Javier Read de Alaniz, Claus D. Eisenbach, Robert M. McMeeking, Craig J. Hawker, Megan T. Valentine
Summary: Additive manufacturing allows the creation of bio-inspired materials with complex architectures and diverse properties. By using a digital light processing strategy, polymer foams with controlled porosity were 3D printed by incorporating thermally expandable microspheres. The foams showed remarkable resilience under cyclic loading, maintaining their modulus and energy dissipation even at large deformations.
COMPOSITES COMMUNICATIONS
(2023)
Article
Nanoscience & Nanotechnology
Yi Chen, Philip Mickel, Huijie Pei, Yingfeng Wen, Xin Guan, Yun Wang, Xuyang Wang, Omar Al Mhtachem, Cheng Zhang, Hui Nie, Xingping Zhou, Petr Kral, Xiaolin Xie
Summary: Researchers have developed a new polymeric separator with functional active sites, forming bioinspired ion-conducting nanochannels. This separator selectively accelerates the transport of lithium ions, leading to improved performance and stability of lithium metal batteries.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Polymer Science
Declan P. Shannon, Joshua D. Moon, Christopher W. Barney, Nairiti J. Sinha, Kai-Chieh Yang, Seamus D. Jones, Ronnie V. Garcia, Matthew E. Helgeson, Rachel A. Segalman, Megan T. Valentine, Craig J. Hawker
Summary: A versatile synthetic procedure is reported to prepare modular PEG-acrylate networks with independently tunable covalent and supramolecular cross-linking. By controlling the ratio of building blocks, dual cross-linked networks reinforced by clustered iron-catechol domains are prepared and exhibit a wide range of properties. This stepwise approach also allows for local patterning of PEG-based films through masking techniques.
Article
Polymer Science
Oscar Nordness, Joshua D. Moon, Nico Marioni, Everett S. Zofchak, Peter M. Richardson, Matthew R. Landsman, Lynn E. Katz, Craig J. Hawker, Venkat Ganesan, Rachel A. Segalman, Raphaele J. Clement
Summary: The effects of ligand basicity on water and ion transport within hydrogel membranes are investigated using a library of functionalizable poly(ethylene glycol) diacrylate (PEGDA) polymer networks. The study reveals that the self-diffusion of water molecules and ions is primarily driven by the hydration level of the membrane. The interaction between triflate anions and the polymer significantly reduces ion and water mobility.
Article
Polymer Science
KaitlinR. Albanese, Yoichi Okayama, Parker T. Morris, Matthias Gerst, Rohini Gupta, Joshua C. Speros, Craig J. Hawker, Chungryong Choi, Javier Read de Alaniz, Christopher M. Bates
Summary: We report a strategy to create degradable poly(acrylate) pressure-sensitive adhesives (PSAs) using 1,2-dithiolanes as drop-in replacements for traditional acrylate comonomers. The resulting PSA materials have comparable thermal and viscoelastic properties to nondegradable analogues, but can undergo reversible transformation between high and low molecular weights through oxidative repolymerization and reductive degradation. This simple and versatile chemistry could play a pivotal role in improving the sustainability of contemporary adhesives.
Article
Chemistry, Multidisciplinary
Robert D. Murphy, Colm Delaney, Srikanth Kolagatla, Larisa Florea, Craig J. Hawker, Andreas Heise
Summary: This study reports the design of photopolymerizable copolypeptides with tailored mechanical properties for additive manufacturing of 3D objects. The copolypeptides are able to form hydrogels suitable for direct ink writing or direct laser writing, leading to mechanically robust 3D structures.
ADVANCED FUNCTIONAL MATERIALS
(2023)
Article
Engineering, Environmental
Zhen Shi, Jirong Wang, Kairui Guo, Hongli Wang, Hui Nie, Zhigang Xue
Summary: Researchers report a class of three-dimensional interconnected polyurea-based electrolytes with enhanced phase separation structure using a deep eutectic solvent (DES). The DES selectively plasticizes the soft segment in polyurea and increases its chain motion, while inducing further aggregation of the hard segment in polyurea and forming an enhanced dynamically physical cross-linking network. The gel polyurea-based electrolytes (GPUEs) with a phase separation structure achieve decoupling of mechanical properties and ionic conductivity, showing a combination of superior mechanical strength (3.2 MPa) and high ionic conductivity (1.5 x 10-4 S cm-1, 30 degrees C). Moreover, the Li|GPUEs|LiFePO4 coin cell shows a satisfactory initial discharge specific capacity (higher than 150 mAh g-1 at 1 C), and the capacity retention is higher than 80% after 500 cycles.
CHEMICAL ENGINEERING JOURNAL
(2023)
Article
Polymer Science
Yoichi Okayama, Taejun Eom, Michael Czuczola, Allison Abdilla, Jacob R. Blankenship, Kaitlin R. Albanese, Javier Read de Alaniz, Christopher M. Bates, Craig J. Hawker
Summary: The synthetic utility of heterotelechelic polydimethylsiloxane (PDMS) derivatives was enhanced by using a specifically designed silyl hydride (Si-H)-based initiator for anionic ring-opening polymerization (AROP) of hexamethylcyclotrisiloxane (D-3) monomers. The resulting PDMS polymers had high chain-end fidelity and heterotelechelic functionality. In situ termination of the propagating chain end with different chlorosilanes and functionalized alkenes further increased the diversity of the PDMS derivatives. The living nature of the polymerization allowed for the synthesis of narrow-dispersity polymers with a wide range of molar masses. Additionally, the feasibility of synthesizing supersoft bottlebrush networks using the PDMS macromonomers was demonstrated.
Article
Polymer Science
Gervase Ng, Zilong Wu, Tong Zhang, Anh Phong Dang, Yin Yao, Andrew R. J. Nelson, Stuart W. Prescott, Almar Postma, Graeme Moad, Craig J. Hawker, Cyrille Boyer
Summary: An oxygen-tolerant SI-PhotoRAFT technique has been developed for efficient synthesis of surface-tethered polymer brushes under low-energy near-infrared light. The technique takes advantage of the unique properties of NIR light to prepare polymeric coatings, even through barriers that are opaque to visible light. It enables precise modulation of brush height and sequential chain extension, as well as orthogonal control over polymerization and cross-linking processes using two different wavelengths.
Article
Chemistry, Multidisciplinary
Ronnie V. Garcia, Elizabeth A. Murphy, Nairiti J. Sinha, Yoichi Okayama, Juan Manuel Uruena, Matthew E. Helgeson, Christopher M. Bates, Craig J. Hawker, Robert D. Murphy, Javier Read de Alaniz
Summary: Shear-recoverable hydrogels with rapid self-recovery based on block copolypeptides have the potential to be used in extrudable and injectable 3D-printing applications. By synthesizing 3-arm star-shaped block copolypeptides with different side chains and block lengths, hydrogels with diverse microstructures and mechanical properties are prepared. The study reveals that non-canonical & beta;-sheet blocks based on phenyl glycine form more stable networks with superior mechanical properties and writability compared to natural amino acid counterparts.
Article
Polymer Science
Colton A. D'Ambra, Michael Czuczola, Patrick T. Getty, Elizabeth A. Murphy, Allison Abdilla, Souvagya Biswas, Jodi M. Mecca, Thomas D. Bekemeier, Steven Swier, Craig J. Hawker, Christopher M. Bates
Summary: A versatile synthetic platform is reported for the synthesis of high molecular weight graft copolymers with excellent control over molecular weight and grafting density. The controlled nature of side-chain growth is confirmed by selective degradation of the siloxane backbone, and grafting density and functionality can be further controlled by using a mixture of thiols.
JOURNAL OF POLYMER SCIENCE
(2023)
Article
Polymer Science
Kaitlin R. Albanese, Jacob R. Blankenship, Timothy Quah, Amy Zhang, Kris T. Delaney, Glenn H. Fredrickson, Christopher M. Bates, Craig J. Hawker
Summary: The potential of ABC triblock terpolymers in improving the mechanical properties of thermoplastic elastomers is demonstrated by comparing them with symmetric ABA/CBC analogs having similar molecular weights and volume fraction of B and A/C domains. The ABC architecture enhances elasticity through full chain bridging between discrete hard domains, minimizing mechanically unproductive loops. In addition, ABC triblock terpolymers allow for a higher fraction of hard-block domains while maintaining elasticity, which is traditionally only possible with non-linear architectures or highly asymmetric ABA triblock copolymers. These advantages provide a tunable platform to create materials with practical applications while improving our fundamental understanding of chain conformation and structure-property relationships in block copolymers.
Review
Nanoscience & Nanotechnology
Yiqing Wang, Zhenzhen Wu, Faezeh Makhlooghi Azad, Yutong Zhu, Lianzhou Wang, Craig J. Hawker, Andrew K. Whittaker, Maria Forsyth, Cheng Zhang
Summary: The incorporation of fluorine into battery components can improve the energy density, safety, and cycling stability of rechargeable batteries. This review explores the design and utilization of fluorine-containing species in advanced batteries, examining the relationship between their chemical structure and battery performance. It also discusses the challenges and opportunities of fluorinated batteries within the present regulatory framework.
NATURE REVIEWS MATERIALS
(2023)
Article
Polymer Science
Jeffrey L. Self, Veronica G. Reynolds, Jacob Blankenship, Erin Mee, Jiaqi Guo, Kaitlin Albanese, Renxuan Xie, Craig J. Hawker, Javier Read de Alaniz, Michael L. Chabinyc, Christopher M. Bates
Summary: A new class of supersoft, conductive composites comprising carbon nanotubes embedded in bottlebrush polymer networks has been reported. These materials are significantly softer than comparable composites and possess typical conductivity. The presence of dynamic polyester bonds in the bottlebrush matrix chemistry allows for thermal (re)processing.