Article
Chemistry, Multidisciplinary
Kaihao Chen, Zhiqi Zhu, Tianwen Bai, Yixuan Mei, Tianlun Shen, Jun Ling, Xufeng Ni
Summary: We designed and performed a novel strategy to produce polyesters using CO2 and olefins, by individually synthesizing PCL and EVL oligomers through anionic ring-opening polymerization and conjugated addition oligomerization, and then inserting EVL oligomers into PCL by transesterification, resulting in polyesters with tunable topology and composition.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Pieter-Jan Voorter, Gayathri Dev, Axel-Laurenz Buckinx, Jinhuo Dai, Priya Subramanian, Anil Kumar, Neil R. Cameron, Tanja Junkers
Summary: This study presents a one-pass continuous flow strategy to directly form block copolymer nanoaggregates from monomers. A significant improvement in continuous flow dialysis, achieved by developing an inline dialysis purification system, enables the fully continuous operation and high throughput operation. The developed system is at least 4-5 times faster than conventional dialysis and reduces the required amount of solvent by almost an order of magnitude compared to conventional methods.
Review
Polymer Science
James M. Eagan
Summary: This paper reviews an efficient route for converting sustainable carbon feedstocks into novel macromolecules by catalytic conversion of carbon dioxide and 1,3-butadiene into unsaturated lactone monomers. The chemical reactivity of this monomer and various polymerization methods are discussed, along with the functional properties of materials derived from these processes. The advances in polymer chemistry and future directions of the field are also highlighted.
MACROMOLECULAR RAPID COMMUNICATIONS
(2023)
Article
Multidisciplinary Sciences
Yongjia Lou, Luyan Xu, Ninglin Gan, Yunyan Sun, Bo-Lin Lin
Summary: This study reports a method for synthesizing chemically recyclable solid polyesters using CO2 and inexpensive bulk chemicals as feedstock. The polyesters have high CO2 content and large molecular weight, and can be used to fabricate transparent membranes with pressure-sensitive adhesive properties. Mechanistic studies reveal water impurity removal as the key to successful polymerization. Complete monomer recovery is achieved, providing a new strategy for scalable chemical utilization of CO2.
Article
Chemistry, Multidisciplinary
Rachel M. Rapagnani, Rachel J. Dunscomb, Alexandra A. Fresh, Ian A. Tonks
Summary: This study presents an alternative route to functionalizable, recyclable polyesters derived from CO2, butadiene, and hydrogen. By catalytic ring-opening polymerization, polyesters with vinyl side chains were synthesized, which have a low ceiling temperature and are inherently biodegradable. This expands access to new polymer feedstocks that were once considered unfeasible.
Article
Chemistry, Applied
Jiansen Pan, Liqin Mei, Huan Zhou, Cong Zhang, Qingyi Xie, Chunfeng Ma
Summary: Degradable hyperbranched anti-biofouling polymers synthesized via RAFT polymerization exhibit inhibitory effects on marine bacteria and diatom adhesion, showing potential for marine anti-biofouling applications.
PROGRESS IN ORGANIC COATINGS
(2022)
Article
Polymer Science
Jian Tang, Zijian Xu, Zelong Liu, Yuan Fu, Jing Hua
Summary: Aluminum-based transition-metal-free catalysts have been extensively studied for alpha-olefin polymerization, but they face challenges in conjugated dienes polymerization. In this study, we developed a series of aluminum-based catalyst precursors for 1,3-butadiene polymerization, achieving high catalytic activity and selectivity. The microstructures of the resulting polymers could be controlled by adjusting the ligands.
Article
Polymer Science
Patricia R. Calvo, Chelsea A. Sparks, Justin Hochberg, Kenneth B. Wagener, Brent S. Sumerlin
Summary: Hyperbranched aminobisphosphonic acid polymers were synthesized via RAFT self-condensing vinyl polymerization. A novel acrylamide-functional chain transfer monomer and a 3-component Kabachnik-Fields reaction were used to introduce functional groups, creating acid-degradable imine hydrogels.
MACROMOLECULAR RAPID COMMUNICATIONS
(2021)
Article
Polymer Science
Murtaza Khan, Thiago R. Guimaraes, Kenneth Choong, Graeme Moad, Sebastien Perrier, Per B. Zetterlund
Summary: The study overcomes the limitation of block copolymer synthesis that requires consideration of the order of blocks by utilizing RAFT emulsion polymerization, successfully preparing an alternating pentablock copolymer composed of methacrylates and styrene.
Article
Polymer Science
Fen You, Xiaoyu Wang, Wenyu Shi, Xuyang Yan, Xiaochao Shi
Summary: This study successfully synthesized polymers with diverse polar functionalities, including highly regular polymers and copolymers, using a rare-earth metal catalytic system. The composition of the copolymers could be easily controlled by the initial comonomer feed ratio.
Article
Polymer Science
Kana Takebayashi, Arihiro Kanazawa, Sadahito Aoshima
Summary: The cationic ring-opening copolymerization of cyclic acetals and 1,3-dioxolan-4-ones (DOLOs) was investigated, with a focus on understanding the polymerization mechanisms. The copolymerization of 1,3-dioxepane and 5-methyl-1,3-dioxolan-4-one successfully occurred using CF3SO3H as a catalyst, resulting in high molecular weight copolymers. NMR spectrometry and electrospray ionization mass spectrometry were used to analyze the detailed structure of the copolymers, which indicated that the copolymerization proceeds through an activated monomer mechanism involving the reaction of a hydroxy group and a proton-attached DOLO. Acid-catalyzed transacetalization reactions also likely occurred during the copolymerization process.
Article
Chemistry, Multidisciplinary
Shan Tang, Yajun Zhao, Kyoko Nozaki
Summary: This study reports a new method to successfully incorporate CO2 into polyethylenes, synthesizing two types of main-chain-functionalized polyethylenes through different copolymerization strategies, providing a new pathway for the preparation of diverse polyethylene materials.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2021)
Article
Materials Science, Multidisciplinary
Siyuan Zhang, Jiao He, Xinjian Cheng
Summary: In this study, amphiphilic hyperbranched polymers (AHBPs) were synthesized using a chain transfer agent (CTA) and reversible addition-fragmentation chain transfer-self-condensing vinyl polymerization (RAFT-SCVP). The synthesized hyperbranched polymer was used as a macromolecular CTA to prepare fluorescent probes via RAFT polymerization. These macromolecular fluorescent probes showed highly sensitive and selective recognition of 4-nitrophenol (4-NP) and revealed a unique fluorescence quenching effect termed enriching inner filter effect (IFE). This research provides a valuable approach for the development of highly sensitive polymer fluorescent probes.
ACS APPLIED POLYMER MATERIALS
(2023)
Article
Chemistry, Multidisciplinary
Jiadong Tang, Maosheng Li, Xianhong Wang, Youhua Tao
Summary: We have achieved the one-pot production of sequence-controlled block copolymer from mixed monomers using a switchable catalyst. The method allows for chemoselective and efficient polymerization reactions, resulting in a high conversion rate of CO2.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Chemistry, Multidisciplinary
Javed R. Pathan, Subhrajyoti Bhandary, Kana M. Sureshan
Summary: We designed and synthesized a malonamide-derived monomer with azide and alkyne units for topochemical polymerization to produce nylon (n,3). Two polymorphs M1 and M2 were obtained upon crystallization of this monomer. The polymorphs exhibited suitable crystal packings for topochemical azide-alkyne cycloaddition polymerization. Depending on the polymorph, heating resulted in the regiospecific formation of either 1,4-disubstituted-1,2,3-triazolyl-linked polymer (M1) or 1,5-disubstituted-1,2,3-triazolyl-linked polymer (M2). These single-crystal-to-single-crystal polymerizations allowed for atomic resolution structure analysis using single-crystal X-ray diffraction. This is the first reported instance of synthesizing two chemically distinct polymers from a single monomer.
JOURNAL OF THE AMERICAN CHEMICAL SOCIETY
(2023)
Article
Chemistry, Multidisciplinary
Huan Qiu, Ting Shen, Zhening Yang, Feng Wu, Xiaohong Li, Yingfeng Tu, Jun Ling
Summary: Janus polymerization was utilized to synthesize multiblock copolymers with self-assembly capabilities, good shape memory properties, and potential applications in biomedical devices. The distinguishable chemical structures and thermal properties between Janus MBCPs and cationic random copolymers were confirmed, providing insights into the unique features of Janus polymerization for advanced material design and applications.
CHINESE JOURNAL OF CHEMISTRY
(2022)
Article
Polymer Science
Siqi Wang, Wanli Chen, Jun Ling
Summary: A random copolymer PiPo was synthesized by copolymerizing N-phenyloxycarbonyl-C-substituted glycine monomers with N-phenyloxycarbonyl-N-substituted glycine monomers. The solubility of PiPo depends on the compositions of the peptide and peptoid repeat units.
Article
Polymer Science
Yanping Li, Songyi Xu, Jun Ling, Ke Pan, Yujian Liu, Yougen Chen
Summary: This study presents a novel controlled/living ring-opening polymerization method for epsilon-caprolactone and delta-valerolactone using EDPP and DPP. The unique equilibrium reaction between the active phosphinite center and its protonated dormant species plays a crucial role in achieving controlled polymerization. The living nature of the polymerization process is confirmed through kinetic studies and chain extension experiments, leading to the synthesis of polyesters with controlled molar masses and moderate dispersities.
Article
Chemistry, Multidisciplinary
Bo Song, Tianwen Bai, Dongming Liu, Rong Hu, Dan Lu, Anjun Qin, Jun Ling, Ben Zhong Tang
Summary: In this study, CO2-based polyesters were successfully degraded into high-value derivatives through controlled reaction conditions. The degradation process was visualized and applied in various fields such as bioimaging and waste recovery, solving the end-of-life issue of polymers.
Article
Chemistry, Multidisciplinary
Kaihao Chen, Zhiqi Zhu, Tianwen Bai, Yixuan Mei, Tianlun Shen, Jun Ling, Xufeng Ni
Summary: We designed and performed a novel strategy to produce polyesters using CO2 and olefins, by individually synthesizing PCL and EVL oligomers through anionic ring-opening polymerization and conjugated addition oligomerization, and then inserting EVL oligomers into PCL by transesterification, resulting in polyesters with tunable topology and composition.
ANGEWANDTE CHEMIE-INTERNATIONAL EDITION
(2022)
Article
Engineering, Biomedical
Jingya Xia, Liying Wang, Tianlun Shen, Ping Li, Peiyun Zhu, Shengnan Xie, Zhenyan Chen, Fei Zhou, Jingfeng Zhang, Jun Ling, Xiangrui Liu, Hong Yu, Jihong Sun
Summary: Despite the initial promise of photothermal ablation (PTA) therapy, the inability to completely ablate large tumors is problematic. This study developed a smart photothermal nanosystem (PBM) based on FDA-approved Prussian blue (PB) nanoparticles, doped with Mn (III) to address this issue. The PBM nanosystem amplified the PTA-induced cGAS-STING pathway, leading to a robust immune response and suppression of both local residual and distant tumors.
ACTA BIOMATERIALIA
(2023)
Article
Chemistry, Multidisciplinary
Yixuan Mei, Kaihao Chen, Jiayu Gu, Jun Ling, Xufeng Ni
Summary: This study reports the successful synthesis of a copolymer of 2-methyltetrahydrofuran (2-MeTHF) and beta-butyrolactone (BBL) through Sc(OTf)(3)-catalysed cationic ring-opening copolymerization. The possibility of copolymerization was verified by density functional theory (DFT) calculations. The obtained copolymer, poly(2-MeTHF-co-BBL), showed promising properties and potential as an environmentally friendly material.
Article
Nanoscience & Nanotechnology
Kai Hao, Ronglu Cui, Lifeng Fang, Jun Ling, Baoku Zhu
Summary: In this study, a neutral surface of polysarcosine (PSar), a hydrophilic polypeptoid, was successfully synthesized and modified to enhance its compatibility with water, reduce protein adsorption and cytotoxicity, and demonstrate good hemocompatibility and antifouling properties.
ACS APPLIED MATERIALS & INTERFACES
(2023)
Article
Polymer Science
Siqi Wang, Tianlun Shen, Kai Hao, Xinfeng Tao, Jihong Sun, Jun Ling
Summary: Hyperbranched poly(a-amino acid)s have attracted attention for their biocompatibility, degradability, and bioactivity. Unique polymerization reactions of di-NNPC resulted in hyperbranched polypeptoids instead of gels. The molecular weights of the hyperbranched polypeptoids were controlled by tuning the initial concentrations of monomer and basic catalyst. The residual glycine pendant groups on the polymer chains were used for Gd3+ complexation and post-modification, making the hyperbranched polypeptoids multifunctional single molecular micelles applicable as contrast agents and probes in magnetic resonance imaging and photoluminescence.
MACROMOLECULAR CHEMISTRY AND PHYSICS
(2023)
Review
Polymer Science
Ting Shen, Kaihao Chen, Yougen Chen, Jun Ling
Summary: To address the plastic waste crisis, there are efforts to develop sustainable polymer materials that can degrade through disposing and decomposing to small molecules (DDM) or via chemical recycling to monomers (CRM). Polyacetals, a type of pH-responsive polymers, can degrade under acidic conditions but remain stable under neutral and basic conditions. Their synthesis through cationic ring-opening polymerization (CROP) has challenges but recent advancements in CRM have renewed interest in this method. Polyacetals offer recyclable materials with DDM and CRM potential, expanding closed-loop recycling options and improving degradation properties of traditional polyesters and polyolefins.
MACROMOLECULAR RAPID COMMUNICATIONS
(2023)
Article
Multidisciplinary Sciences
Jie Zhang, Tianwen Bai, Weixi Liu, Mingzhao Li, Qiguang Zang, Canbin Ye, Jing Zhi Sun, Yaocheng Shi, Jun Ling, Anjun Qin, Ben Zhong Tang
Summary: High refractive index polymers (HRIPs) with excellent optical transparency are prepared by using organobase catalyzed polymerization. The HRIPs exhibit high refractive indices, high molecular weights, and low propagation loss. The polymers also have aggregation-induced emission feature for monitoring the uniformity and continuity of optical waveguides.
NATURE COMMUNICATIONS
(2023)
Review
Chemistry, Multidisciplinary
Kaihao Chen, Yixuan Mei, Zhuorui Zhang, Jun Ling, Xufeng Ni
Summary: As a substituted-delta-valerolactone, alpha-ethylidene-delta-vinyl-delta-valerolactone (EVL) offers a method to utilize carbon dioxide and 1,3-butadiene in producing functional polymers. Recent successful attempts in polymerizing EVL have led to the development of novel synthetic strategies and functional polymers. This review highlights the ring-opening reactions of EVL and its derivatives, as well as the ring-opening (co)polymerizations, showcasing the unique properties of the obtained functional polymers and their application potential in various fields.
Article
Polymer Science
Jianping Wang, Peng Zhou, Ting Shen, Songyi Xu, Tianwen Bai, Jun Ling
Summary: This study developed a novel method to synthesize glycine-rich poly-(amino acid)-s (PAAs) through controlled ring-opening copolymerization. The synthesized copolymers exhibited predictable molecular weights and tunable glycine incorporation, and could form nanoparticles or hydrogel in water. The beta-sheet folding of poly-(Gly-r-Lys) remained intact in a neutral environment. This strategy opens up new possibilities for engineering glycine-rich PAAs and expanding their applications.
Article
Materials Science, Biomaterials
Shangyu Chen, Peng Zhou, Wan Yang, Danni Hu, Pengfei Chen, Pengfei Sun, Jun Ling, Quli Fan
Summary: In this study, a modified near-infrared II (NIR-II) small-molecule-based polymer was prepared for efficient breast cancer pulmonary metastasis imaging. The polymer showed good solubility, high fluorescence quantum yield, and prolonged blood circulation half-life, and demonstrated better tumor accumulation capability even at low dye concentration. The successful use of this polymer in noninvasive NIR-II fluorescence imaging for breast cancer pulmonary metastasis was demonstrated.
BIOMATERIALS SCIENCE
(2023)
Article
Nanoscience & Nanotechnology
Huiyang Wang, Siqi Wang, Xisong Zhu, Wenxiu Ding, Tianlun Shen, Hongjie Fan, Yanhua Zhang, Lijun Peng, Hong Yuan, Xiangrui Liu, Jun Ling, Jihong Sun
Summary: In this study, an iron-based solid lipid nanoparticle (SLN) was developed, which can be absorbed by the intestinal wall and enhance contrast in MRI. Experimental results using mouse models showed that the SLN has better diagnostic value for acute ulcerative colitis and colon adenocarcinoma. Confocal fluorescence microscopy confirmed that the SLN mainly distributes in the intestinal mucosa and tumor capsule.
INTERNATIONAL JOURNAL OF NANOMEDICINE
(2022)
