Angewandte Chemie最新文献

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Selenium-Substitution Strategy for Enhanced Mobility, Tunable Bandgap, and Improved Electrochemical Energy Storage in Semiconducting Conjugated Coordination Polymers
Angewandte Chemie Pub Date : 2025-01-21 DOI: 10.1002/ange.202419865
Sha Wu, Dr. Xing Huang, Dr. Shuai Fu, Ze Li, Siping Yin, Wenkai Liao, Dr. Mingchao Wang, Dr. Yang Lu, Prof. Mischa Bonn, Dr. Yimeng Sun, Prof. Xinliang Feng, Prof. Wei Xu
{"title":"Selenium-Substitution Strategy for Enhanced Mobility, Tunable Bandgap, and Improved Electrochemical Energy Storage in Semiconducting Conjugated Coordination Polymers","authors":"Sha Wu,&nbsp;Dr. Xing Huang,&nbsp;Dr. Shuai Fu,&nbsp;Ze Li,&nbsp;Siping Yin,&nbsp;Wenkai Liao,&nbsp;Dr. Mingchao Wang,&nbsp;Dr. Yang Lu,&nbsp;Prof. Mischa Bonn,&nbsp;Dr. Yimeng Sun,&nbsp;Prof. Xinliang Feng,&nbsp;Prof. Wei Xu","doi":"10.1002/ange.202419865","DOIUrl":"https://doi.org/10.1002/ange.202419865","url":null,"abstract":"<p>Conjugated coordination polymers (c-CPs), a novel class of organic–inorganic hybrid materials, are distinguished by their unique structural characteristics and exceptional charge transport properties. The electronic properties of these materials are critically determined by the constituting coordination atoms, with electron-rich selenol ligands emerging as promising candidates for constructing high-mobility semiconducting c-CPs. Despite their potential, c-CPs incorporating selenium-substituted ligands remain scarce due to the synthetic challenges associated with both the ligands and the coordination polymers. In this study, we successfully synthesized a new tetraselenol-hydroxyquinone (TSHQ) ligand using a “4+2” design strategy and developed a semiconducting three-dimensional Ag−Se coordination polymer, Ag<sub>4</sub>TSHQ. Ag<sub>4</sub>TSHQ exhibits room-temperature electrical conductivity of up to 1.6 S/m and shares the same structural topology as Ag<sub>4</sub>TTHQ (TTHQ=tetrathiol-hydroxyquinone), enabling precise band gap modulation from 0.6 eV to 1.5 eV via a mixed-ligand approach. Time-resolved terahertz spectroscopy reveals that the charge mobility of Ag<sub>4</sub>TSHQ in the dc limit is ~350 cm<sup>2</sup>/V ⋅ s, which is twice that of its sulfur counterpart, Ag<sub>4</sub>TTHQ. Furthermore, our evaluations of their electrochemical energy storage capabilities demonstrate that Ag<sub>4</sub>TSHQ effectively utilizes its redox potential, achieving a remarkable specific capacitance of up to 340 F/g-significantly outperforming Ag<sub>4</sub>TTHQ, which has a capacitance of 294 F/g. These findings underscore the potential of selenium-ligand-based c-CPs for optoelectronic applications and energy storage technologies.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 9","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-21","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143475275","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Remote Hydrogen Bonding between Ligand and Substrate Accelerates C–H Bond Activation and Enables Switchable Site Selectivity
Angewandte Chemie Pub Date : 2025-01-20 DOI: 10.1002/ange.202419144
Dr. Pinaki Bhusan De, Dr. Kazuhiro Okamoto, Jayakumar Sekar, Dr. Sobi Asako, Dr. Laurean Ilies
{"title":"Remote Hydrogen Bonding between Ligand and Substrate Accelerates C–H Bond Activation and Enables Switchable Site Selectivity","authors":"Dr. Pinaki Bhusan De,&nbsp;Dr. Kazuhiro Okamoto,&nbsp;Jayakumar Sekar,&nbsp;Dr. Sobi Asako,&nbsp;Dr. Laurean Ilies","doi":"10.1002/ange.202419144","DOIUrl":"https://doi.org/10.1002/ange.202419144","url":null,"abstract":"<p>Transition-metal-catalyzed selective and efficient activation of an inert C−H bond in an organic substrate is of importance for the development of streamlined synthetic methodologies. An attractive approach is the design of a metal catalyst capable of recognizing an organic substrate through noncovalent interactions to control reactivity and selectivity. We report here a spirobipyridine ligand that bears a hydroxy group which recognizes pyridine and quinoline substrates through hydrogen bonding, and in combination with an iridium catalyst enables site-selective C−H borylation. The site selectivity can be switched by simply changing the position of the hydroxy group on the ligand. The catalyst also accelerates the reactions, overrides steric bias, and selectively recognizes a pyridine substrate in the presence of other hydrogen bond acceptors. These features are reminiscent of enzymatic catalysis and suggest that judicious design of the recognition group on the ligand can become a general strategy to selectively and efficiently functionalize organic substrates.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 8","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143431816","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Reprocessable and Recyclable Materials for 3D Printing via Reversible Thia-Michael Reactions
Angewandte Chemie Pub Date : 2025-01-20 DOI: 10.1002/ange.202423522
Dr. Yong-Liang Su, Dr. Liang Yue, McKinley K. Paul, Dr. Joseph Kern, Kaitlyn S. Otte, Prof. Rampi Ramprasad, Prof. H. Jerry Qi, Prof. Will R. Gutekunst
{"title":"Reprocessable and Recyclable Materials for 3D Printing via Reversible Thia-Michael Reactions","authors":"Dr. Yong-Liang Su,&nbsp;Dr. Liang Yue,&nbsp;McKinley K. Paul,&nbsp;Dr. Joseph Kern,&nbsp;Kaitlyn S. Otte,&nbsp;Prof. Rampi Ramprasad,&nbsp;Prof. H. Jerry Qi,&nbsp;Prof. Will R. Gutekunst","doi":"10.1002/ange.202423522","DOIUrl":"https://doi.org/10.1002/ange.202423522","url":null,"abstract":"<p>The development of chemically recyclable polymers for sustainable 3D printing is crucial to reducing plastic waste and advancing towards a circular polymer economy. Here, we introduce a new class of polythioenones (PCTE) synthesized via Michael addition-elimination ring-opening polymerization (MAEROP) of cyclic thioenone (CTE) monomers. The designed monomers are straightforward to synthesize, scalable and highly modular, and the resulting polymers display mechanical performance superior to commodity polyolefins such as polyethylene and polypropylene. The material was successfully employed in 3D printing using fused-filament fabrication (FFF), showcasing excellent printability and mechanical recyclability. Notably, PCTE−Ph retains its tensile strength and thermal stability after multiple mechanical recycling cycles. Furthermore, PCTE−Ph can be depolymerized back to its original monomer with a 90 % yield, allowing for repolymerization and establishing a successful closed-loop life cycle, making it a sustainable alternative for additive manufacturing applications.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 8","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202423522","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143431815","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Cu(I)-Induced G-Quartets: Robust Supramolecular Polymers Exhibiting Heating-Induced Aqueous Phase Transitions Into Gel or Precipitate
Angewandte Chemie Pub Date : 2025-01-20 DOI: 10.1002/ange.202417508
Nihar Sahu, Chandrakanta Guchhait, Indrajit Mohanta, Vembanan Suriyaa, Dr. Bimalendu Adhikari
{"title":"Cu(I)-Induced G-Quartets: Robust Supramolecular Polymers Exhibiting Heating-Induced Aqueous Phase Transitions Into Gel or Precipitate","authors":"Nihar Sahu,&nbsp;Chandrakanta Guchhait,&nbsp;Indrajit Mohanta,&nbsp;Vembanan Suriyaa,&nbsp;Dr. Bimalendu Adhikari","doi":"10.1002/ange.202417508","DOIUrl":"https://doi.org/10.1002/ange.202417508","url":null,"abstract":"<p>Certain proteins and synthetic covalent polymers experience aqueous phase transitions, driving functional self-assembly. Herein, we unveil the ability of supramolecular polymers (SPs) formed by G<sub>4</sub>.Cu<sup>+</sup> to undergo heating-induced unexpected aqueous phase transitions. For the first time, guided by Cu<sup>+</sup>, guanosine (G) formed a highly stable G-quartet (G<sub>4</sub>.Cu<sup>+</sup>)/G-quadruplex as a non-canonical DNA secondary structure with temperature tolerance, distinct from the well-known G<sub>4</sub>.K<sup>+</sup>. The G<sub>4</sub>.Cu<sup>+</sup> self-assembled in water through π-π stacking, metallophilic and hydrophobic interactions, forming thermally robust SPs. This enhanced stability is attributed to the stronger coordination of Cu<sup>+</sup> to four carbonyl oxygens of G-quartet and the presence of Cu<sup>+</sup>- - -Cu<sup>+</sup> attractive metallophilic interactions in Cu<sup>+</sup>-induced G-quadruplex, exhibiting a significantly higher interaction energy than K<sup>+</sup> as determined computationally. Remarkably, the aqueous SP solution exhibited heating-induced phase transitions—forming a hydrogel through dehydration-driven crosslinking of SPs below cloud temperature (<i>T</i><sub>cp</sub>) and a hydrophobic collapse-induced solid precipitate above <i>T</i><sub>cp</sub>, showcasing a lower critical solution temperature (LCST) behavior. Notably, this LCST behavior of G<sub>4</sub>.Cu<sup>+</sup> SP originates from biomolecular functionality rather than commonly exploited thermo-responsive oligoethylene glycols with supramolecular assemblies. Furthermore, exploiting the redox reversibility of Cu<sup>+</sup>/Cu<sup>2+</sup>, we demonstrated control over the assembly and disassembly of G-quartets/G-quadruplex and gelation reversibly.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 9","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143475351","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Isoreticular Tolerance and Phase Selection in the Synthesis of Multi-Module Metal–Organic Frameworks for Gas Separation and Electrocatalytic OER
Angewandte Chemie Pub Date : 2025-01-20 DOI: 10.1002/ange.202422635
Dr. Yuchen Xiao, Prof. Xianhui Bu, Prof. Pingyun Feng
{"title":"Isoreticular Tolerance and Phase Selection in the Synthesis of Multi-Module Metal–Organic Frameworks for Gas Separation and Electrocatalytic OER","authors":"Dr. Yuchen Xiao,&nbsp;Prof. Xianhui Bu,&nbsp;Prof. Pingyun Feng","doi":"10.1002/ange.202422635","DOIUrl":"https://doi.org/10.1002/ange.202422635","url":null,"abstract":"<p>Although metal–organic frameworks are coordination-driven assemblies, the structural prediction and design using metal-ligand interactions can be unreliable due to other competing interactions. Leveraging non-coordination interactions to develop porous assemblies could enable new materials and applications. Here, we use a multi-module MOF system to explore important and pervasive impact of ligand-ligand interactions on metal-ligand as well as ligand-ligand co-assembly process. It is found that ligand-ligand interactions play critical roles on the scope or breakdown of isoreticular chemistry. With cooperative di- and tri-topic ligands, a family of Ni-MOFs has been synthesized in various structure types including partitioned MIL-88-acs (<i>pacs</i>), interrupted <i>pacs</i> (i-<i>pacs</i>), and UMCM-1-muo. A new type of isoreticular chemistry on the muo platform is established between two drastically different chemical systems. The gas sorption and electrocatalytic studies were performed that reveal excellent performance such as high C<sub>2</sub>H<sub>2</sub>/CO<sub>2</sub> selectivity of 21.8 and high C<sub>2</sub>H<sub>2</sub> uptake capacity of 114.5 cm<sup>3</sup>/g at 298 K and 1 bar.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 8","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143431817","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Enzyme-Inspired Single Selenium Site for Selective Oxygen Reduction
Angewandte Chemie Pub Date : 2025-01-20 DOI: 10.1002/ange.202418897
Dr. Peng-Yang Zhang, Dr. Xia Xu, Dr. Wen-Song Yu, Prof. Zhi-Yao Duan, Prof. Huan Huang, Prof. Tao Wang, Prof. Gang Fu, Prof. Zhi-You Zhou, Yu-Cheng Wang, Prof. Shi-Gang Sun
{"title":"Enzyme-Inspired Single Selenium Site for Selective Oxygen Reduction","authors":"Dr. Peng-Yang Zhang,&nbsp;Dr. Xia Xu,&nbsp;Dr. Wen-Song Yu,&nbsp;Prof. Zhi-Yao Duan,&nbsp;Prof. Huan Huang,&nbsp;Prof. Tao Wang,&nbsp;Prof. Gang Fu,&nbsp;Prof. Zhi-You Zhou,&nbsp;Yu-Cheng Wang,&nbsp;Prof. Shi-Gang Sun","doi":"10.1002/ange.202418897","DOIUrl":"https://doi.org/10.1002/ange.202418897","url":null,"abstract":"<p>Learning from nature has garnered significant attention in the scientific community for its potential to inspire creative solutions in material or catalyst design. The study highlights the design of a biomimetic single selenium (Se) site-modified carbon (C) moiety that retains the unique reactivity of selenoenzyme with peroxides, which plays crucial roles in selectively catalyzing the oxygen reduction reaction (ORR). The as-designed Se−C demonstrates nearly 100 % 4-electron selectivity, evidenced by 0.039 % of H<sub>2</sub>O<sub>2</sub> yield at 0.5 V versus reversible hydrogen electrode, outperforming commercial platinum (Pt) by 65 times. In situ X-ray absorption spectroscopy and theoretical calculations attribute this exceptional selectivity to the enzyme-like behaviors of the Se site to steal an O atom from peroxide intermediates. The second achievement is the significantly increased consecutive 2+2 electron selectivity. Benefiting from the enzyme-like H<sub>2</sub>O<sub>2</sub> reduction activity with a higher onset potential of 0.915 V compared to Pt at 0.875 V, the Se−C as a secondary catalytic site reduced the H<sub>2</sub>O<sub>2</sub> yields of the Co−N−C, Fe−N−C, and N−C catalysts by 96 %, 67 %, and 98 %, respectively, via a consecutive 2+2 electron pathway. This also leads to more stable catalysts via protecting the active sites from oxidative attacks. This work establishes new pathways for precise tuning of reaction selectivity in ORR and beyond.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 8","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143431818","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
Precise Tailoring of Unprecedent Layered Perovskite-Type Heterostructure Ferroelectric via Chemical Molecular Scissor
Angewandte Chemie Pub Date : 2025-01-20 DOI: 10.1002/ange.202424279
Yu Ma, Wenjing Li, Yi Liu, Wuqian Guo, Haojie Xu, Liwei Tang, Qingshun Fan, Hao Rong, Prof. Junhua Luo, Prof. Zhihua Sun
{"title":"Precise Tailoring of Unprecedent Layered Perovskite-Type Heterostructure Ferroelectric via Chemical Molecular Scissor","authors":"Yu Ma,&nbsp;Wenjing Li,&nbsp;Yi Liu,&nbsp;Wuqian Guo,&nbsp;Haojie Xu,&nbsp;Liwei Tang,&nbsp;Qingshun Fan,&nbsp;Hao Rong,&nbsp;Prof. Junhua Luo,&nbsp;Prof. Zhihua Sun","doi":"10.1002/ange.202424279","DOIUrl":"https://doi.org/10.1002/ange.202424279","url":null,"abstract":"<p>Precise stacking of distinct two-dimensional (2D) rigid slabs to build heterostructures has renewed the portfolio of 2D materials, e.g., magic-angle graphene, due to the emergence of exotic physical properties. Recently, single-crystal heterostructures of layered perovskites have emerged as an exciting branch, while it remains scarce to achieve strong ferroelectricity in this new heterostructure family. Here, we present the first ferroelectric of 2D perovskite heterostructures as single crystal, (EA<sub>3</sub>Pb<sub>2</sub>Br<sub>7</sub>)EA<sub>4</sub>Pb<sub>3</sub>Br<sub>10</sub> (<b>1</b>, EA=ethylamine), by precisely tailoring inorganic sheets via <i>a</i> chemical molecular scissor. It has notable ferroelectricity of large spontaneous polarization (<i>P</i><sub>s</sub>~5.0 μC/cm<sup>2</sup>) and high Curie temperature (<i>T</i><sub>c</sub>~375 K). Structurally, its inorganic framework adopts a unique 2D heterostructure that contains two different rigid slabs of {EA<sub>3</sub>Pb<sub>2</sub>Br<sub>7</sub>}<sub>n</sub> and {EA<sub>4</sub>Pb<sub>3</sub>Br<sub>10</sub>}<sub>n</sub>. This motif is self-assembled by layer-by-layer clipping of rigid prototype sheets, using extra neopentylamine as a molecular chemical scissor. Unlike epitaxial growth, such a molecule-level stacking facilitates the growth of heterostructure single crystals. Combining its strong ferroelectricity and inherent anisotropy, crystal-based device of <b>1</b> exhibits an ultrahigh polarized-light sensitivity up to ~37 in self-powered mode, being the highest level of 2D perovskite ferroelectric family. Our work will facilitate the further development of ferroelectric materials for optoelectronic device applications.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 9","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143475389","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
The Interplay of Methylidyne and Carbido Species: Modeling a Fundamental Step in the Fischer–Tropsch Synthesis
Angewandte Chemie Pub Date : 2025-01-20 DOI: 10.1002/ange.202424699
Dr. Liam K. Burt, Prof. Dr. Anthony F. Hill
{"title":"The Interplay of Methylidyne and Carbido Species: Modeling a Fundamental Step in the Fischer–Tropsch Synthesis","authors":"Dr. Liam K. Burt,&nbsp;Prof. Dr. Anthony F. Hill","doi":"10.1002/ange.202424699","DOIUrl":"https://doi.org/10.1002/ange.202424699","url":null,"abstract":"<p>Heterobimetallic μ-methylidyne complexes [WPt(μ<sub>2</sub>-CH)(CO)<sub>2</sub>L<sub>2</sub>(Tp*)], where L<sub>2</sub>=(PPh<sub>3</sub>)<sub>2</sub>, (PPh<sub>3</sub>)(CO), (dppe), (PPh<sub>3</sub>)(CNC<sub>6</sub>H<sub>2</sub>Me<sub>3</sub>), have been obtained via the intermediacy of transient hydrido-μ-carbido complexes that undergo carbido-hydrido coupling to model a fundamental step in the proposed mechanism for Fischer–Tropsch synthesis.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 9","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/ange.202424699","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143475390","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
A Regio- and Stereoselective Ring-Opening Polymerization Approach to Isotactic Alternating Poly(lactic-co-glycolic acid) with Stereocomplexation
Angewandte Chemie Pub Date : 2025-01-20 DOI: 10.1002/ange.202422147
Yu-Ting Huang, Hao-Yi Huang, Jing-Liang Cheng, Min Xie, Prof. Liang-Wen Feng, Prof. Zhongzheng Cai, Prof. Jian-Bo Zhu
{"title":"A Regio- and Stereoselective Ring-Opening Polymerization Approach to Isotactic Alternating Poly(lactic-co-glycolic acid) with Stereocomplexation","authors":"Yu-Ting Huang,&nbsp;Hao-Yi Huang,&nbsp;Jing-Liang Cheng,&nbsp;Min Xie,&nbsp;Prof. Liang-Wen Feng,&nbsp;Prof. Zhongzheng Cai,&nbsp;Prof. Jian-Bo Zhu","doi":"10.1002/ange.202422147","DOIUrl":"https://doi.org/10.1002/ange.202422147","url":null,"abstract":"<p>Poly(lactic-<i>co</i>-glycolic acid) (PLGA) has been widely employed for various biomedical applications owing to its biodegradability and biocompatibility. The discovery of the stereocomplex formation between enantiomeric alternating PLGA pairs underscored its potential as high-performance biodegradable materials with diverse material properties and biodegradability. Herein, we have established a regio- and stereoselective ring-opening polymerization approach for the synthesis of stereocomplexed isoenriched alternating PLGA from racemic methyl-glycolide (<i>rac</i>-MG). The high sequence and tacticity control was accomplished by an optimized enantiopure scandium catalyst bearing a spiro-salen scaffold. Varying polymer stereoregularity <i>P</i><sub>m</sub> from 0.4 to 0.91 led to a transformation of the resulting alternating PLGA from amorphous to semicrystalline materials. Notably, the stereocomplexed alternating PLGA demonstrated enhanced melting transition temperature (<i>T</i><sub>m</sub> up to 191 °C) and crystallization rate. This regio- and stereocontrolled polymerization represented a versatile approach for the preparation of high-performance biodegradable PLGA materials.</p>","PeriodicalId":7803,"journal":{"name":"Angewandte Chemie","volume":"137 9","pages":""},"PeriodicalIF":0.0,"publicationDate":"2025-01-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143475499","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
引用次数: 0
pH-responsive Polyglycerol-Nanogele zur Behandlung von Parodontitis durch antibakterielle und pro-angiogenetische Wirkung
Angewandte Chemie Pub Date : 2025-01-19 DOI: 10.1002/ange.202418882
Guoxin Ma, Ke Xu, Prof. Dr. Leixiao Yu, Prof. Dr. Rainer Haag
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