Yuying Wang, Jibin Wang, Xiaoyan Ding, Xinjun Yu, Yudan Zhao, Zhengxuan Pan, Longwu Xu, Wenchang Cheng, Meng Ji, Chuanming Yuan*, Tao Wang* and Baolong Zhou*,
{"title":"“Bacterial Suicide”: An Aminal-Linked Covalent Organic Polymer with Infection-Microenvironment-Enhanced Synergistic Photothermal and Enzymatic Activities for Wound Therapy","authors":"Yuying Wang, Jibin Wang, Xiaoyan Ding, Xinjun Yu, Yudan Zhao, Zhengxuan Pan, Longwu Xu, Wenchang Cheng, Meng Ji, Chuanming Yuan*, Tao Wang* and Baolong Zhou*, ","doi":"10.1021/acsapm.4c0260710.1021/acsapm.4c02607","DOIUrl":"https://doi.org/10.1021/acsapm.4c02607https://doi.org/10.1021/acsapm.4c02607","url":null,"abstract":"<p >The infected microenvironment provides fertile ground for bacterial growth and the progression of inflammation, making it challenging to cure related diseases. Here, a covalent organic polymer (COP)-based antibacterial agent, denoted as PF-COP, was developed. PF-COP has intrinsic photothermal capacity, which allows it to take advantage of the infected microenvironment for enhanced synergistic wound infection therapy. PF-COP was prepared via the copolymerization of piperazine with ferrocene diformaldehyde using catalyst-free aminal chemistry, in which the piperazine units could easily bind with acid to generate the cationic skeleton, while the ferrocene components could convert the endogenous H<sub>2</sub>O<sub>2</sub> into a toxic hydroxyl radical. This effectively regulates the infection of the microenvironment. The acidified positively charged structures could enhance material adhesion with bacterial cell membranes and improve photothermal responsiveness, significantly improving the therapeutic effect. As a result, PF-COP amalgamating photothermal and enzyme catalytic capacities could serve as an infection microenvironment-enhanced therapeutic agent. It could disrupt the balance of the infection microenvironment, destroying the optimal growth environment for bacteria and inducing “bacterial suicide”, and regulate the microenvironment to promote the growth of normal cells, thus accelerating the wound healing. Therefore, this work presents a promising construction strategy for the precise development of COP-based therapeutics facilitating wound healing through direct infectious microenvironment utilization and regulation.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"6 22","pages":"13764–13774 13764–13774"},"PeriodicalIF":4.4,"publicationDate":"2024-11-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142691551","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Wonyong Choi, Brian Chaplin, Fan Dong, Jingyun Fang, Jaehong Kim, Margaret Mills* and Rob Nerenberg,
{"title":"Recognizing Excellence in Environmental Engineering Research: The 2023 ACS ES&T Engineering’s Best Paper Awards","authors":"Wonyong Choi, Brian Chaplin, Fan Dong, Jingyun Fang, Jaehong Kim, Margaret Mills* and Rob Nerenberg, ","doi":"10.1021/acsestengg.4c0071910.1021/acsestengg.4c00719","DOIUrl":"https://doi.org/10.1021/acsestengg.4c00719https://doi.org/10.1021/acsestengg.4c00719","url":null,"abstract":"","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"4 11","pages":"2585–2586 2585–2586"},"PeriodicalIF":7.4,"publicationDate":"2024-11-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142608302","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Kexin Chen, Aman Liu, Xiaojing Zhang, Jianxiong Hu, Jian Li, Qiang Ren and Chenyi Wang*,
{"title":"Highly Stable Poly(diphenyl sulfide piperidine) Anion Exchange Membrane Grafting with Flexible Side-Chain Cationic Group for Water Electrolysis","authors":"Kexin Chen, Aman Liu, Xiaojing Zhang, Jianxiong Hu, Jian Li, Qiang Ren and Chenyi Wang*, ","doi":"10.1021/acsapm.4c0297710.1021/acsapm.4c02977","DOIUrl":"https://doi.org/10.1021/acsapm.4c02977https://doi.org/10.1021/acsapm.4c02977","url":null,"abstract":"<p >Aryl-piperidine polymers are preferred for anion exchange membranes (AEMs) due to their excellent designability and alkaline resistance stability. In the present work, a poly(diphenyl sulfide piperidine) polymer backbone, distinct from the conventional poly(biphenyl piperidine), is synthesized via a superacid-catalyzed reaction. Subsequently, a series of AEMs (PPSP-<i>x</i>Pip) are achieved by grafting cationic groups with long flexible alkyl chains onto the main chain. All membranes demonstrate good membrane-forming ability and toughness with elongation at break ranging from 16.8 to 34.5%. The OH<sup>–</sup> conductivity of them is in the range of 88.4–117.1 mS cm<sup>–1</sup> at 80 °C, attributed to the high water uptake and the favorable microphase separation structure. The representative PPSP-35Pip membrane exhibits high alkaline stability with 89% of the conductivity retention ratio in 2 M NaOH after 520 h at 80 °C. The current density of its water electrolyzer cell reaches 0.619 A cm<sup>–2</sup> in 2 M NaOH electrolyte at 2.0 V. After 520 h of endurance testing, the water electrolyzer maintains excellent stability with the voltage fluctuation of only 1.07%.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"6 22","pages":"13937–13948 13937–13948"},"PeriodicalIF":4.4,"publicationDate":"2024-11-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142694476","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ruan R. Henriques, Gabriel Perli, Bluma G. Soares, Jannick Duchet-Rumeau and Sebastien Livi*,
{"title":"The Next Generation of Recyclable Epoxy-anhydride Networks Combining Metallic Ionic Liquid (MIL) and Epoxidized IL-Based Monomers","authors":"Ruan R. Henriques, Gabriel Perli, Bluma G. Soares, Jannick Duchet-Rumeau and Sebastien Livi*, ","doi":"10.1021/acsapm.4c0296510.1021/acsapm.4c02965","DOIUrl":"https://doi.org/10.1021/acsapm.4c02965https://doi.org/10.1021/acsapm.4c02965","url":null,"abstract":"<p >According to the political and ethical demands of our times, scholars and industries are pushed to search for sustainable solutions, i.e., to design recyclable, reusable, or degradable materials. The challenge is to go beyond conventional epoxy networks based on visphenol A diglycidyl ether (DGEBA), which firstly contain bisphenol A (BPA) and secondly cannot be recycled. Here, a generation of recyclable epoxy thermosets was designed and developed for the first time from the copolymerization between tri- and tetra-IL based monomers containing cleavable bonds with conventional anhydride (MTHPA) with our without the presence of a metallic ionic liquid (MIL). Thus, the influence of these monomers and the MIL on the curing kinetics, the epoxy conversion, and the physical properties of the resulting networks was assessed. In particular, the combination of the two has proved to be a powerful tool to tailor the architecture–physical property relationships of the resulting IL-modified epoxy networks and to produce recyclable networks. As a consequence, the glass transition temperature <i>T</i><sub>g</sub> of the networks ranged from 60 to 140 °C, while the mechanical performances varied from 2.5 to 3.5 GPa, combined with a thermal stability up to 330 °C. Then, the epoxy networks were subjected to physical recycling (a solvent-free method, i.e., hot-pressed process) and a chemical recycling process using dissolution in ethylene glycol and repolymerization at 150 °C. Finally, all the epoxy networks showed their ability to be recycled, which was highly dependent on the network architecture.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"6 22","pages":"13916–13926 13916–13926"},"PeriodicalIF":4.4,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142692162","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Chemical Surface Metallization for Elastomers with Biphasic Liquid Metals","authors":"Yang Gu, Zixun Chen and Yan Peng*, ","doi":"10.1021/acsapm.4c0238410.1021/acsapm.4c02384","DOIUrl":"https://doi.org/10.1021/acsapm.4c02384https://doi.org/10.1021/acsapm.4c02384","url":null,"abstract":"<p >Growing interest has been received in lightweight, cost-effective, and easily processable conductive materials with the rapid development of wearable electronics, smart robotics, and bioengineering. Flexible polymer metallization is the most prevalent method to inherit the merits of both metals and elastomers. This work explores and optimizes the metallization process and successfully fabricates a three-layer flexible conductive material through electroless copper plating and gallium electroplating on the surface of elastomers. The material obtained in this work exhibits strong adhesion between the coating layer and soft polymer (peel strength: 1.52 N/mm), considerable stretchability (elongation at break: 507%), high electrical conductivity (3.11 × 10<sup>4</sup> S/m), and outstanding electromechanical stability (2000 cycles). Interestingly, the integration with photolithography enabled selective metallization on specific regions of the elastomer substrate, providing applications in flexible and intelligent devices. This work contributes to the advancement of surface treatment technologies based on the combination of metals and elastomers, which is beneficial for diverse advanced technologies including E-skin, wearable electronics, microelectronics, and nanotechnology.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"6 22","pages":"13681–13689 13681–13689"},"PeriodicalIF":4.4,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142691321","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Qi Jiang, Han Hu*, Qingyang Luan, Hanxu Zhu, Jinggang Wang* and Jin Zhu,
{"title":"High Impact, Heat-Resistant, and Chemically Recyclable PEF Copolyester for Sustainable Transparent Packaging","authors":"Qi Jiang, Han Hu*, Qingyang Luan, Hanxu Zhu, Jinggang Wang* and Jin Zhu, ","doi":"10.1021/acsapm.4c0299310.1021/acsapm.4c02993","DOIUrl":"https://doi.org/10.1021/acsapm.4c02993https://doi.org/10.1021/acsapm.4c02993","url":null,"abstract":"<p >Poly(ethylene 2,5-furandicarboxylate) (PEF) is a type of biobased polyester with a high gas barrier, which has the potential to replace polyethylene terephthalate (PET). In view of the poor toughness of PEF, an innovative attempt was made to install a small amount of 2,5-thiophenedicarboxylic acid (TDCA) into the PEF backbone and synthesize the poly(ethylene furandicarboxylate-<i>co</i>-thiophenedicarboxylate) (PEFS-n) copolyester. The obtained PEFS-n demonstrates thermal stability and glass transition temperature (<i>T</i><sub>g</sub>) comparable to that of PEF. Additionally, the tensile properties of PEFS-n exhibit appreciable enhancements. The impact strength of PEFS-n exhibited a markedly higher value than that of PEF, particularly in the case of PEFS-5, which displays a 138% increase in impact strength. Concurrently, PEFS-n exhibits enhanced barrier characteristics (oxygen, carbon dioxide, and water) than PET, in addition to outstanding solvent resistance and transparency. After 4 h of hydrolysis in alkaline solutions at 80 °C, subsequently simply washing and filtering, more than 90% of FDCA monomer could be recovered. This work provides a direction for high impact and heat-resistant green packaging, as sustainable alternatives to PET.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"6 22","pages":"13949–13956 13949–13956"},"PeriodicalIF":4.4,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142691254","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Wenzhao Xiong, Cuifen Zhang, Shenbo Zhu, Wenting Liang, Zhibo Wang, Guangye Zhang, Zaifei Ma and Huawei Hu*,
{"title":"Precision Fluorine Functionalization in Alkyl Side Chains of Polymer Donors for Highly Efficient Organic Solar Cells","authors":"Wenzhao Xiong, Cuifen Zhang, Shenbo Zhu, Wenting Liang, Zhibo Wang, Guangye Zhang, Zaifei Ma and Huawei Hu*, ","doi":"10.1021/acsapm.4c0254210.1021/acsapm.4c02542","DOIUrl":"https://doi.org/10.1021/acsapm.4c02542https://doi.org/10.1021/acsapm.4c02542","url":null,"abstract":"<p >Fluorination of polymer donors has demonstrated considerable potential for boosting the performance of organic solar cells (OSCs). However, achieving optimal performance requires careful management of fluorine levels, as excessive fluorination may adversely affect device efficiency. In this study, we introduce a controlled number of fluorine atoms into the alkyl side chains of polymer donors to optimize their temperature-dependent aggregation and intermolecular interactions. Four polymers (PTF0, PTF1, PTF2, and PTF3) with reduced synthetic complexity and varying levels of fluorine incorporation were synthesized, allowing precise control over their optoelectronic properties. Notably, PTF1, featuring a single fluorine atom, effectively tunes the energy levels and promotes beneficial intermolecular interactions with the corresponding nonfullerene acceptor. Moreover, PTF1 demonstrates enhanced aggregation and crystallinity, leading to efficient charge generation and transport, resulting in binary and ternary OSCs with PCEs of 13.0% and 18.6%, respectively. This study suggests the potential of precise fluorine functionalization in polymer donors as a potent strategy for crafting highly efficient OSCs and provides valuable insights for designing next-generation OSC materials, paving the way for future advancements.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"6 22","pages":"13735–13743 13735–13743"},"PeriodicalIF":4.4,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142685196","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Aanchal Jaisingh, Matthew W. Halloran, Bhausaheb S. Rajput, Robert J. Chambers, Jaysen Reindel, Katherine A. O’Shea, Shengqiang Cai and Michael D. Burkart*,
{"title":"Correction to “Tailoring High Hardness and Rigidity in Biodegradable Thermoplastic Polyurethanes”","authors":"Aanchal Jaisingh, Matthew W. Halloran, Bhausaheb S. Rajput, Robert J. Chambers, Jaysen Reindel, Katherine A. O’Shea, Shengqiang Cai and Michael D. Burkart*, ","doi":"10.1021/acsapm.4c0337710.1021/acsapm.4c03377","DOIUrl":"https://doi.org/10.1021/acsapm.4c03377https://doi.org/10.1021/acsapm.4c03377","url":null,"abstract":"","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"6 22","pages":"14022 14022"},"PeriodicalIF":4.4,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142691352","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Denise Lovison, Philipp Weingarten, Alexandra Sebeschuk, Bernhard Rieger* and Angela Casini*,
{"title":"Micellar Transfer Hydrogenation Catalysis in Water with Monocarbonyl Ruthenium(II)-poly(vinylphosphonate)-Containing Polymers: Achieving Reduction of Biomass-Derived Aldehydes","authors":"Denise Lovison, Philipp Weingarten, Alexandra Sebeschuk, Bernhard Rieger* and Angela Casini*, ","doi":"10.1021/acsapm.4c0276210.1021/acsapm.4c02762","DOIUrl":"https://doi.org/10.1021/acsapm.4c02762https://doi.org/10.1021/acsapm.4c02762","url":null,"abstract":"<p >With the aim to build a supramolecular organometallic catalyst for transfer hydrogenation (TH) reactions of hydrophobic substrates, micellar architectures of different sizes were obtained using amphiphilic diblock copolymers (BCPs) tethered to a Ru(II) monocarbonyl complex. An end-group functionalization strategy was employed to incorporate a bipyridyl end-group, used to further coordinate the cationic ruthenium fragment, to amphiphilic poly(2-vinylpyridine)-<i>b</i>-poly(diethyl vinylphosphonate). Owing to their amphiphilic character, the polymers form spherical micelles in water, which were characterized by different spectroscopic and analytical methods at different pH values and temperatures. The most suitable core–shell micellar system could level the catalytic activity of the ruthenium complex toward hydrophobic and biomass-derived aldehydes, which could be successfully reduced to the corresponding alcohols in water using potassium formate as a hydride source. Depending on the substrate’s hydrophobicity and concentration, the catalytic activity varied significantly. In addition, the polymer’s properties hardly changed during catalysis, facilitating effective recycling until the third catalytic cycle.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"6 22","pages":"13855–13864 13855–13864"},"PeriodicalIF":4.4,"publicationDate":"2024-11-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acsapm.4c02762","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142691257","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Maria Guillot-Ferriols, Carlos M Costa, Daniela M Correia, José Carlos Rodríguez-Hernández, Penelope M Tsimbouri, Senentxu Lanceros-Méndez, Matthew J Dalby, José Luis Gómez Ribelles, Gloria Gallego-Ferrer
{"title":"Piezoelectric Stimulation Induces Osteogenesis in Mesenchymal Stem Cells Cultured on Electroactive Two-Dimensional Substrates.","authors":"Maria Guillot-Ferriols, Carlos M Costa, Daniela M Correia, José Carlos Rodríguez-Hernández, Penelope M Tsimbouri, Senentxu Lanceros-Méndez, Matthew J Dalby, José Luis Gómez Ribelles, Gloria Gallego-Ferrer","doi":"10.1021/acsapm.4c02485","DOIUrl":"10.1021/acsapm.4c02485","url":null,"abstract":"<p><p>Physical cues have been shown to be effective in inducing osteogenic differentiation of mesenchymal stem cells (MSCs). Here, we propose piezoelectric stimulation as a potential osteogenic cue mimicking the electroactive properties of bone's extracellular matrix. When combined with a magnetostrictive component, piezoelectric polymers can be used for MSC stimulation by applying an external magnetic field. The deformation of the magnetostrictive component produces a deformation in the polymer matrix, generating a change in the surface charge that induces an electric field that can be transmitted to the cells. Cell adhesion, cytoskeleton changes, and metabolomics are the first evidence of MSC osteoblastogenesis and can be used to study initial MSC response to this kind of stimulation. In the current study, poly(vinylidene) fluoride (PVDF) piezoelectric films with and without cobalt ferrite oxide (CFO) crystallized from the melt in the presence of the ionic liquid 1-butyl-3-methyl-imidazolium chloride ([Bmim][Cl]) were produced. [Bmim][Cl] allowed the production of the β-phase, the most electroactive phase, even without CFO. After ionic liquid removal, PVDF and PVDF-CFO films presented high percentages of the β-phase and similar crystalline content. Incorporating CFO nanoparticles was effective, allowing the electromechanical stimulation of MSCs by applying a magnetic field with a bioreactor. Before stimulation, the initial response of MSCs was characterized in static conditions, showing that the produced films were biocompatible and noncytotoxic, allowing MSC adhesion and proliferation in the short term. Stimulation experiments revealed that MSCs electromechanically stimulated for 3 days in PVDF-CFO supports showed longer focal adhesions and decreased vimentin cytoskeletal density, both signals of early osteogenic differentiation. Furthermore, they rearranged their energy metabolism toward an osteogenic phenotype after 7 days of culture under the same stimulation. The results prove that MSCs respond to electromechanical stimulation by osteogenic differentiation.</p>","PeriodicalId":7,"journal":{"name":"ACS Applied Polymer Materials","volume":"6 22","pages":"13710-13722"},"PeriodicalIF":4.4,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11590054/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142737703","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}