ACS Central Science最新文献_第2页

Data-Driven Workflow for the Development and Discovery of N-Oxyl Hydrogen Atom Transfer Catalysts 数据驱动的工作流程开发和发现n -氧氢原子转移催化剂

IF 12.7 1区化学

ACS Central Science Pub Date : 2025-03-24 DOI: 10.1021/acscentsci.4c0191910.1021/acscentsci.4c01919

Cheng Yang, Thérèse Wild, Yulia Rakova, Stephen Maldonado*, Matthew S. Sigman* and Corey R. J. Stephenson*,

{"title":"Data-Driven Workflow for the Development and Discovery of N-Oxyl Hydrogen Atom Transfer Catalysts","authors":"Cheng Yang, Thérèse Wild, Yulia Rakova, Stephen Maldonado*, Matthew S. Sigman* and Corey R. J. Stephenson*, ","doi":"10.1021/acscentsci.4c0191910.1021/acscentsci.4c01919","DOIUrl":"https://doi.org/10.1021/acscentsci.4c01919https://doi.org/10.1021/acscentsci.4c01919","url":null,"abstract":"N-oxyl species are promising hydrogen atom transfer (HAT) catalysts to advance C–H bond activation reactions. However, because of the complex structure–activity relationship within the N-oxyl structure, catalyst optimization is a key challenge, particularly for simultaneous improvement across multiple parameters. This paper describes a data-driven approach to optimize N-oxyl hydrogen atom transfer catalysts. A focused library of 50 N-hydroxy compounds was synthesized and characterized by three parameters─oxidation peak potential, HAT reactivity, and stability─to generate a database. Statistical modeling of these activities described by their intrinsic physical organic parameters was used to build predictive models for catalyst discovery and to understand their structure–activity relationships. Virtual screening of 102 synthesizable candidates allowed for rapid identification of several ideal catalyst candidates. These statistical models clearly suggest that N-oxyl substructures bearing an adjacent heteroatom are more optimal HAT catalysts compared to the historical focus, phthalimide-N-oxyl, by striking the best balance among all three target experimental properties.Machine learning models revealed that N-oxyl compounds bearing adjacent heteroatoms to carbonyls are more promising hydrogen atom transfer catalysts by striking a balance between multiple parameters.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 4","pages":"592–600 592–600"},"PeriodicalIF":12.7,"publicationDate":"2025-03-24","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acscentsci.4c01919","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858377","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Host–Guest Synergy of Metal–Organic Frameworks for Enhanced Near-Infrared Ultrafast Laser Responsiveness 金属-有机框架的主客体协同作用增强近红外超快激光响应性

IF 12.7 1区化学

ACS Central Science Pub Date : 2025-03-18 DOI: 10.1021/acscentsci.5c0002210.1021/acscentsci.5c00022

Ruibing Lv, Lei Sun, Zhenghang Luo, Yujie Song, Shuo Li and Qi Zhang,

{"title":"Host–Guest Synergy of Metal–Organic Frameworks for Enhanced Near-Infrared Ultrafast Laser Responsiveness","authors":"Ruibing Lv, Lei Sun, Zhenghang Luo, Yujie Song, Shuo Li and Qi Zhang, ","doi":"10.1021/acscentsci.5c0002210.1021/acscentsci.5c00022","DOIUrl":"https://doi.org/10.1021/acscentsci.5c00022https://doi.org/10.1021/acscentsci.5c00022","url":null,"abstract":"Host–guest metal–organic frameworks (MOFs) offer significant potential and value in regulating and optimizing novel material properties and functionalities, owing to the synergistic effects between the host framework and the guest units. This study reported two silver-based host–guest MOFs, [Ag(ATRZ)(BrO3)]n (CMOF-1) and [Ag(ATRZ)1.5(ClO4)]n (CMOF-2), as promising candidates for laser-responsive materials. These materials feature 1D and 3D structures, respectively, comprising Ag-ATRZ cationic MOF frameworks integrated with two distinct oxidizing anionic guests, BrO3– and ClO4–. CMOF-1 and CMOF-2 are synthesized through straightforward, environmentally benign methods, enabling rapid fabrication. The exceptional near-infrared (NIR) laser responsiveness of CMOF-1 and CMOF-2 was achieved through the modulation of the cationic MOFs (CMOFs) architectures and synergistic interactions between the host and guest components. Moreover, both exhibit ultrafast deflagration-to-detonation transition (DDT) capabilities, alongside excellent thermal stability. This work expands the application scope of host–guest MOFs, and provides an effective strategy for developing high-performance laser-responsive materials.This study reports Ag-based host−guest MOFs with ultrafast NIR laser responsiveness: CMOF-1 and CMOF-2, which exhibit excellent ultrafast deflagration-to-detonation transition and thermal stability.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 4","pages":"583–591 583–591"},"PeriodicalIF":12.7,"publicationDate":"2025-03-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acscentsci.5c00022","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858373","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Hastened Fusion-Dependent Endosomal Escape Improves Activity of Delivered Enzyme Cargo 加速融合依赖的内体逃逸提高了递送酶货物的活性

IF 12.7 1区化学

ACS Central Science Pub Date : 2025-03-17 DOI: 10.1021/acscentsci.5c0001210.1021/acscentsci.5c00012

Angel Luis Vázquez-Maldonado, Teresia Chen, Diego Rodriguez, Madeline Zoltek and Alanna Schepartz*,

{"title":"Hastened Fusion-Dependent Endosomal Escape Improves Activity of Delivered Enzyme Cargo","authors":"Angel Luis Vázquez-Maldonado, Teresia Chen, Diego Rodriguez, Madeline Zoltek and Alanna Schepartz*, ","doi":"10.1021/acscentsci.5c0001210.1021/acscentsci.5c00012","DOIUrl":"https://doi.org/10.1021/acscentsci.5c00012https://doi.org/10.1021/acscentsci.5c00012","url":null,"abstract":"There is enormous interest in strategies to traffic biologics into the mammalian cell cytosol. Not only must these materials reach the appropriate cellular locale intact and in therapeutically relevant concentrations, they must also retain activity upon arrival. The question of residual activity is especially critical when delivery involves the late endocytic pathway, whose acidic environment can denature and/or degrade internalized material. ZF5.3 is a compact mini-protein that escapes efficiently from late endocytic vesicles, with or without covalently linked protein cargo. Here, we redesign the sequence of ZF5.3 to hasten the timing of endosomal escape. The new mini-protein we describe, AV5.3, escapes earlier than ZF5.3 along the endocytic pathway with no loss in efficiency, with or without enzyme cargo. More importantly, earlier endosomal escape translates into higher enzymatic activity of a pH-sensitive enzyme upon arrival in the cytosol. Delivery of the pH-sensitive enzyme DHFR with AV5.3 results in substantial catalytic activity in the cytosol, whereas delivery with ZF5.3 does not. The activity of delivered AV5.3-DHFR successfully rescues a DHFR deletion in CHO cells. AV5.3 represents an improved strategy for the efficient and direct delivery of active therapeutic proteins and enzymes.Rational redesign of a zinc finger mini-protein delivery agent hastens the timing of endosomal escape and avoids irreversible denaturation of enzyme cargo in late endocytic vesicles.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 4","pages":"574–582 574–582"},"PeriodicalIF":12.7,"publicationDate":"2025-03-17","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acscentsci.5c00012","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858369","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Supramolecular Engineering of Narrow Absorption Bands by Exciton Coupling in Pristine and Mixed Solid-State Dye Aggregates 原始和混合固态染料聚集体中激子耦合窄吸收带的超分子工程

IF 12.7 1区化学

ACS Central Science Pub Date : 2025-03-14 DOI: 10.1021/acscentsci.4c0215710.1021/acscentsci.4c02157

Tim Schembri, Julius Albert, Hendrik Hebling, Vladimir Stepanenko, Olga Anhalt, Kazutaka Shoyama, Matthias Stolte and Frank Würthner*,

{"title":"Supramolecular Engineering of Narrow Absorption Bands by Exciton Coupling in Pristine and Mixed Solid-State Dye Aggregates","authors":"Tim Schembri, Julius Albert, Hendrik Hebling, Vladimir Stepanenko, Olga Anhalt, Kazutaka Shoyama, Matthias Stolte and Frank Würthner*, ","doi":"10.1021/acscentsci.4c0215710.1021/acscentsci.4c02157","DOIUrl":"https://doi.org/10.1021/acscentsci.4c02157https://doi.org/10.1021/acscentsci.4c02157","url":null,"abstract":"Tunability of functional properties in a continuous manner is desired but challenging to accomplish for organic solid-state materials. Herein, we describe a method for tuning optoelectronic properties of solid-state aggregates with narrow absorption bands. First, we systematically shift the absorption maxima of highly dipolar merocyanine dyes in solution by chemical alterations of their chromophore cores. This leaves their solid-state packing arrangements unchanged, affording similar J- and H-coupled aggregate absorption bands at different wavelengths. Next, mixing these isostructural dyes leads to a spectral fine-tuning of the mixed layers, which could be characterized as crystalline organic solid solutions and utilized in narrowband color-selective organic photodiodes. Finally, we devise a semiempirical model, which explains the observed spectral tuning in terms of the molecular exciton theory. Thus, we demonstrate narrowband absorbing solid-state aggregates spanning the wavelength range of 437–760 nm, whose absorption can be fine-tuned over 40% of the visible light range.Spectral tuning of absorption properties for color sensing is achieved by design of isostructural compounds and binary mixtures thereof, which self-assemble into identical supramolecular aggregates.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 3","pages":"452–464 452–464"},"PeriodicalIF":12.7,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acscentsci.4c02157","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143696245","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Supramolecular Engineering of Narrow Absorption Bands by Exciton Coupling in Pristine and Mixed Solid-State Dye Aggregates. 原始和混合固态染料聚集体中激子耦合窄吸收带的超分子工程。

IF 12.7 1区化学

ACS Central Science Pub Date : 2025-03-14 eCollection Date: 2025-03-26 DOI: 10.1021/acscentsci.4c02157

Tim Schembri, Julius Albert, Hendrik Hebling, Vladimir Stepanenko, Olga Anhalt, Kazutaka Shoyama, Matthias Stolte, Frank Würthner

{"title":"Supramolecular Engineering of Narrow Absorption Bands by Exciton Coupling in Pristine and Mixed Solid-State Dye Aggregates.","authors":"Tim Schembri, Julius Albert, Hendrik Hebling, Vladimir Stepanenko, Olga Anhalt, Kazutaka Shoyama, Matthias Stolte, Frank Würthner","doi":"10.1021/acscentsci.4c02157","DOIUrl":"10.1021/acscentsci.4c02157","url":null,"abstract":"Tunability of functional properties in a continuous manner is desired but challenging to accomplish for organic solid-state materials. Herein, we describe a method for tuning optoelectronic properties of solid-state aggregates with narrow absorption bands. First, we systematically shift the absorption maxima of highly dipolar merocyanine dyes in solution by chemical alterations of their chromophore cores. This leaves their solid-state packing arrangements unchanged, affording similar J- and H-coupled aggregate absorption bands at different wavelengths. Next, mixing these isostructural dyes leads to a spectral fine-tuning of the mixed layers, which could be characterized as crystalline organic solid solutions and utilized in narrowband color-selective organic photodiodes. Finally, we devise a semiempirical model, which explains the observed spectral tuning in terms of the molecular exciton theory. Thus, we demonstrate narrowband absorbing solid-state aggregates spanning the wavelength range of 437-760 nm, whose absorption can be fine-tuned over 40% of the visible light range.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 3","pages":"452-464"},"PeriodicalIF":12.7,"publicationDate":"2025-03-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11950854/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143750244","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Plastic Pores for Switchable and Optimized Adsorption Behaviors 可切换和优化吸附行为的塑料孔

IF 12.7 1区化学

ACS Central Science Pub Date : 2025-03-13 DOI: 10.1021/acscentsci.4c0215510.1021/acscentsci.4c02155

Xue-Wen Zhang, Rong-Hua Wang, Jie-Peng Zhang* and Xiao-Ming Chen,

{"title":"Plastic Pores for Switchable and Optimized Adsorption Behaviors","authors":"Xue-Wen Zhang, Rong-Hua Wang, Jie-Peng Zhang* and Xiao-Ming Chen, ","doi":"10.1021/acscentsci.4c0215510.1021/acscentsci.4c02155","DOIUrl":"https://doi.org/10.1021/acscentsci.4c02155https://doi.org/10.1021/acscentsci.4c02155","url":null,"abstract":"Similar to conventional solids, porous materials have demonstrated rigid and flexible behaviors. Here, we show that flexible pores can be not just elastic but also plastic. By variation of the hydrogen-bonding ability and steric hindrance of ligand side groups, the energy difference and barrier between metastable states of a porous framework are fine-tuned to enable the plastic behavior. All metastable pore structures can transform to the target ones in atmospheres of the target guests with sufficiently high pressures, and all shaped pores can remain unchanged after guest removal, resulting in optimized host–guest recognitions for the target guests. Up to a 6-fold increase of adsorption selectivity and 9-fold increase of purification productivity for CO2 capture and coalmine CH4 upgrading, and even inversion of CO2/C2H2 selectivity, have been achieved by reversible pore-shaping of a single plastic-pore adsorbent. The realization of plastic pores creates an opportunity for on-demand switching of adsorption and separation functions with optimized performances.While porous materials possess rigid or flexible/elastic pores, a plastic pore is realized for the first time, which can be shaped by target guest molecules to meet needs of different applications.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 3","pages":"479–485 479–485"},"PeriodicalIF":12.7,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acscentsci.4c02155","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143696536","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

The Spin-Phonon Relaxation Mechanism of Single-Molecule Magnets in the Presence of Strong Exchange Coupling 强交换耦合存在下单分子磁体的自旋声子弛豫机制

IF 12.7 1区化学

ACS Central Science Pub Date : 2025-03-13 DOI: 10.1021/acscentsci.4c0213910.1021/acscentsci.4c02139

Sourav Mondal, Julia Netz, David Hunger, Simon Suhr, Biprajit Sarkar, Joris van Slageren, Andreas Köhn and Alessandro Lunghi*,

{"title":"The Spin-Phonon Relaxation Mechanism of Single-Molecule Magnets in the Presence of Strong Exchange Coupling","authors":"Sourav Mondal, Julia Netz, David Hunger, Simon Suhr, Biprajit Sarkar, Joris van Slageren, Andreas Köhn and Alessandro Lunghi*, ","doi":"10.1021/acscentsci.4c0213910.1021/acscentsci.4c02139","DOIUrl":"https://doi.org/10.1021/acscentsci.4c02139https://doi.org/10.1021/acscentsci.4c02139","url":null,"abstract":"Magnetic relaxation in coordination compounds is largely dominated by the interaction of the spin with phonons. Although a comprehensive understanding of spin-phonon relaxation has been achieved for mononuclear complexes, only a qualitative picture is available for polynuclear compounds. Large zero-field splitting and exchange coupling values have been empirically found to strongly suppress spin relaxation and have been used as the main guideline for designing molecular compounds with long spin lifetime, also known as single-molecule magnets, but no microscopic rationale for these observations is available. Here we fill this critical knowledge gap by providing a full first-principles description of spin-phonon relaxation in an air-stable Co(II) dimer with both large single-ion anisotropy and exchange coupling. Simulations reproduce the experimental relaxation data with excellent accuracy and provide a microscopic understanding of Orbach and Raman relaxation pathways and their dependency on exchange coupling, zero-field splitting, and molecular vibrations. Theory and numerical simulations show that increasing cluster nuclearity to just four cobalt units would lead to a complete suppression of low-temperature Raman relaxation. These results hold a general validity for polynuclear single-molecule magnets, providing a deeper understanding of their relaxation and revised strategies for their improvement.Spin relaxation in polynuclear coordination complexes is unraveled through ab initio open quantum system simulations, revealing new strategies to fully suppress Raman relaxation at low temperature.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 4","pages":"550–559 550–559"},"PeriodicalIF":12.7,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acscentsci.4c02139","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143858712","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Polyacrylamide-Based Antimicrobial Copolymers to Replace or Rescue Antibiotics. 基于聚丙烯酰胺的抗菌共聚物取代或挽救抗生素。

IF 12.7 1区化学

ACS Central Science Pub Date : 2025-03-13 eCollection Date: 2025-03-26 DOI: 10.1021/acscentsci.4c01973

Shoshana C Williams, Madeline B Chosy, Carolyn K Jons, Changxin Dong, Alexander N Prossnitz, Xinyu Liu, Hector Lopez Hernandez, Lynette Cegelski, Eric A Appel

{"title":"Polyacrylamide-Based Antimicrobial Copolymers to Replace or Rescue Antibiotics.","authors":"Shoshana C Williams, Madeline B Chosy, Carolyn K Jons, Changxin Dong, Alexander N Prossnitz, Xinyu Liu, Hector Lopez Hernandez, Lynette Cegelski, Eric A Appel","doi":"10.1021/acscentsci.4c01973","DOIUrl":"10.1021/acscentsci.4c01973","url":null,"abstract":"Antibiotics save countless lives each year and have dramatically improved human health outcomes since their introduction in the 20th century. Unfortunately, bacteria are now developing resistance to antibiotics at an alarming rate, with many new strains of \"superbugs\" showing simultaneous resistance to multiple classes of antibiotics. To mitigate the global burden of antimicrobial resistance, we must develop new antibiotics that are broadly effective, safe, and highly stable to enable global access. In this manuscript, we report the development of polyacrylamide-based copolymers as a class of broad-spectrum antibiotics with efficacy against several critical pathogens. We demonstrate that these copolymer drugs are selective for bacteria over mammalian cells, indicating a favorable safety profile. We show that they kill bacteria through a membrane disruption mechanism, which allows them to overcome traditional mechanisms of antimicrobial resistance. Finally, we demonstrate their ability to rehabilitate an existing small-molecule antibiotic that is highly subject to resistance development by improving its potency and eliminating the development of resistance in a combination treatment. This work represents a significant step toward combating antimicrobial resistance.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 3","pages":"486-496"},"PeriodicalIF":12.7,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11950845/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143750241","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Polyacrylamide-Based Antimicrobial Copolymers to Replace or Rescue Antibiotics 基于聚丙烯酰胺的抗菌共聚物取代或挽救抗生素

IF 12.7 1区化学

ACS Central Science Pub Date : 2025-03-13 DOI: 10.1021/acscentsci.4c0197310.1021/acscentsci.4c01973

Shoshana C. Williams, Madeline B. Chosy, Carolyn K. Jons, Changxin Dong, Alexander N. Prossnitz, Xinyu Liu, Hector Lopez Hernandez, Lynette Cegelski and Eric A. Appel*,

{"title":"Polyacrylamide-Based Antimicrobial Copolymers to Replace or Rescue Antibiotics","authors":"Shoshana C. Williams, Madeline B. Chosy, Carolyn K. Jons, Changxin Dong, Alexander N. Prossnitz, Xinyu Liu, Hector Lopez Hernandez, Lynette Cegelski and Eric A. Appel*, ","doi":"10.1021/acscentsci.4c0197310.1021/acscentsci.4c01973","DOIUrl":"https://doi.org/10.1021/acscentsci.4c01973https://doi.org/10.1021/acscentsci.4c01973","url":null,"abstract":"Antibiotics save countless lives each year and have dramatically improved human health outcomes since their introduction in the 20th century. Unfortunately, bacteria are now developing resistance to antibiotics at an alarming rate, with many new strains of “superbugs” showing simultaneous resistance to multiple classes of antibiotics. To mitigate the global burden of antimicrobial resistance, we must develop new antibiotics that are broadly effective, safe, and highly stable to enable global access. In this manuscript, we report the development of polyacrylamide-based copolymers as a class of broad-spectrum antibiotics with efficacy against several critical pathogens. We demonstrate that these copolymer drugs are selective for bacteria over mammalian cells, indicating a favorable safety profile. We show that they kill bacteria through a membrane disruption mechanism, which allows them to overcome traditional mechanisms of antimicrobial resistance. Finally, we demonstrate their ability to rehabilitate an existing small-molecule antibiotic that is highly subject to resistance development by improving its potency and eliminating the development of resistance in a combination treatment. This work represents a significant step toward combating antimicrobial resistance.Polyacrylamide-based copolymers function as broad-spectrum antibiotics via a membrane disruption mechanism. They can prevent or delay the onset of resistance and rehabilitate existing antibiotics.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 3","pages":"486–496 486–496"},"PeriodicalIF":12.7,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acscentsci.4c01973","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143696537","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Plastic Pores for Switchable and Optimized Adsorption Behaviors. 可切换和优化吸附行为的塑料孔。

IF 12.7 1区化学

ACS Central Science Pub Date : 2025-03-13 eCollection Date: 2025-03-26 DOI: 10.1021/acscentsci.4c02155

Xue-Wen Zhang, Rong-Hua Wang, Jie-Peng Zhang, Xiao-Ming Chen

{"title":"Plastic Pores for Switchable and Optimized Adsorption Behaviors.","authors":"Xue-Wen Zhang, Rong-Hua Wang, Jie-Peng Zhang, Xiao-Ming Chen","doi":"10.1021/acscentsci.4c02155","DOIUrl":"10.1021/acscentsci.4c02155","url":null,"abstract":"Similar to conventional solids, porous materials have demonstrated rigid and flexible behaviors. Here, we show that flexible pores can be not just elastic but also plastic. By variation of the hydrogen-bonding ability and steric hindrance of ligand side groups, the energy difference and barrier between metastable states of a porous framework are fine-tuned to enable the plastic behavior. All metastable pore structures can transform to the target ones in atmospheres of the target guests with sufficiently high pressures, and all shaped pores can remain unchanged after guest removal, resulting in optimized host-guest recognitions for the target guests. Up to a 6-fold increase of adsorption selectivity and 9-fold increase of purification productivity for CO2 capture and coalmine CH4 upgrading, and even inversion of CO2/C2H2 selectivity, have been achieved by reversible pore-shaping of a single plastic-pore adsorbent. The realization of plastic pores creates an opportunity for on-demand switching of adsorption and separation functions with optimized performances.","PeriodicalId":10,"journal":{"name":"ACS Central Science","volume":"11 3","pages":"479-485"},"PeriodicalIF":12.7,"publicationDate":"2025-03-13","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC11950851/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143750240","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"化学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0