Chemistry of Materials最新文献_第7页

In-Situ Deposition of a Zeolite Imidazole Framework to Decorate a Polyacrylonitrile Fiber Membrane for Efficient Removal of Multiple Water Pollutants

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2025-03-08 DOI: 10.1021/acs.chemmater.4c03010

Jingjing Zhang, Jiapeng Li, Zhaolian Han, Qiushi Jiang, Zehang Jia, Dongxing Dong, Chengcheng Zhang, Caixia Wu, Zhiqiang Cheng

{"title":"In-Situ Deposition of a Zeolite Imidazole Framework to Decorate a Polyacrylonitrile Fiber Membrane for Efficient Removal of Multiple Water Pollutants","authors":"Jingjing Zhang, Jiapeng Li, Zhaolian Han, Qiushi Jiang, Zehang Jia, Dongxing Dong, Chengcheng Zhang, Caixia Wu, Zhiqiang Cheng","doi":"10.1021/acs.chemmater.4c03010","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03010","url":null,"abstract":"A composite adsorption filter membrane that is efficient, fast, and recyclable was created in order to boost the adsorption capacity and reduce loss during application. We created a polyacrylonitrile (PAN) fiber membrane using electrospinning technology as a composite adsorbent substrate material. After that, we stirred the membrane at room temperature to deposit a two-dimensional flaky zeolitic imidazolate framework (ZIF-L) on the PAN substrate’s surface. Better thermal stability, multipore size distribution, high specific surface area, and good crystallinity are all features of the synthesized ZIF-L@PAN composite fiber membrane The composite membrane demonstrated high efficiency and universality in adsorbing and removing various water pollutants, along with good antibacterial properties. The synthesized fiber composite membrane exhibits a more pronounced adsorption capacity at pH values of 7 to 8 when compared to ZIF-L and PAN membranes. Accordingly, the 10 mg composite membrane’s adsorption capacity for 500 mg/L pollutants [tetracycline hydrochloride, sulfamethoxazole, Congo red (CR), methylene blue, and Cu2+] was 437.74, 401.73, 497.83, 425.39, and 437.76 mg/g, respectively. Simultaneous adsorption is carried out through multiple steps. Intraparticle diffusion is not the only rate-controlling step. Adsorption is chemical adsorption. Notably, ZIF-L@PAN exhibits outstanding cycle stability and a maximum adsorption capacity of 3915.14 mg/g for CR. By designing a multipurpose adsorption filter membrane that can remove refractory, organic, and inorganic pollutants, this study hopes to make it easier to filter and purify different kinds of sewage.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"53 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143576256","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

In-Situ Deposition of a Zeolite Imidazole Framework to Decorate a Polyacrylonitrile Fiber Membrane for Efficient Removal of Multiple Water Pollutants

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2025-03-08 DOI: 10.1021/acs.chemmater.4c0301010.1021/acs.chemmater.4c03010

Jingjing Zhang, Jiapeng Li, Zhaolian Han, Qiushi Jiang, Zehang Jia, Dongxing Dong, Chengcheng Zhang, Caixia Wu and Zhiqiang Cheng*,

{"title":"In-Situ Deposition of a Zeolite Imidazole Framework to Decorate a Polyacrylonitrile Fiber Membrane for Efficient Removal of Multiple Water Pollutants","authors":"Jingjing Zhang, Jiapeng Li, Zhaolian Han, Qiushi Jiang, Zehang Jia, Dongxing Dong, Chengcheng Zhang, Caixia Wu and Zhiqiang Cheng*, ","doi":"10.1021/acs.chemmater.4c0301010.1021/acs.chemmater.4c03010","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03010https://doi.org/10.1021/acs.chemmater.4c03010","url":null,"abstract":"A composite adsorption filter membrane that is efficient, fast, and recyclable was created in order to boost the adsorption capacity and reduce loss during application. We created a polyacrylonitrile (PAN) fiber membrane using electrospinning technology as a composite adsorbent substrate material. After that, we stirred the membrane at room temperature to deposit a two-dimensional flaky zeolitic imidazolate framework (ZIF-L) on the PAN substrate’s surface. Better thermal stability, multipore size distribution, high specific surface area, and good crystallinity are all features of the synthesized ZIF-L@PAN composite fiber membrane The composite membrane demonstrated high efficiency and universality in adsorbing and removing various water pollutants, along with good antibacterial properties. The synthesized fiber composite membrane exhibits a more pronounced adsorption capacity at pH values of 7 to 8 when compared to ZIF-L and PAN membranes. Accordingly, the 10 mg composite membrane’s adsorption capacity for 500 mg/L pollutants [tetracycline hydrochloride, sulfamethoxazole, Congo red (CR), methylene blue, and Cu2+] was 437.74, 401.73, 497.83, 425.39, and 437.76 mg/g, respectively. Simultaneous adsorption is carried out through multiple steps. Intraparticle diffusion is not the only rate-controlling step. Adsorption is chemical adsorption. Notably, ZIF-L@PAN exhibits outstanding cycle stability and a maximum adsorption capacity of 3915.14 mg/g for CR. By designing a multipurpose adsorption filter membrane that can remove refractory, organic, and inorganic pollutants, this study hopes to make it easier to filter and purify different kinds of sewage.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 6","pages":"2166–2176 2166–2176"},"PeriodicalIF":7.2,"publicationDate":"2025-03-08","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143678915","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Evolution of Structural Order and Magnetic Anisotropy in Yb0.5(Co1–xFex)3Ge3 through Doping of a Kagome Lattice

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2025-03-07 DOI: 10.1021/acs.chemmater.5c00119

Rahul Meduri, Mario A. Plata, Gregory T. McCandless, Benny C. Schundelmier, Mehak Ghafoor, Kaya Wei, Julia Y. Chan

{"title":"Evolution of Structural Order and Magnetic Anisotropy in Yb0.5(Co1–xFex)3Ge3 through Doping of a Kagome Lattice","authors":"Rahul Meduri, Mario A. Plata, Gregory T. McCandless, Benny C. Schundelmier, Mehak Ghafoor, Kaya Wei, Julia Y. Chan","doi":"10.1021/acs.chemmater.5c00119","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c00119","url":null,"abstract":"Kagome materials provide fruitful grounds for exploring the intersection of topology and magnetism. In this article, the single crystal growth of Yb0.5(Co1–xFex)3Ge3 (x = 0.00, 0.25, 0.50, 0.75, and 1.00) is reported. As Fe is substituted into the Co-containing kagome net, the structure transforms from the disordered Y0.5Co3Ge3/CoSn-type hybrid structure to the ordered HfFe6Ge6-type structure. Diffusive scattering is observed in all doped concentrations that eventually converge to a single reflection in the Fe end member, ultimately doubling the unit cell along the c-axis. Anisotropic magnetic measurements were performed to evaluate how the magnetism of the kagome lattice is influenced by Fe substitution. Magnetic interactions are primarily observed along the c-axis. Additionally, a reorientation of the magnetic easy axis is observed with increasing Fe incorporation, highlighting how the magnetism of this material can be chemically tuned. Resistivity with unusual behavior observed in the doped compositions is also reported. The rationale behind the structural evolution from disordered to ordered is discussed.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"39 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143575350","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Deciphering the Antibacterial Mechanism of Hollow Sphere Metal–Organic Frameworks against Staphylococcus aureus and Its Application in Wound Healing

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2025-03-07 DOI: 10.1021/acs.chemmater.4c03165

Qian Zhang, Rui Liu, Shuguang Yan, Xueting Yan, Yi Lv

{"title":"Deciphering the Antibacterial Mechanism of Hollow Sphere Metal–Organic Frameworks against Staphylococcus aureus and Its Application in Wound Healing","authors":"Qian Zhang, Rui Liu, Shuguang Yan, Xueting Yan, Yi Lv","doi":"10.1021/acs.chemmater.4c03165","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03165","url":null,"abstract":"Staphylococcus aureus infection and antimicrobial resistance (AMR) to antibiotics are two significant factors that pose escalating threats to public health, potentially leading to persistent pain or even death. Consequently, there is an urgent need for the development of alternative antibacterial materials. In this study, we have successfully developed a biocompatible nanosystem based on hollow spherical zeolitic imidazolate framework-67 (ZIF-67 HS), which exhibits remarkable bactericidal efficacy against Gram-positive S. aureus both in vitro and in vivo. Importantly, our findings demonstrate that prolonged exposure of S. aureus to subminimum inhibitory concentrations of ZIF-67 HS does not induce secondary resistance as observed with conventional antibiotics; instead, it maintains sustained susceptibility toward antibiotic-resistant strains. Multiomics analyses (including transcriptomics, metabolomics, and metalomics) have indicated that ZIF-67 HS regulates 95 genes, 261 metabolites, and 2 metal elements in S. aureus. Through bioinformatics analysis in combination with bioassays, we demonstrated that ZIF-67 HS disrupted multiple essential pathways in the pathogen, including amino acid metabolism, iron metabolism, membrane transport, reactive oxygen species (ROS), and S. aureus infection pathways. Our findings suggest that ZIF-67 HS induces bacterial death through multiple mechanisms rather than a single target and highlight its long-lasting antibacterial properties. This study presents valuable insights into the potential of nanobiomedicine for eradicating bacteria and elucidates the related molecular mechanism.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"8 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143575169","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Surface Exciton Polariton in Cesium Lead Halide Perovskites

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2025-03-07 DOI: 10.1021/acs.chemmater.4c0326210.1021/acs.chemmater.4c03262

Jason Hao, Jeffrey Owrutsky, Daniel C. Ratchford, Blake Simpkins and Alexander L. Efros*,

{"title":"Surface Exciton Polariton in Cesium Lead Halide Perovskites","authors":"Jason Hao, Jeffrey Owrutsky, Daniel C. Ratchford, Blake Simpkins and Alexander L. Efros*, ","doi":"10.1021/acs.chemmater.4c0326210.1021/acs.chemmater.4c03262","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03262https://doi.org/10.1021/acs.chemmater.4c03262","url":null,"abstract":"In this article, we developed a theory describing surface exciton polaritons (SEPs) that accounts for the spatial dispersion of the dielectric constant connected with exciton momentum. Due to strong coupling between light and bulk excitons in the frequency separation, ℏωLT, between the longitudinal and transverse excitons, the SEP is formed and behaves as partially light and partially matter. The dispersion of the SEP was found through a combined solution of Maxwell’s and Thomas-Hopfield’s equations. The analytical theory describes SEPs at any bulk exciton/vacuum interface and provides its complete dispersion if one knows ℏωLT, the exciton effective mass, M, and the high-frequency dielectric constant, κ∞. The presented theory is in excellent agreement with the only numerical modeling of this problem, which was conducted for SEPs at a ZnO/vacuum interface. Calculations show the spatial dispersion of the dielectric constant leads to rather small broadening of the photon-like quasi-particle and suggest using SEPs for long-range coherence transfer. The theory was used to describe SEP dispersion in CsPbCl3 and CsPbBr3 perovskites.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 6","pages":"2251–2257 2251–2257"},"PeriodicalIF":7.2,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143678792","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Evolution of Structural Order and Magnetic Anisotropy in Yb0.5(Co1–xFex)3Ge3 through Doping of a Kagome Lattice

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2025-03-07 DOI: 10.1021/acs.chemmater.5c0011910.1021/acs.chemmater.5c00119

Rahul Meduri, Mario A. Plata, Gregory T. McCandless, Benny C. Schundelmier, Mehak Ghafoor, Kaya Wei and Julia Y. Chan*,

{"title":"Evolution of Structural Order and Magnetic Anisotropy in Yb0.5(Co1–xFex)3Ge3 through Doping of a Kagome Lattice","authors":"Rahul Meduri, Mario A. Plata, Gregory T. McCandless, Benny C. Schundelmier, Mehak Ghafoor, Kaya Wei and Julia Y. Chan*, ","doi":"10.1021/acs.chemmater.5c0011910.1021/acs.chemmater.5c00119","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c00119https://doi.org/10.1021/acs.chemmater.5c00119","url":null,"abstract":"Kagome materials provide fruitful grounds for exploring the intersection of topology and magnetism. In this article, the single crystal growth of Yb0.5(Co1–xFex)3Ge3 (x = 0.00, 0.25, 0.50, 0.75, and 1.00) is reported. As Fe is substituted into the Co-containing kagome net, the structure transforms from the disordered Y0.5Co3Ge3/CoSn-type hybrid structure to the ordered HfFe6Ge6-type structure. Diffusive scattering is observed in all doped concentrations that eventually converge to a single reflection in the Fe end member, ultimately doubling the unit cell along the c-axis. Anisotropic magnetic measurements were performed to evaluate how the magnetism of the kagome lattice is influenced by Fe substitution. Magnetic interactions are primarily observed along the c-axis. Additionally, a reorientation of the magnetic easy axis is observed with increasing Fe incorporation, highlighting how the magnetism of this material can be chemically tuned. Resistivity with unusual behavior observed in the doped compositions is also reported. The rationale behind the structural evolution from disordered to ordered is discussed.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 6","pages":"2302–2313 2302–2313"},"PeriodicalIF":7.2,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143678850","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Deciphering the Antibacterial Mechanism of Hollow Sphere Metal–Organic Frameworks against Staphylococcus aureus and Its Application in Wound Healing

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2025-03-07 DOI: 10.1021/acs.chemmater.4c0316510.1021/acs.chemmater.4c03165

Qian Zhang, Rui Liu, Shuguang Yan, Xueting Yan* and Yi Lv,

{"title":"Deciphering the Antibacterial Mechanism of Hollow Sphere Metal–Organic Frameworks against Staphylococcus aureus and Its Application in Wound Healing","authors":"Qian Zhang, Rui Liu, Shuguang Yan, Xueting Yan* and Yi Lv, ","doi":"10.1021/acs.chemmater.4c0316510.1021/acs.chemmater.4c03165","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03165https://doi.org/10.1021/acs.chemmater.4c03165","url":null,"abstract":"Staphylococcus aureus infection and antimicrobial resistance (AMR) to antibiotics are two significant factors that pose escalating threats to public health, potentially leading to persistent pain or even death. Consequently, there is an urgent need for the development of alternative antibacterial materials. In this study, we have successfully developed a biocompatible nanosystem based on hollow spherical zeolitic imidazolate framework-67 (ZIF-67 HS), which exhibits remarkable bactericidal efficacy against Gram-positive S. aureus both in vitro and in vivo. Importantly, our findings demonstrate that prolonged exposure of S. aureus to subminimum inhibitory concentrations of ZIF-67 HS does not induce secondary resistance as observed with conventional antibiotics; instead, it maintains sustained susceptibility toward antibiotic-resistant strains. Multiomics analyses (including transcriptomics, metabolomics, and metalomics) have indicated that ZIF-67 HS regulates 95 genes, 261 metabolites, and 2 metal elements in S. aureus. Through bioinformatics analysis in combination with bioassays, we demonstrated that ZIF-67 HS disrupted multiple essential pathways in the pathogen, including amino acid metabolism, iron metabolism, membrane transport, reactive oxygen species (ROS), and S. aureus infection pathways. Our findings suggest that ZIF-67 HS induces bacterial death through multiple mechanisms rather than a single target and highlight its long-lasting antibacterial properties. This study presents valuable insights into the potential of nanobiomedicine for eradicating bacteria and elucidates the related molecular mechanism.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 6","pages":"2204–2219 2204–2219"},"PeriodicalIF":7.2,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143678856","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Gram-Scale Synthesis of Imine-Linked Covalent Organic Frameworks at Ambient Conditions Using Metal Triflimides

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2025-03-07 DOI: 10.1021/acs.chemmater.4c0339810.1021/acs.chemmater.4c03398

Harsh Vardhan, Bongki Shin, Xu Wang, Shu-Yan Jiang, Abdullah Alazmi, Ruoyang Zhang, Yimo Han, Xiaowei Wu and Rafael Verduzco*,

{"title":"Gram-Scale Synthesis of Imine-Linked Covalent Organic Frameworks at Ambient Conditions Using Metal Triflimides","authors":"Harsh Vardhan, Bongki Shin, Xu Wang, Shu-Yan Jiang, Abdullah Alazmi, Ruoyang Zhang, Yimo Han, Xiaowei Wu and Rafael Verduzco*, ","doi":"10.1021/acs.chemmater.4c0339810.1021/acs.chemmater.4c03398","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03398https://doi.org/10.1021/acs.chemmater.4c03398","url":null,"abstract":"Imine-linked covalent organic frameworks (COFs) are crystalline and permanently porous networks with significant prospects for addressing current challenges pertinent to energy and environmental sustainabilities, including gas adsorption, energy storage, catalysis, optoelectronics, and many more. These crystalline networks are conventionally prepared by condensing a polyfunctional aldehyde and amine building blocks of different symmetricities and point groups for multiple days at an elevated temperature. Here, we demonstrate the catalytic role of metal triflimides in accelerating the synthesis of robust and fragile imine-linked COFs under ambient conditions. We first tested a range of metal triflimides, Zn(NTf2)2, Co(NTf2)2, Mg(NTf2)2, and Sc(NTf2)3, for the synthesis of a model TAPB-PDA COF and found that all metal triflimides afforded crystalline frameworks in quantitative yields under ambient temperatures and in the presence of air. Zn(NTf2)2 was found to produce the most crystalline framework in less than 15 min under optimized catalyst loading. Zn(NTf2)2 was further tested as a catalyst for over 15 different COFs of varying building blocks, substituents, and topologies, and it effectively catalyzed the rapid fabrication of all imine frameworks targeted, including previously unreported TAPB-DMTPDA COFs. Notably, this catalyst was also successful in the gram-scale fabrication of both robust and fragile COFs underlining a simple, scalable, low-cost, rapid, and benchtop approach for the synthesis of imine-linked COFs that can potentially eliminate barriers to the commercialization of imine COFs for a variety of applications.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 6","pages":"2258–2267 2258–2267"},"PeriodicalIF":7.2,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143678913","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Gram-Scale Synthesis of Imine-Linked Covalent Organic Frameworks at Ambient Conditions Using Metal Triflimides

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2025-03-07 DOI: 10.1021/acs.chemmater.4c03398

Harsh Vardhan, Bongki Shin, Xu Wang, Shu-Yan Jiang, Abdullah Alazmi, Ruoyang Zhang, Yimo Han, Xiaowei Wu, Rafael Verduzco

{"title":"Gram-Scale Synthesis of Imine-Linked Covalent Organic Frameworks at Ambient Conditions Using Metal Triflimides","authors":"Harsh Vardhan, Bongki Shin, Xu Wang, Shu-Yan Jiang, Abdullah Alazmi, Ruoyang Zhang, Yimo Han, Xiaowei Wu, Rafael Verduzco","doi":"10.1021/acs.chemmater.4c03398","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03398","url":null,"abstract":"Imine-linked covalent organic frameworks (COFs) are crystalline and permanently porous networks with significant prospects for addressing current challenges pertinent to energy and environmental sustainabilities, including gas adsorption, energy storage, catalysis, optoelectronics, and many more. These crystalline networks are conventionally prepared by condensing a polyfunctional aldehyde and amine building blocks of different symmetricities and point groups for multiple days at an elevated temperature. Here, we demonstrate the catalytic role of metal triflimides in accelerating the synthesis of robust and fragile imine-linked COFs under ambient conditions. We first tested a range of metal triflimides, Zn(NTf2)2, Co(NTf2)2, Mg(NTf2)2, and Sc(NTf2)3, for the synthesis of a model TAPB-PDA COF and found that all metal triflimides afforded crystalline frameworks in quantitative yields under ambient temperatures and in the presence of air. Zn(NTf2)2 was found to produce the most crystalline framework in less than 15 min under optimized catalyst loading. Zn(NTf2)2 was further tested as a catalyst for over 15 different COFs of varying building blocks, substituents, and topologies, and it effectively catalyzed the rapid fabrication of all imine frameworks targeted, including previously unreported TAPB-DMTPDA COFs. Notably, this catalyst was also successful in the gram-scale fabrication of both robust and fragile COFs underlining a simple, scalable, low-cost, rapid, and benchtop approach for the synthesis of imine-linked COFs that can potentially eliminate barriers to the commercialization of imine COFs for a variety of applications.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"17 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143569989","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Surface Exciton Polariton in Cesium Lead Halide Perovskites

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2025-03-07 DOI: 10.1021/acs.chemmater.4c03262

Jason Hao, Jeffrey Owrutsky, Daniel C. Ratchford, Blake Simpkins, Alexander L. Efros

{"title":"Surface Exciton Polariton in Cesium Lead Halide Perovskites","authors":"Jason Hao, Jeffrey Owrutsky, Daniel C. Ratchford, Blake Simpkins, Alexander L. Efros","doi":"10.1021/acs.chemmater.4c03262","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03262","url":null,"abstract":"In this article, we developed a theory describing surface exciton polaritons (SEPs) that accounts for the spatial dispersion of the dielectric constant connected with exciton momentum. Due to strong coupling between light and bulk excitons in the frequency separation, ℏωLT, between the longitudinal and transverse excitons, the SEP is formed and behaves as partially light and partially matter. The dispersion of the SEP was found through a combined solution of Maxwell’s and Thomas-Hopfield’s equations. The analytical theory describes SEPs at any bulk exciton/vacuum interface and provides its complete dispersion if one knows ℏωLT, the exciton effective mass, M, and the high-frequency dielectric constant, κ∞. The presented theory is in excellent agreement with the only numerical modeling of this problem, which was conducted for SEPs at a ZnO/vacuum interface. Calculations show the spatial dispersion of the dielectric constant leads to rather small broadening of the photon-like quasi-particle and suggest using SEPs for long-range coherence transfer. The theory was used to describe SEP dispersion in CsPbCl3 and CsPbBr3 perovskites.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"91 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-03-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143569988","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0