Chemistry of Materials最新文献_第8页

Correction to “Thermal Stability of Amorphous Metal Oxides: The Interplay of Secondary Cations, Degree of Substitution and Local Structure” 对“非晶金属氧化物的热稳定性：仲阳离子、取代度和局部结构的相互作用”的修正

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2025-05-07 DOI: 10.1021/acs.chemmater.5c00481

Li Zeng, D. Bruce Buchholz, Denis T. Keane, Tobin J. Marks, Julia E. Medvedeva, Michael J. Bedzyk

{"title":"Correction to “Thermal Stability of Amorphous Metal Oxides: The Interplay of Secondary Cations, Degree of Substitution and Local Structure”","authors":"Li Zeng, D. Bruce Buchholz, Denis T. Keane, Tobin J. Marks, Julia E. Medvedeva, Michael J. Bedzyk","doi":"10.1021/acs.chemmater.5c00481","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c00481","url":null,"abstract":"The correct MRSEC grant number should be DMR-2308691, rather than DMR-230869. The corrected Acknowledgment is below. The authors thank the Northwestern Materials Research Center, NSF MRSEC grants DMR-1720139 and DMR-2308691, for financial support of this work. The X-ray scattering work was performed at the DuPont-Northwestern-Dow Collaborative Access Team (DND-CAT) located at Sector 5 of the Advanced Photon Source (APS). DND-CAT is supported by Northwestern University, The Dow Chemical Company, and DuPont de Nemours, Inc. This research used resources from the Advanced Photon Source, a U.S. Department of Energy (DOE) Office of Science User Facility operated for the DOE Office of Science by Argonne National Laboratory under Contract No. DE-AC02-06CH11357. This work made use of the Pulsed Laser Deposition Facility of Northwestern University supported by the MRSEC program of the National Science Foundation (DMR-2308691) at the Materials Research Center of Northwestern University and the Soft and Hybrid Nanotechnology Experimental Resource (NSF ECCS-2025633). J.E.M. thanks NSF-DMREF grants DMR-1729779 and DMR-1842467 and DOE grant DE-EE0009346 for support and NSF-MRI grant OAC-1919789 for computational facilities. This article has not yet been cited by other publications.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"119 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143920787","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

A Tunable Hydrogel Platform Based on Platinum-Containing Polymeric Arsenicals 基于含铂聚合物砷的可调水凝胶平台

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2025-05-07 DOI: 10.1021/acs.chemmater.5c00184

Alexandros Magiakos, Evelina Liarou, Spyridon Efstathiou, Andrea Dsouza, Chrystala Constantinidou, Marc Walker, Constantinos Methenitis, Paul Wilson

{"title":"A Tunable Hydrogel Platform Based on Platinum-Containing Polymeric Arsenicals","authors":"Alexandros Magiakos, Evelina Liarou, Spyridon Efstathiou, Andrea Dsouza, Chrystala Constantinidou, Marc Walker, Constantinos Methenitis, Paul Wilson","doi":"10.1021/acs.chemmater.5c00184","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c00184","url":null,"abstract":"Platinum and arsenic (e.g., cisplatin, As2O3) have been used extensively in modern medicine due to their strong anticancer and antimicrobial activities. Here, polymeric arsenical scaffolds with varying As-functionalized acrylamide monomer (AsAm) composition are combined with PtII giving rise to hydrogels (P1-Pt–P4-Pt) with their properties being dependent on the AsAm content. The nature of the Pt–polymer interaction has been thoroughly investigated by 1H and 195Pt NMR spectroscopy as well as FT-IR, SEM, XPS, and potentiometric titration suggesting that cross-linking occurs primarily via coordination between oxygen atoms of the pendant arsenic acid group and PtII, while secondary noncovalent interactions are proposed to provide further structural integrity and stability. Importantly, the hydrogels demonstrate potential self-healing properties, while the nature of the cross-linking promotes deep penetration of water into the loosely cross-linked networks. Finally, preliminary qualitative antimicrobial evaluation conducted via disk diffusion assay indicates that P4-Pt is active against Gram-negative (uropathogenic Escherichia coli CFT073 and Escherichia coli K12MG1655) and Gram-positive (Bacillus subtilis and Staphylococcus aureus USA 300 JE2) bacterial strains. Overall, the combination of polymeric arsenical scaffolds with PtII results in the formation of cross-linked networks generating soft, strong, and self-healing hydrogels with tunable stiffness and elasticity and preliminary indications of antimicrobial potential.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"25 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143915554","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

Change in Magnetic Order in NiPS3 Single Crystals Induced by a Molecular Intercalation 分子插层诱导NiPS3单晶磁序的变化

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2025-05-07 DOI: 10.1021/acs.chemmater.4c02724

Nirman Chakraborty, Adi Harchol, Beatriz Costa Arnold, Kusha Sharma, Diksha Prabhu Gaonkar, Azhar Abu-Hariri, Rajesh Kumar Yadav, Muhamed Dawod, Anna Eyal, Yaron Amouyal, Thomas Brumme, Thomas Heine, Doron Naveh, Efrat Lifshitz

{"title":"Change in Magnetic Order in NiPS3 Single Crystals Induced by a Molecular Intercalation","authors":"Nirman Chakraborty, Adi Harchol, Beatriz Costa Arnold, Kusha Sharma, Diksha Prabhu Gaonkar, Azhar Abu-Hariri, Rajesh Kumar Yadav, Muhamed Dawod, Anna Eyal, Yaron Amouyal, Thomas Brumme, Thomas Heine, Doron Naveh, Efrat Lifshitz","doi":"10.1021/acs.chemmater.4c02724","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c02724","url":null,"abstract":"Intercalation is a robust method for tuning the physical properties of a vast number of van der Waals (vdW) materials. However, the prospects of using intercalation to modify magnetism in van der Waals (vdW) systems and the associated mechanisms have not been adequately studied. In this work, we modulated magnetic order in XY antiferromagnet NiPS3 single crystals by introducing pyridine molecules into the vdW’s gap under different thermal conditions. X-ray diffraction measurements indicated pronounced changes in the lattice parameter β, while magnetization measurements at in-plane and out-of-plane configurations exposed reversal trends in the crystals’ Néel temperatures through intercalation/deintercalation processes. The changes in magnetic ordering were also supported by three-dimensional thermal diffusivity experiments. The preferred orientation of the pyridine dipoles within the vdW gaps was deciphered via polarized Raman spectroscopy. The results highlighted the relationship between the preferential alignment of the intercalants, thermal transport, and crystallographic disorder, along with the modulation of anisotropy in the magnetic order. DFT + U calculations indicated that the varying interlayer exchange interactions, regulated by intercalants, were responsible for modulating samples’ magnetic ordering. The study uncovers the possible merit of intercalation for manipulating spin orientations in spin electronics and advanced quantum devices.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"8 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-05-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143915552","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

Ionic Mobility in Energy Materials: Through the Lens of Quasielastic Neutron Scattering 能量材料中的离子迁移：通过准弹性中子散射透镜

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2025-05-06 DOI: 10.1021/acs.chemmater.5c0023810.1021/acs.chemmater.5c00238

Bettina Schwaighofer*, Miguel A. Gonzalez, Mark R. Johnson, John S. O. Evans and Ivana Radosavljević Evans*,

{"title":"Ionic Mobility in Energy Materials: Through the Lens of Quasielastic Neutron Scattering","authors":"Bettina Schwaighofer*, Miguel A. Gonzalez, Mark R. Johnson, John S. O. Evans and Ivana Radosavljević Evans*, ","doi":"10.1021/acs.chemmater.5c0023810.1021/acs.chemmater.5c00238","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c00238https://doi.org/10.1021/acs.chemmater.5c00238","url":null,"abstract":"Many energy-related materials rely on ionic migration for their function. Examples include the flow of ions in battery or fuel cell electrolytes or the coupled flow of ions and electrons in electrodes and membrane materials. As such, understanding, controlling, and improving ionic migration is a major focus of modern materials science. Significant and invaluable insight into the structure of materials and the collective motion of their atoms (phonons) is routinely obtained by elastic (diffraction) and inelastic (INS) neutron scattering methods. Here we focus on quasielastic neutron scattering (QENS) which can give unique atomic-level information on dynamics in the solid state. QENS can be used to measure the length- and time-scales of both local and long-range ionic motion and to give detailed insight into migration pathways. The length- and time-scales probed are comparable to computational techniques such as molecular dynamics, meaning that QENS can help test and validate theory. The information provided is also highly complementary to techniques such as tracer diffusion measurements, conductivity measurements, impedance studies, and solid-state NMR. We provide an introduction to the theory and experimental methods for QENS, presenting the concepts in a language accessible to materials chemists. We then review the insights given by QENS studies on energy materials that show oxide, sodium, and lithium ion migration in the solid state.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 10","pages":"3575–3593 3575–3593"},"PeriodicalIF":7.2,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://pubs.acs.org/doi/epdf/10.1021/acs.chemmater.5c00238","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144137595","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}

引用次数: 0

Ionic Mobility in Energy Materials: Through the Lens of Quasielastic Neutron Scattering 能量材料中的离子迁移：通过准弹性中子散射透镜

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2025-05-06 DOI: 10.1021/acs.chemmater.5c00238

Bettina Schwaighofer, Miguel A. Gonzalez, Mark R. Johnson, John S. O. Evans, Ivana Radosavljević Evans

{"title":"Ionic Mobility in Energy Materials: Through the Lens of Quasielastic Neutron Scattering","authors":"Bettina Schwaighofer, Miguel A. Gonzalez, Mark R. Johnson, John S. O. Evans, Ivana Radosavljević Evans","doi":"10.1021/acs.chemmater.5c00238","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c00238","url":null,"abstract":"Many energy-related materials rely on ionic migration for their function. Examples include the flow of ions in battery or fuel cell electrolytes or the coupled flow of ions and electrons in electrodes and membrane materials. As such, understanding, controlling, and improving ionic migration is a major focus of modern materials science. Significant and invaluable insight into the structure of materials and the collective motion of their atoms (phonons) is routinely obtained by elastic (diffraction) and inelastic (INS) neutron scattering methods. Here we focus on quasielastic neutron scattering (QENS) which can give unique atomic-level information on dynamics in the solid state. QENS can be used to measure the length- and time-scales of both local and long-range ionic motion and to give detailed insight into migration pathways. The length- and time-scales probed are comparable to computational techniques such as molecular dynamics, meaning that QENS can help test and validate theory. The information provided is also highly complementary to techniques such as tracer diffusion measurements, conductivity measurements, impedance studies, and solid-state NMR. We provide an introduction to the theory and experimental methods for QENS, presenting the concepts in a language accessible to materials chemists. We then review the insights given by QENS studies on energy materials that show oxide, sodium, and lithium ion migration in the solid state.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"47 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143910746","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

La Doping ATaO3 (A = Li, Na, K) to Improve Performance for Photocatalytic Pollutant Degradation La掺杂ATaO3 （A = Li, Na， K）提高光催化污染物降解性能

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2025-05-06 DOI: 10.1021/acs.chemmater.4c0344310.1021/acs.chemmater.4c03443

Rachael K. Matthews, Huong T. L. Nguyen, Fengxu Yang, Tara L. Pukala, Jack D. Evans* and Cameron J. Shearer*,

{"title":"La Doping ATaO3 (A = Li, Na, K) to Improve Performance for Photocatalytic Pollutant Degradation","authors":"Rachael K. Matthews, Huong T. L. Nguyen, Fengxu Yang, Tara L. Pukala, Jack D. Evans* and Cameron J. Shearer*, ","doi":"10.1021/acs.chemmater.4c0344310.1021/acs.chemmater.4c03443","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03443https://doi.org/10.1021/acs.chemmater.4c03443","url":null,"abstract":"ATaO3 (A = Li, Na, K) photocatalysts are among the most efficient photocatalysts, and efficiency can be further improved by La doping. In this study, the effect of La doping on ATaO3 perovskites was explored for several A site elements. ATaO3 (A = Li, Na, K) nanoparticles were synthesized via a solid-state high temperature synthesis with varying La mol % doping (0–10%). Homogeneous La doping within NaTaO3 and KTaO3 bulk was achieved, with an additional single (at times double) atomic layer at the surface of the nanoparticles, as confirmed by scanning transmission electron microscopy. Doping in LiTaO3 was inhomogeneous and requires further development. Formation and surface energy calculations and corresponding Wulff shapes were correlated to these experimental observations, confirming the role of La dopants in the observed shape of these nanoparticles. Model pollutant photocatalytic reactions under flow conditions confirmed an increase in photocatalytic activity with La doping for all ATaO3, with the largest improvement observed for NaTaO3. The findings of this study highlight the effect of La doping in ATaO3 (A = Li, Na, K) perovskites to improve photocatalytic performance for various applications, including energy and pollutant degradation.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 10","pages":"3696–3708 3696–3708"},"PeriodicalIF":7.2,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"144137593","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

La Doping ATaO3 (A = Li, Na, K) to Improve Performance for Photocatalytic Pollutant Degradation La掺杂ATaO3 （A = Li, Na， K）提高光催化污染物降解性能

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2025-05-06 DOI: 10.1021/acs.chemmater.4c03443

Rachael K. Matthews, Huong T. L. Nguyen, Fengxu Yang, Tara L. Pukala, Jack D. Evans, Cameron J. Shearer

{"title":"La Doping ATaO3 (A = Li, Na, K) to Improve Performance for Photocatalytic Pollutant Degradation","authors":"Rachael K. Matthews, Huong T. L. Nguyen, Fengxu Yang, Tara L. Pukala, Jack D. Evans, Cameron J. Shearer","doi":"10.1021/acs.chemmater.4c03443","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c03443","url":null,"abstract":"ATaO3 (A = Li, Na, K) photocatalysts are among the most efficient photocatalysts, and efficiency can be further improved by La doping. In this study, the effect of La doping on ATaO3 perovskites was explored for several A site elements. ATaO3 (A = Li, Na, K) nanoparticles were synthesized via a solid-state high temperature synthesis with varying La mol % doping (0–10%). Homogeneous La doping within NaTaO3 and KTaO3 bulk was achieved, with an additional single (at times double) atomic layer at the surface of the nanoparticles, as confirmed by scanning transmission electron microscopy. Doping in LiTaO3 was inhomogeneous and requires further development. Formation and surface energy calculations and corresponding Wulff shapes were correlated to these experimental observations, confirming the role of La dopants in the observed shape of these nanoparticles. Model pollutant photocatalytic reactions under flow conditions confirmed an increase in photocatalytic activity with La doping for all ATaO3, with the largest improvement observed for NaTaO3. The findings of this study highlight the effect of La doping in ATaO3 (A = Li, Na, K) perovskites to improve photocatalytic performance for various applications, including energy and pollutant degradation.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"56 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-05-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143910745","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

Broadband Pyro-Phototronic Effect in Lead-Free Double Perovskite Crystal Enables UV-to-NIR and Polarization-Sensitive Detection 无铅双钙钛矿晶体的宽带热光电子效应使紫外-近红外和偏振敏感检测成为可能

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2025-05-05 DOI: 10.1021/acs.chemmater.5c00190

Xianmei Zhao, Wen Weng, Liwei Tang, Haojie Xu, Yu Ma, Hao Rong, Huaimin Ni, Jingtian Zhang, Junhua Luo, Zhihua Sun

{"title":"Broadband Pyro-Phototronic Effect in Lead-Free Double Perovskite Crystal Enables UV-to-NIR and Polarization-Sensitive Detection","authors":"Xianmei Zhao, Wen Weng, Liwei Tang, Haojie Xu, Yu Ma, Hao Rong, Huaimin Ni, Jingtian Zhang, Junhua Luo, Zhihua Sun","doi":"10.1021/acs.chemmater.5c00190","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c00190","url":null,"abstract":"Broadband spectral detection holds a significant promise for diverse applications in environmental monitoring, infrared sensing, and biomedicine. However, the photoresponsive ranges of most photoactive materials are often limited by the intrinsic optical bandgap, which predominantly focuses on the ultraviolet and visible spectral region, thus hindering their broadband optical applications. Therefore, achieving high-performance broadband spectral photodetection is essential for advancing various cutting-edge technologies. In this study, we have obtained a lead-free double perovskite (FPEA)4AgBiI8 (1, FPEA+ is p-fluorophenethylammonium), which has strong structural polarity and a narrow bandgap (Eg) of ∼1.80 eV. The π–π stacking of interlayer FPEA+ cations creates a robust interlayer connection that contributes to the growth of high-quality single crystals. Notably, the inherent polarity of 1 allows a broadband pyro-phototronic effect that covers a wide spectral range from the ultraviolet (UV, 377 nm) to the near-infrared (NIR, 2000 nm) region, breaking the limitation of its optical bandgap. This unique pyro-phototronic effect significantly enhances the photoelectric performance of 1, of which the photopyroelectric peak current at 637 nm illumination is 427% larger than the photovoltaic current. Additionally, combining the advantages of structural anisotropy and pyro-phototronic effect, the crystal-based device of 1 creates superior polarization-sensitive photodetection behaviors. This study not only enriches the portfolio of photoactive perovskite candidates but also provides an effective strategy for assembling high-performance optoelectronic devices.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"58 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-05-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143905533","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

Broadband Pyro-Phototronic Effect in Lead-Free Double Perovskite Crystal Enables UV-to-NIR and Polarization-Sensitive Detection 无铅双钙钛矿晶体的宽带热光电子效应使紫外-近红外和偏振敏感检测成为可能

IF 7.2 2区材料科学

Chemistry of Materials Pub Date : 2025-05-05 DOI: 10.1021/acs.chemmater.5c0019010.1021/acs.chemmater.5c00190

Xianmei Zhao, Wen Weng*, Liwei Tang, Haojie Xu, Yu Ma, Hao Rong, Huaimin Ni, Jingtian Zhang, Junhua Luo and Zhihua Sun*,

{"title":"Broadband Pyro-Phototronic Effect in Lead-Free Double Perovskite Crystal Enables UV-to-NIR and Polarization-Sensitive Detection","authors":"Xianmei Zhao, Wen Weng*, Liwei Tang, Haojie Xu, Yu Ma, Hao Rong, Huaimin Ni, Jingtian Zhang, Junhua Luo and Zhihua Sun*, ","doi":"10.1021/acs.chemmater.5c0019010.1021/acs.chemmater.5c00190","DOIUrl":"https://doi.org/10.1021/acs.chemmater.5c00190https://doi.org/10.1021/acs.chemmater.5c00190","url":null,"abstract":"Broadband spectral detection holds a significant promise for diverse applications in environmental monitoring, infrared sensing, and biomedicine. However, the photoresponsive ranges of most photoactive materials are often limited by the intrinsic optical bandgap, which predominantly focuses on the ultraviolet and visible spectral region, thus hindering their broadband optical applications. Therefore, achieving high-performance broadband spectral photodetection is essential for advancing various cutting-edge technologies. In this study, we have obtained a lead-free double perovskite (FPEA)4AgBiI8 (1, FPEA+ is p-fluorophenethylammonium), which has strong structural polarity and a narrow bandgap (Eg) of ∼1.80 eV. The π–π stacking of interlayer FPEA+ cations creates a robust interlayer connection that contributes to the growth of high-quality single crystals. Notably, the inherent polarity of 1 allows a broadband pyro-phototronic effect that covers a wide spectral range from the ultraviolet (UV, 377 nm) to the near-infrared (NIR, 2000 nm) region, breaking the limitation of its optical bandgap. This unique pyro-phototronic effect significantly enhances the photoelectric performance of 1, of which the photopyroelectric peak current at 637 nm illumination is 427% larger than the photovoltaic current. Additionally, combining the advantages of structural anisotropy and pyro-phototronic effect, the crystal-based device of 1 creates superior polarization-sensitive photodetection behaviors. This study not only enriches the portfolio of photoactive perovskite candidates but also provides an effective strategy for assembling high-performance optoelectronic devices.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"37 9","pages":"3384–3391 3384–3391"},"PeriodicalIF":7.2,"publicationDate":"2025-05-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143934500","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

Electride-Induced Electron Transfer to Metal Phthalocyanines: A Mechanistic and Catalytic Study 电极诱导电子转移到金属酞菁：机制和催化研究

IF 8.6 2区材料科学

Chemistry of Materials Pub Date : 2025-05-04 DOI: 10.1021/acs.chemmater.4c02801

Zhilin Guo, Yijia Liu, Xinmeng Hu, Jiazhen Wu

{"title":"Electride-Induced Electron Transfer to Metal Phthalocyanines: A Mechanistic and Catalytic Study","authors":"Zhilin Guo, Yijia Liu, Xinmeng Hu, Jiazhen Wu","doi":"10.1021/acs.chemmater.4c02801","DOIUrl":"https://doi.org/10.1021/acs.chemmater.4c02801","url":null,"abstract":"Recent studies have indicated that electride materials with low work-function properties are effective electron donors in surface processes, particularly in catalysis. While the electron transfer from the electride to the active metal center is a crucial step, direct experimental observation of this process has yet to be achieved. Here, the integration of stable and redox-rich metal phthalocyanine complexes MII(Pc) with electrides successfully enabled the visualization of electron transfer through observable color changes, as well as ultraviolet–visible spectroscopy, X-ray photoelectron spectroscopy, and magnetic measurements. The proposed mechanism reveals that an electride donates electrons mainly to the 3d orbitals of divalent Co(II) or Fe(II) ions to produce monovalent Co(I) or Fe(I) anions, with less influence on ligand orbitals. Furthermore, the resulting MPc@electride composite can effectively trigger methyl methacrylate polymerization reactions with high conversions, which cannot be achieved by pure MII(Pc) or electrides alone. This study provides an effective electron donation route for designing catalysts with low-valence transition metals.","PeriodicalId":33,"journal":{"name":"Chemistry of Materials","volume":"280 1","pages":""},"PeriodicalIF":8.6,"publicationDate":"2025-05-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143905534","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