Pub Date : 2024-08-05DOI: 10.1016/j.mtchem.2024.102233
Nikiwe Mhlanga, Ntsoaki Mphuthi, Hendriëtte Van der Walt, Sanele Nyembe, Teboho Mokhena, Lucky Sikhwivhilu
Global health continues to be under threat evidenced by the recent surge of Covid-19 that crippled the world's biosecurity. Prevention, diagnosis, treatment and management of diseases are crucial in maintaining global health. Nanostructures and nanoparticles merited by a plethora of outstanding properties are cementing themselves in nanomedicine. The account examines their possible application in imaging diagnostics using the different modalities: magnetic resonance, optical imaging, ultrasonic molecular imaging, photoacoustic imaging, X-ray computed tomography and nuclear molecular imaging. The nanostructures are proposed as the next-generation contrast agents for enhanced imaging purposes. Hence, their stability, body clearance, biocompatibility and blood half-life are highlighted in this review. The next generation of proposed nanostructure-based contrast agents is not devoid of challenges. Multimodal imaging and engineered nanostructure composites are proposed mitigations in pursuit of biocompatible, blood pools, and enhanced imaging contrast agents with reasonable body clearance.
{"title":"Nanostructures and nanoparticles as medical diagnostic imaging contrast agents: A review","authors":"Nikiwe Mhlanga, Ntsoaki Mphuthi, Hendriëtte Van der Walt, Sanele Nyembe, Teboho Mokhena, Lucky Sikhwivhilu","doi":"10.1016/j.mtchem.2024.102233","DOIUrl":"https://doi.org/10.1016/j.mtchem.2024.102233","url":null,"abstract":"Global health continues to be under threat evidenced by the recent surge of Covid-19 that crippled the world's biosecurity. Prevention, diagnosis, treatment and management of diseases are crucial in maintaining global health. Nanostructures and nanoparticles merited by a plethora of outstanding properties are cementing themselves in nanomedicine. The account examines their possible application in imaging diagnostics using the different modalities: magnetic resonance, optical imaging, ultrasonic molecular imaging, photoacoustic imaging, X-ray computed tomography and nuclear molecular imaging. The nanostructures are proposed as the next-generation contrast agents for enhanced imaging purposes. Hence, their stability, body clearance, biocompatibility and blood half-life are highlighted in this review. The next generation of proposed nanostructure-based contrast agents is not devoid of challenges. Multimodal imaging and engineered nanostructure composites are proposed mitigations in pursuit of biocompatible, blood pools, and enhanced imaging contrast agents with reasonable body clearance.","PeriodicalId":18353,"journal":{"name":"Materials Today Chemistry","volume":"95 1","pages":""},"PeriodicalIF":7.3,"publicationDate":"2024-08-05","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141939652","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}
Pub Date : 2024-08-03DOI: 10.1016/j.mtchem.2024.102224
Miaomiao Chen, Hailong Xu, Xiaoyu Liang, Huili Zhao, Xinkui Wang, Min Ji, Min Wang
Frustrated Lewis pairs (FLPs) have demonstrated remarkable efficacy in metal-free hydrogenation, yet necessitate rigorous anhydrous reaction conditions. To address this concern, we propose a novel approach to enhance the water resistance of FLP by establishing a hydrophobic microenvironment. The inclusion of B(CF) within a MIL-101 framework, enveloped by hydrophobic polydimethylsiloxane (PDMS) coating, facilitates the in-situ formation of FLP in a solvent of 1,4-dioxane. The hydrophobic PDMS effectively prevents the ingress of water into the MOF nanocages, while simultaneously enabling the diffusion of 1,4-dioxane into the MOF nanocages for FLP formation. Consequently, the as-prepared FLP/MIL-101@PDMS composite exhibits superior water tolerance in the hydrogenation of benzaldehyde and can be utilized directly in commercially available solvents without necessitating stringent inert conditions. Remarkably, FLP/MIL-101@PDMS showcases unparalleled water tolerance even in the presence of 15 equivalents of water relative to B(CF). This research introduces innovative concepts for designing water-tolerant FLP.
{"title":"Hydrophobic MIL-101@PDMS composite confined Frustrated Lewis pairs: Excellent water-tolerance emerged in the hydrogenation of carbonyl compounds","authors":"Miaomiao Chen, Hailong Xu, Xiaoyu Liang, Huili Zhao, Xinkui Wang, Min Ji, Min Wang","doi":"10.1016/j.mtchem.2024.102224","DOIUrl":"https://doi.org/10.1016/j.mtchem.2024.102224","url":null,"abstract":"Frustrated Lewis pairs (FLPs) have demonstrated remarkable efficacy in metal-free hydrogenation, yet necessitate rigorous anhydrous reaction conditions. To address this concern, we propose a novel approach to enhance the water resistance of FLP by establishing a hydrophobic microenvironment. The inclusion of B(CF) within a MIL-101 framework, enveloped by hydrophobic polydimethylsiloxane (PDMS) coating, facilitates the in-situ formation of FLP in a solvent of 1,4-dioxane. The hydrophobic PDMS effectively prevents the ingress of water into the MOF nanocages, while simultaneously enabling the diffusion of 1,4-dioxane into the MOF nanocages for FLP formation. Consequently, the as-prepared FLP/MIL-101@PDMS composite exhibits superior water tolerance in the hydrogenation of benzaldehyde and can be utilized directly in commercially available solvents without necessitating stringent inert conditions. Remarkably, FLP/MIL-101@PDMS showcases unparalleled water tolerance even in the presence of 15 equivalents of water relative to B(CF). This research introduces innovative concepts for designing water-tolerant FLP.","PeriodicalId":18353,"journal":{"name":"Materials Today Chemistry","volume":"58 1","pages":""},"PeriodicalIF":7.3,"publicationDate":"2024-08-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141939653","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}
Advancing the performance of NiFe catalytic systems for oxygen evolution reaction (OER) is challenging, notably upon incorporating a third transition metal to create a trimetallic configuration. This study introduces a Cu-doped NiFe electrocatalyst, synthesized via a streamlined redeposition technique. The catalyst exhibits a Tafel slope of 38 mV dec and a low overpotential of 248 mV at a current density of 100 mA cm, plus a 2.5-fold boost in intrinsic activity. Density Functional Theory (DFT) and spectroscopic analyses demonstrate that Cu doping refines the electronic structure, enhancing charge density around the Fermi level and multiplying active OER sites. The Cu1Fe6Ni18 catalyst features robust Cu–O and Fe–O bond interactions, enhancing charge transport and OER kinetics. Our research elucidates the synergistic effects of Cu and Fe in a trimetallic system, offering an impactful approach to elevate trimetallic catalyst performance.
提高镍铁催化系统在氧进化反应（OER）中的性能具有挑战性，尤其是在加入第三种过渡金属以形成三金属构型时。本研究介绍了一种铜掺杂的镍铁合金电催化剂，它是通过简化的再沉积技术合成的。该催化剂的塔菲尔斜率为 38 mV dec，电流密度为 100 mA cm 时过电位低至 248 mV，而且内在活性提高了 2.5 倍。密度泛函理论（DFT）和光谱分析表明，掺杂铜可改善电子结构，提高费米级附近的电荷密度，并使活性 OER 位点成倍增加。Cu1Fe6Ni18 催化剂具有强大的 Cu-O 和 Fe-O 键相互作用，增强了电荷传输和 OER 动力学。我们的研究阐明了铜和铁在三金属体系中的协同效应，为提高三金属催化剂性能提供了一种有影响力的方法。
{"title":"Copper-doped nickel–iron metal/metal oxide electrode with improved performance by promoting synergistic effects in the oxygen evolution reaction","authors":"Xiaoyu Gong, Jiawei Ge, Jun Qi, Honghe Ding, Leijie Zhang, Peiyu Ma, Zuohuan Chen, Nian Zhang, Jilong Xu, Lijuan Zhu, Jiaxiang Lu, Guiqiang Li, Junjie Ge, Yifan Ye","doi":"10.1016/j.mtchem.2024.102225","DOIUrl":"https://doi.org/10.1016/j.mtchem.2024.102225","url":null,"abstract":"Advancing the performance of NiFe catalytic systems for oxygen evolution reaction (OER) is challenging, notably upon incorporating a third transition metal to create a trimetallic configuration. This study introduces a Cu-doped NiFe electrocatalyst, synthesized via a streamlined redeposition technique. The catalyst exhibits a Tafel slope of 38 mV dec and a low overpotential of 248 mV at a current density of 100 mA cm, plus a 2.5-fold boost in intrinsic activity. Density Functional Theory (DFT) and spectroscopic analyses demonstrate that Cu doping refines the electronic structure, enhancing charge density around the Fermi level and multiplying active OER sites. The Cu1Fe6Ni18 catalyst features robust Cu–O and Fe–O bond interactions, enhancing charge transport and OER kinetics. Our research elucidates the synergistic effects of Cu and Fe in a trimetallic system, offering an impactful approach to elevate trimetallic catalyst performance.","PeriodicalId":18353,"journal":{"name":"Materials Today Chemistry","volume":"179 1","pages":""},"PeriodicalIF":7.3,"publicationDate":"2024-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141880535","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}
Pub Date : 2024-08-01DOI: 10.1016/j.mtchem.2024.102193
Marta Santos, Igor Tiago, Marcos Mariz, Paula Ferreira, Susana Alarico
This study presents the development of a polyurethane-based sensor, with potential applications in biotechnology and biomedicine, focusing on prevention and non-invasive diagnostic.
{"title":"Development of a sugar-based polyurethane foam colorimetric sensor for E. coli detection","authors":"Marta Santos, Igor Tiago, Marcos Mariz, Paula Ferreira, Susana Alarico","doi":"10.1016/j.mtchem.2024.102193","DOIUrl":"https://doi.org/10.1016/j.mtchem.2024.102193","url":null,"abstract":"This study presents the development of a polyurethane-based sensor, with potential applications in biotechnology and biomedicine, focusing on prevention and non-invasive diagnostic.","PeriodicalId":18353,"journal":{"name":"Materials Today Chemistry","volume":"3 1","pages":""},"PeriodicalIF":7.3,"publicationDate":"2024-08-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142204543","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}
Pub Date : 2024-07-31DOI: 10.1016/j.mtchem.2024.102234
Pierre Frangville, Arvin Sain Tanwar, Shiv Kumar, Michel Gelbcke, Nathalie Wauthoz, Sergey Basov, Margriet J. Van Bael, Kristof Van Hecke, Franck Meyer
The present study delves into the synthesis and characterization of multi-stimuli responsive polymers, demonstrating their sensitivity towards magnetic field, pH level, light irradiation, and electron-rich species through halogen bonding (XB). Detailed X-ray analyses of two azobenzene derivatives, each incorporating a tetrafluoroiodobenzene group, provided the compelling evidence of engagement of the building blocks in the formation of halogen bonds. Interestingly, the investigation of an ammonium analog, featuring a tetrahalogenoferrate(III) anion, not only showcased a magnetic response even upheld its ability to undergo isomerization under UV irradiation. These functional properties were subsequently harnessed in the form of multi-responsive compounds through the random quaternization of poly(2-(N,-dimethylamino) ethyl methacrylate) (PDMAEMA), and by employing varying proportions of XB-donor dye (8, 11, 15, 21, and 43 %) followed by magnetic anion exchange. Leveraging the presence of free ternary amino groups and diazobenzene moieties, the resulting polymers demonstrated pronounced sensitivity towards a variation of pH and UV light stimuli, while a careful modulation of magnetic susceptibility was found to be directly proportional to the degree of quaternization. An NMR titration, conducted using a synthetic intermediate, revealed the formation of I⋯Cl‾ interactions in the solution state, thereby underscoring the materials' sensitivity to electron-rich species. Moreover, the electron microscopic analysis displayed an alteration in morphology upon the application of a magnetic field and UV irradiation. Thus, the presented strategic framework offers an avenue for the development of multi-stimuli responsive materials for remotely controlled smart devices to act in response to a diverse set of four stimuli, and heralding a significant advancement in the realm of responsive material design.
{"title":"Sensing diversity in halogen-bonded multi-stimuli responsive materials: Light, pH, magnetism, and electron-rich species","authors":"Pierre Frangville, Arvin Sain Tanwar, Shiv Kumar, Michel Gelbcke, Nathalie Wauthoz, Sergey Basov, Margriet J. Van Bael, Kristof Van Hecke, Franck Meyer","doi":"10.1016/j.mtchem.2024.102234","DOIUrl":"https://doi.org/10.1016/j.mtchem.2024.102234","url":null,"abstract":"The present study delves into the synthesis and characterization of multi-stimuli responsive polymers, demonstrating their sensitivity towards magnetic field, pH level, light irradiation, and electron-rich species through halogen bonding (XB). Detailed X-ray analyses of two azobenzene derivatives, each incorporating a tetrafluoroiodobenzene group, provided the compelling evidence of engagement of the building blocks in the formation of halogen bonds. Interestingly, the investigation of an ammonium analog, featuring a tetrahalogenoferrate(III) anion, not only showcased a magnetic response even upheld its ability to undergo isomerization under UV irradiation. These functional properties were subsequently harnessed in the form of multi-responsive compounds through the random quaternization of poly(2-(N,-dimethylamino) ethyl methacrylate) (PDMAEMA), and by employing varying proportions of XB-donor dye (8, 11, 15, 21, and 43 %) followed by magnetic anion exchange. Leveraging the presence of free ternary amino groups and diazobenzene moieties, the resulting polymers demonstrated pronounced sensitivity towards a variation of pH and UV light stimuli, while a careful modulation of magnetic susceptibility was found to be directly proportional to the degree of quaternization. An NMR titration, conducted using a synthetic intermediate, revealed the formation of I⋯Cl‾ interactions in the solution state, thereby underscoring the materials' sensitivity to electron-rich species. Moreover, the electron microscopic analysis displayed an alteration in morphology upon the application of a magnetic field and UV irradiation. Thus, the presented strategic framework offers an avenue for the development of multi-stimuli responsive materials for remotely controlled smart devices to act in response to a diverse set of four stimuli, and heralding a significant advancement in the realm of responsive material design.","PeriodicalId":18353,"journal":{"name":"Materials Today Chemistry","volume":"74 1","pages":""},"PeriodicalIF":7.3,"publicationDate":"2024-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141880534","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}
Pub Date : 2024-07-31DOI: 10.1016/j.mtchem.2024.102232
Jiayao Wen, Susu Huang, Qiaoying Hu, Wei He, Zhijian Wei, Lei Wang, Jinghui Lu, Xuetian Yue, Shaojie Men, Chengxu Miao, Zhijing He, Xiaoye Yang, Guangxi Zhai, Junjie Li, Lei Ye
Biological contamination seriously restricts the development and application of medical devices, causing severe health threats and economic losses. Non-specific protein adhesion is generally considered to be the first step in biological contamination, and it is well acknowledged that hydrophilic surfaces can effectively reduce protein adsorption. Based on this principle, many anti-biofouling materials have been developed. In recent years, zwitterionic polymers with ultra-low protein adsorption and excellent biocompatibility have made them a research hotspot for the new generation of antifouling materials and attracted great attention in biomedical applications. The repeating unit carries a pair of opposite charges, and the whole molecule is electrically neutral, showing super-hydrophilic properties. Coating strategies are considered to be a promising solution to the biofouling of medical devices due to their low impact on substrates and their ability to adapt to a variety of complex surfaces. Therefore, the zwitterionic-based coating layer is the most effective way and promising candidate to solve biological contamination. In this review, we summarized the formation process of biological contamination, antifouling surface properties, up-to-date zwitterionic monomers, the strategies for non-fouling coating preparation, and their applications in biomedical fields.
{"title":"Recent advances in zwitterionic polymers-based non-fouling coating strategies for biomedical applications","authors":"Jiayao Wen, Susu Huang, Qiaoying Hu, Wei He, Zhijian Wei, Lei Wang, Jinghui Lu, Xuetian Yue, Shaojie Men, Chengxu Miao, Zhijing He, Xiaoye Yang, Guangxi Zhai, Junjie Li, Lei Ye","doi":"10.1016/j.mtchem.2024.102232","DOIUrl":"https://doi.org/10.1016/j.mtchem.2024.102232","url":null,"abstract":"Biological contamination seriously restricts the development and application of medical devices, causing severe health threats and economic losses. Non-specific protein adhesion is generally considered to be the first step in biological contamination, and it is well acknowledged that hydrophilic surfaces can effectively reduce protein adsorption. Based on this principle, many anti-biofouling materials have been developed. In recent years, zwitterionic polymers with ultra-low protein adsorption and excellent biocompatibility have made them a research hotspot for the new generation of antifouling materials and attracted great attention in biomedical applications. The repeating unit carries a pair of opposite charges, and the whole molecule is electrically neutral, showing super-hydrophilic properties. Coating strategies are considered to be a promising solution to the biofouling of medical devices due to their low impact on substrates and their ability to adapt to a variety of complex surfaces. Therefore, the zwitterionic-based coating layer is the most effective way and promising candidate to solve biological contamination. In this review, we summarized the formation process of biological contamination, antifouling surface properties, up-to-date zwitterionic monomers, the strategies for non-fouling coating preparation, and their applications in biomedical fields.","PeriodicalId":18353,"journal":{"name":"Materials Today Chemistry","volume":"42 1","pages":""},"PeriodicalIF":7.3,"publicationDate":"2024-07-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141880610","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}
Pub Date : 2024-07-30DOI: 10.1016/j.mtchem.2024.102226
Krishna Kumar Yadav, Marina M.S. Cabral-Pinto, Amel Gacem, Ahmed M. Fallatah, Balasubramani Ravindran, Shahabaldin Rezania, Jari S. Algethami, Lienda Bashier Eltayeb, Mohamed Abbas, Tasneem Hassan Al-shareef, Vandana Vinayak, Cao Truong Son, Maha Awjan Alreshidi, Joan Manuel Rodríguez-Díaz, Raad Z. Homod
In the contemporary period characterized by limited availability of water resources, the efficient treatment of wastewater is a fundamental requirement for the advancement of the economy. The development and implementation of modern wastewater treatment technologies that exhibit high efficiency and low capital requirements are of utmost importance. Currently, nanotechnology is a highly prioritized field of research in numerous nations because of its significant potential and economic implications. Nanotechnology has shown great potential in the field of water treatment and remediation. Through the utilization of different nanomaterials, water can be purified using various mechanisms. These mechanisms include the adsorption of heavy metals, dyes, and other contaminants, as well as the inactivation and elimination of pathogens. Additionally, nanotechnology enables the conversion of harmful materials into less harmful compounds, further enhancing its effectiveness in water treatment and remediation. This article aims to present a comprehensive review of contemporary advancements in nanotechnologies utilized for water and wastewater treatment. The discussed techniques include adsorption, photocatalytic water treatment methods such as nanoelectro-catalysts and Fenton catalysts, disinfection, nanosponges, nanomembrane, aerobic digestion, and core-shell plasmonic nanosensors. Furthermore, the article provides insights into the various opportunities, limitations, and future prospects associated with these advancements.
{"title":"Recent advances in the application of nanoparticle-based strategies for water remediation as a novel clean technology–A comprehensive review","authors":"Krishna Kumar Yadav, Marina M.S. Cabral-Pinto, Amel Gacem, Ahmed M. Fallatah, Balasubramani Ravindran, Shahabaldin Rezania, Jari S. Algethami, Lienda Bashier Eltayeb, Mohamed Abbas, Tasneem Hassan Al-shareef, Vandana Vinayak, Cao Truong Son, Maha Awjan Alreshidi, Joan Manuel Rodríguez-Díaz, Raad Z. Homod","doi":"10.1016/j.mtchem.2024.102226","DOIUrl":"https://doi.org/10.1016/j.mtchem.2024.102226","url":null,"abstract":"In the contemporary period characterized by limited availability of water resources, the efficient treatment of wastewater is a fundamental requirement for the advancement of the economy. The development and implementation of modern wastewater treatment technologies that exhibit high efficiency and low capital requirements are of utmost importance. Currently, nanotechnology is a highly prioritized field of research in numerous nations because of its significant potential and economic implications. Nanotechnology has shown great potential in the field of water treatment and remediation. Through the utilization of different nanomaterials, water can be purified using various mechanisms. These mechanisms include the adsorption of heavy metals, dyes, and other contaminants, as well as the inactivation and elimination of pathogens. Additionally, nanotechnology enables the conversion of harmful materials into less harmful compounds, further enhancing its effectiveness in water treatment and remediation. This article aims to present a comprehensive review of contemporary advancements in nanotechnologies utilized for water and wastewater treatment. The discussed techniques include adsorption, photocatalytic water treatment methods such as nanoelectro-catalysts and Fenton catalysts, disinfection, nanosponges, nanomembrane, aerobic digestion, and core-shell plasmonic nanosensors. Furthermore, the article provides insights into the various opportunities, limitations, and future prospects associated with these advancements.","PeriodicalId":18353,"journal":{"name":"Materials Today Chemistry","volume":"82 1","pages":""},"PeriodicalIF":7.3,"publicationDate":"2024-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141886893","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}
Pub Date : 2024-07-30DOI: 10.1016/j.mtchem.2024.102219
Xinhao Li, Chen Wang, Wenzheng Nan, Sikan Peng, Jin Liu, Shaojiu Yan
Polyether electrolytes, which possess benefits in terms of lithium salt solubility, compatibility with lithium metal, and material availability, are promising candidate materials for solid-state lithium metal batteries with high safety and specific energy. However, achieving stable cycling at high rates under room temperature conditions for high-voltage lithium metal solid-state batteries is a significant challenge. In this study, a polyether-based composite solid-state electrolyte was fabricated via in situ polymerization, and a novel polyether matrix (PDSi) was synthesized by copolymerization of 1,3-dioxolane (DOL) and 3-(glycidoxypropyl)triethoxysilane (GPTES). The triethoxysilicon groups of PDSi improve the antioxidant capacity of polyether and interact with anionic groups, thereby enabling a wide electrochemical window of 5.5 V and a high lithium-ion transference number t of 0.56 at room temperature. In addition, a prepared PDSi@LLZTO electrolyte with an asymmetric structure mitigated the side reaction between the LLZTO ceramic filler and lithium. Here, PDSi@LLZTO exhibited a lithium-ion transference number of 0.67 and ionic conductivity of 1.28 × 10 S cm at 20 °C. More importantly, the Li|PDSi@LLZTO|NCM523 cell demonstrated excellent capacity retention of 83.9 % after 200 cycles at a high-rate discharge of 3C. The proposed material and structure design provide a unique perspective for the development of an effective polymer-based electrolyte for high-voltage lithium metal batteries.
{"title":"Polyether-based composite solid-state electrolyte to realize stable high-rate cycling for high-voltage lithium metal batteries at room temperature","authors":"Xinhao Li, Chen Wang, Wenzheng Nan, Sikan Peng, Jin Liu, Shaojiu Yan","doi":"10.1016/j.mtchem.2024.102219","DOIUrl":"https://doi.org/10.1016/j.mtchem.2024.102219","url":null,"abstract":"Polyether electrolytes, which possess benefits in terms of lithium salt solubility, compatibility with lithium metal, and material availability, are promising candidate materials for solid-state lithium metal batteries with high safety and specific energy. However, achieving stable cycling at high rates under room temperature conditions for high-voltage lithium metal solid-state batteries is a significant challenge. In this study, a polyether-based composite solid-state electrolyte was fabricated via in situ polymerization, and a novel polyether matrix (PDSi) was synthesized by copolymerization of 1,3-dioxolane (DOL) and 3-(glycidoxypropyl)triethoxysilane (GPTES). The triethoxysilicon groups of PDSi improve the antioxidant capacity of polyether and interact with anionic groups, thereby enabling a wide electrochemical window of 5.5 V and a high lithium-ion transference number t of 0.56 at room temperature. In addition, a prepared PDSi@LLZTO electrolyte with an asymmetric structure mitigated the side reaction between the LLZTO ceramic filler and lithium. Here, PDSi@LLZTO exhibited a lithium-ion transference number of 0.67 and ionic conductivity of 1.28 × 10 S cm at 20 °C. More importantly, the Li|PDSi@LLZTO|NCM523 cell demonstrated excellent capacity retention of 83.9 % after 200 cycles at a high-rate discharge of 3C. The proposed material and structure design provide a unique perspective for the development of an effective polymer-based electrolyte for high-voltage lithium metal batteries.","PeriodicalId":18353,"journal":{"name":"Materials Today Chemistry","volume":"41 1","pages":""},"PeriodicalIF":7.3,"publicationDate":"2024-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141880606","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}
Developing high-performance broadband NIR (near-infrared) phosphors remains a crucial pursuit for the next-generation smart NIR light source. This study demonstrates the successful synthesis of BaCaMgSiO:Cr phosphors exhibiting exceptional broadband NIR emission a high-temperature solid-state reaction. Notably, the 0.03Cr doped composition, under 485 nm excitation, shines with a remarkable broadband emission spanning 700 nm–1100 nm and boasts a full width at half maximum (FWHM) of 134 nm. This work meticulously explores the intricate interplay between Cr doping concentration, temperature, crystal field strength, and the Huang-Rhys parameter, shedding light on the underlying luminescence mechanisms. Moreover, the BaCaMgSiO:0.03Cr phosphor exhibits exceptional thermal stability, retaining approximately 70 % of its integrated emission intensity at 425 K compared to room temperature. To further expand the excitation range, Eu was introduced as a co-dopant, successfully broadening the excitation spectrum to encompass nearly the entire ultraviolet–visible region (ranging from 250 nm to 750 nm). The presence of Eu→Cr energy transfer was elucidated, and the impact of Eu doping was thoroughly investigated. Moreover, the synthesized phosphor has been successfully integrated into a NIR phosphor-converted light-emitting diode (pc-LED), showcasing their potential application in the realms of night vision and NIR vascular imaging. These findings offer invaluable insights into Cr luminescence behavior and pave the way for the development of novel NIR phosphors with enhanced functionalities, propelling us closer to the realization of next-generation smart lighting solutions.
{"title":"Remarkable broadband NIR emission of BaCa2MgSi2O8:Cr3+ phosphors and Eu2+ co-doping modulation","authors":"Dejian Hou, Zaidong Chen, Rui Huang, Jianhong Dong, Wenxing Zhang, Hongliang Li, Huihong Lin, Jin-Yan Li, Lei Zhou, Mingmei Wu","doi":"10.1016/j.mtchem.2024.102214","DOIUrl":"https://doi.org/10.1016/j.mtchem.2024.102214","url":null,"abstract":"Developing high-performance broadband NIR (near-infrared) phosphors remains a crucial pursuit for the next-generation smart NIR light source. This study demonstrates the successful synthesis of BaCaMgSiO:Cr phosphors exhibiting exceptional broadband NIR emission a high-temperature solid-state reaction. Notably, the 0.03Cr doped composition, under 485 nm excitation, shines with a remarkable broadband emission spanning 700 nm–1100 nm and boasts a full width at half maximum (FWHM) of 134 nm. This work meticulously explores the intricate interplay between Cr doping concentration, temperature, crystal field strength, and the Huang-Rhys parameter, shedding light on the underlying luminescence mechanisms. Moreover, the BaCaMgSiO:0.03Cr phosphor exhibits exceptional thermal stability, retaining approximately 70 % of its integrated emission intensity at 425 K compared to room temperature. To further expand the excitation range, Eu was introduced as a co-dopant, successfully broadening the excitation spectrum to encompass nearly the entire ultraviolet–visible region (ranging from 250 nm to 750 nm). The presence of Eu→Cr energy transfer was elucidated, and the impact of Eu doping was thoroughly investigated. Moreover, the synthesized phosphor has been successfully integrated into a NIR phosphor-converted light-emitting diode (pc-LED), showcasing their potential application in the realms of night vision and NIR vascular imaging. These findings offer invaluable insights into Cr luminescence behavior and pave the way for the development of novel NIR phosphors with enhanced functionalities, propelling us closer to the realization of next-generation smart lighting solutions.","PeriodicalId":18353,"journal":{"name":"Materials Today Chemistry","volume":"16 1","pages":""},"PeriodicalIF":7.3,"publicationDate":"2024-07-30","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141880607","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}
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