Yutian Qin, Jing Du, Qingyun Zhang, Chuanqi Cheng, Zefei Dong, Qi Zhang, Shaopeng Li, Jun Guo, Zhiyong Tang, Meiting Zhao
Imide covalent organic frameworks (COFs) are considered promising materials in various fields due to their exceptional stability, large surface area, and high porosity. However, current synthesis methods of imide COFs typically involve complex vacuum operations, large amounts of solvents, and long reaction times at high temperatures, limiting their scalability for industrial production. Herein, a facile self-accelerated strategy is developed for rapid, low-cost, and large-scale synthesis of eight imide COFs (SACOFs) under solvent-free, vacuum-free, and low-temperature conditions. Mechanistic studies reveal that the self-accelerated synthesis is driven by the self-generated water under atmospheric conditions, which accelerates the reversible self-healing of disordered polymers, ultimately leading to the rapid synthesis of highly crystalline COFs. Notably, the only additive required besides the COF monomers is o-substituted benzoic acid, a small amount of which is grafted onto the imide COFs, enabling their straightforward functionalization. Thiol-functionalized SACOFs are synthesized as supports for anchoring Pd nanoparticles. The as-prepared Pd@SACOFs exhibit high activity and selectivity in the hydrogenation of substituted nitrobenzene due to the surface modulation of Pd by thiol groups. The self-accelerated synthetic strategy enables rapid, low-cost, and large-scale production of imide COFs, potentially paving the way for their transition from laboratory research to commercial applications.
{"title":"Rapid and Large-Scale Synthesis of High-Crystalline Imide Covalent Organic Frameworks Accelerated by Self-Generated Water","authors":"Yutian Qin, Jing Du, Qingyun Zhang, Chuanqi Cheng, Zefei Dong, Qi Zhang, Shaopeng Li, Jun Guo, Zhiyong Tang, Meiting Zhao","doi":"10.1002/adma.202419515","DOIUrl":"https://doi.org/10.1002/adma.202419515","url":null,"abstract":"Imide covalent organic frameworks (COFs) are considered promising materials in various fields due to their exceptional stability, large surface area, and high porosity. However, current synthesis methods of imide COFs typically involve complex vacuum operations, large amounts of solvents, and long reaction times at high temperatures, limiting their scalability for industrial production. Herein, a facile self-accelerated strategy is developed for rapid, low-cost, and large-scale synthesis of eight imide COFs (SACOFs) under solvent-free, vacuum-free, and low-temperature conditions. Mechanistic studies reveal that the self-accelerated synthesis is driven by the self-generated water under atmospheric conditions, which accelerates the reversible self-healing of disordered polymers, ultimately leading to the rapid synthesis of highly crystalline COFs. Notably, the only additive required besides the COF monomers is <i>o</i>-substituted benzoic acid, a small amount of which is grafted onto the imide COFs, enabling their straightforward functionalization. Thiol-functionalized SACOFs are synthesized as supports for anchoring Pd nanoparticles. The as-prepared Pd@SACOFs exhibit high activity and selectivity in the hydrogenation of substituted nitrobenzene due to the surface modulation of Pd by thiol groups. The self-accelerated synthetic strategy enables rapid, low-cost, and large-scale production of imide COFs, potentially paving the way for their transition from laboratory research to commercial applications.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"20 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-02-12","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143393872","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Shane Scott, Maria Villiou, Federico Colombo, Angeles De la Cruz-García, Leon Tydecks, Lotta Toelke, Katharina Siemsen, Christine Selhuber-Unkel
Cells are highly responsive to changes in their mechanical environment, influencing processes such as stem cell differentiation and tumor progression. To meet the growing demand for materials used for high throughput mechanotransduction studies, simple means of dynamically adjusting the environmental viscoelasticity of cell cultures are needed. Here, a novel method is presented to dynamically and reversibly control the viscoelasticity of naturally derived polymer hydrogels through interactions with poly (ethylene glycol) (PEG). Interactions between PEG and hydrogel polymers, possibly involving hydrogen bonding, stiffen the hydrogel matrices. By dynamically changing the PEG concentration of the solution in which polymer hydrogels are incubated, their viscoelastic properties are adjusted, which in turn affects cell adhesion and cytoskeletal organization. Importantly, this effects is reversible, providing a cost-effective and simple strategy for dynamically adjusting the viscoelasticity of polymer hydrogels. This method holds promise for applications in mechanobiology, biomedicine, and the life sciences.
{"title":"Dynamic and Reversible Tuning of Hydrogel Viscoelasticity by Transient Polymer Interactions for Controlling Cell Adhesion","authors":"Shane Scott, Maria Villiou, Federico Colombo, Angeles De la Cruz-García, Leon Tydecks, Lotta Toelke, Katharina Siemsen, Christine Selhuber-Unkel","doi":"10.1002/adma.202408616","DOIUrl":"https://doi.org/10.1002/adma.202408616","url":null,"abstract":"Cells are highly responsive to changes in their mechanical environment, influencing processes such as stem cell differentiation and tumor progression. To meet the growing demand for materials used for high throughput mechanotransduction studies, simple means of dynamically adjusting the environmental viscoelasticity of cell cultures are needed. Here, a novel method is presented to dynamically and reversibly control the viscoelasticity of naturally derived polymer hydrogels through interactions with poly (ethylene glycol) (PEG). Interactions between PEG and hydrogel polymers, possibly involving hydrogen bonding, stiffen the hydrogel matrices. By dynamically changing the PEG concentration of the solution in which polymer hydrogels are incubated, their viscoelastic properties are adjusted, which in turn affects cell adhesion and cytoskeletal organization. Importantly, this effects is reversible, providing a cost-effective and simple strategy for dynamically adjusting the viscoelasticity of polymer hydrogels. This method holds promise for applications in mechanobiology, biomedicine, and the life sciences.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"78 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143394031","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Bei Li, Yan Tan, Josh Haipeng Lei, Min Deng, Xinwang Yu, Xinyi Wang, Lek Man Lei, Lin He, Chu-Xia Deng, Yunlu Dai
Failures of radiotherapy (RT) in adaptive antitumor immunomodulation often associate with recruited tissue-repairing macrophages. Although training these macrophages to phagocytose post-RT cancer cells reverses their protumoral performance, engulfed tumor antigens are severely underrated. In fact, regulating the processing and presentation of tumor antigens, a key determinant of tumor immunogenicity, can fundamentally affect adaptive immune responses. Here it is reported that a simple Alum-like adjuvant (MgAl-based hydrotalcite, bLDH) improves radioimmunotherapy via inducing antigen cross-presentation by macrophages, independent of phenotypes. It is identified that cytidine monophosphate guanosine oligodeoxynucleotide engenders macrophages to phagocytose irradiated cancer cells. However, as semiprofessional antigen-presenting cells, macrophages possess powerful proteolytic function that is detrimental to antigen presentation. The administration of alkaline bLDH intriguingly relieves the activity of phagolysosomal proteases with acidic pH optima by preventing phagosomal acidification resulting from the vacuolar-type ATPase proton pump. The adjuvant-modulated phagolysosomes thus limit antigen degradation and enhance tumor antigen cross-presentation over tenfold. To examine from an in vivo breast tumor model, trained macrophages successfully cross-prime antigen-specific CD8+ T cells and curb RT-associated metastasis. The findings propose to pay close attention to the effect of adjuvants on precision immunotherapy and highlight the positive contribution of cross-presenting macrophages in radioimmunotherapy.
{"title":"Alkaline Adjuvant Regulates Proteolytic Activity of Macrophages for Antigen Cross-Presentation and Potentiates Radioimmunotherapy","authors":"Bei Li, Yan Tan, Josh Haipeng Lei, Min Deng, Xinwang Yu, Xinyi Wang, Lek Man Lei, Lin He, Chu-Xia Deng, Yunlu Dai","doi":"10.1002/adma.202416690","DOIUrl":"https://doi.org/10.1002/adma.202416690","url":null,"abstract":"Failures of radiotherapy (RT) in adaptive antitumor immunomodulation often associate with recruited tissue-repairing macrophages. Although training these macrophages to phagocytose post-RT cancer cells reverses their protumoral performance, engulfed tumor antigens are severely underrated. In fact, regulating the processing and presentation of tumor antigens, a key determinant of tumor immunogenicity, can fundamentally affect adaptive immune responses. Here it is reported that a simple Alum-like adjuvant (MgAl-based hydrotalcite, bLDH) improves radioimmunotherapy via inducing antigen cross-presentation by macrophages, independent of phenotypes. It is identified that cytidine monophosphate guanosine oligodeoxynucleotide engenders macrophages to phagocytose irradiated cancer cells. However, as semiprofessional antigen-presenting cells, macrophages possess powerful proteolytic function that is detrimental to antigen presentation. The administration of alkaline bLDH intriguingly relieves the activity of phagolysosomal proteases with acidic pH optima by preventing phagosomal acidification resulting from the vacuolar-type ATPase proton pump. The adjuvant-modulated phagolysosomes thus limit antigen degradation and enhance tumor antigen cross-presentation over tenfold. To examine from an in vivo breast tumor model, trained macrophages successfully cross-prime antigen-specific CD8<sup>+</sup> T cells and curb RT-associated metastasis. The findings propose to pay close attention to the effect of adjuvants on precision immunotherapy and highlight the positive contribution of cross-presenting macrophages in radioimmunotherapy.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"161 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143393873","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Muhammad Imran, Da Bin Kim, Pan Xia, Francisco Yarur Villanueva, Benjamin Rehl, Joao M. Pina, Yanjiang Liu, Yangning Zhang, Oleksandr Voznyy, Eugenia Kumacheva, Sjoerd Hoogland, Edward H. Sargent
InSb colloidal quantum dots (CQDs) hold promise in short-wave infrared sensing; however, their synthesis presents ongoing challenges, particularly in achieving precise size control – this is the result of poorly controlled reactivity among the precursors. Herein, the use of alkyl-phosphine and amine-based organic additives to control the reactivity of In and Sb precursors during the nucleation and growth of CQDs is developed. This interplay between organic additive and precursors enables the synthesis of InSb CQDs having narrowed size distributions; and bandgaps tunable across the 1.2–1.5 µm spectral range; all this leading to peak-to-valley ratios >1.4 in absorption spectra. The CQDs are surface-terminated with a mixture of oleylamine, halides, and oxide-like species, and this hinders ligand exchange reactions and subsequent integration into photodiodes. We therefore resurface the CQDs with alkanethiols, displacing the native ligands via an acid-base mechanism, an approach that removes oxide species. Using a layer-by-layer fabrication process, the ligands of the resurfaced InSb CQDs are exchanged with short organic and halide ligands and incorporated films into n-i-p photodiode structures. The resultant devices exhibit a detectivity of 10¹2 Jones, an external quantum efficiency (EQE) of 33% at 1380 nm, and T90 operating stability of >19 h under continuous illuminated operation.
{"title":"Control Over Metal-Halide Reactivity Enables Uniform Growth of InSb Colloidal Quantum Dots for Enhanced SWIR Light Detection","authors":"Muhammad Imran, Da Bin Kim, Pan Xia, Francisco Yarur Villanueva, Benjamin Rehl, Joao M. Pina, Yanjiang Liu, Yangning Zhang, Oleksandr Voznyy, Eugenia Kumacheva, Sjoerd Hoogland, Edward H. Sargent","doi":"10.1002/adma.202420273","DOIUrl":"https://doi.org/10.1002/adma.202420273","url":null,"abstract":"InSb colloidal quantum dots (CQDs) hold promise in short-wave infrared sensing; however, their synthesis presents ongoing challenges, particularly in achieving precise size control – this is the result of poorly controlled reactivity among the precursors. Herein, the use of alkyl-phosphine and amine-based organic additives to control the reactivity of In and Sb precursors during the nucleation and growth of CQDs is developed. This interplay between organic additive and precursors enables the synthesis of InSb CQDs having narrowed size distributions; and bandgaps tunable across the 1.2–1.5 µm spectral range; all this leading to peak-to-valley ratios >1.4 in absorption spectra. The CQDs are surface-terminated with a mixture of oleylamine, halides, and oxide-like species, and this hinders ligand exchange reactions and subsequent integration into photodiodes. We therefore resurface the CQDs with alkanethiols, displacing the native ligands via an acid-base mechanism, an approach that removes oxide species. Using a layer-by-layer fabrication process, the ligands of the resurfaced InSb CQDs are exchanged with short organic and halide ligands and incorporated films into <i>n-i-p</i> photodiode structures. The resultant devices exhibit a detectivity of 10¹<sup>2</sup> Jones, an external quantum efficiency (EQE) of 33% at 1380 nm, and <i>T<sub>90</sub></i> operating stability of >19 h under continuous illuminated operation.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"30 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143393874","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Minwook Yoon, Yunkyu Park, Hyeji Sim, Hee Ryeung Kwon, Yujeong Lee, Ho Won Jang, Si-Young Choi, Junwoo Son
Light-driven energy conversion devices call for the atomic-level manipulation of defects associated with electronic states in solids. However, previous approaches to produce oxygen vacancy (VO) as a source of sub-bandgap energy levels have hampered the precise control of the distribution and concentration of VO. Here, a new strategy to spatially confine VO at the homo-interfaces is demonstrated by exploiting the sequential growth of anatase TiO2 under dissimilar thermodynamic conditions. Remarkably, metallic behavior with high carrier density and electron mobility is observed after sequential growth of the TiO2 films under low pressure and temperature (L-TiO2) on top of high-quality anatase TiO2 epitaxial films (H-TiO2), despite the insulating properties of L-TiO2 and H-TiO2 single layers. Multiple characterizations elucidate that the VO layer is geometrically confined within 4 unit cells at the interface, along with low-temperature crystallization of upper L-TiO2 films; this 2D VO layer is responsible for the formation of in-gap states, promoting photocarrier lifetime (≈300%) and light absorption. These results suggest a synthetic strategy to locally confine functional defects and emphasize how sub-bandgap energy levels in the confined imperfections influence the kinetics of light-driven catalytic reactions.
{"title":"2D Vacancy Confinement in Anatase TiO2 for Enhanced Photocatalytic Activities","authors":"Minwook Yoon, Yunkyu Park, Hyeji Sim, Hee Ryeung Kwon, Yujeong Lee, Ho Won Jang, Si-Young Choi, Junwoo Son","doi":"10.1002/adma.202413062","DOIUrl":"https://doi.org/10.1002/adma.202413062","url":null,"abstract":"Light-driven energy conversion devices call for the atomic-level manipulation of defects associated with electronic states in solids. However, previous approaches to produce oxygen vacancy (<i>V<sub>O</sub></i>) as a source of sub-bandgap energy levels have hampered the precise control of the distribution and concentration of <i>V<sub>O</sub></i>. Here, a new strategy to spatially confine <i>V<sub>O</sub></i> at the homo-interfaces is demonstrated by exploiting the sequential growth of anatase TiO<sub>2</sub> under dissimilar thermodynamic conditions. Remarkably, metallic behavior with high carrier density and electron mobility is observed after sequential growth of the TiO<sub>2</sub> films under low pressure and temperature (L-TiO<sub>2</sub>) on top of high-quality anatase TiO<sub>2</sub> epitaxial films (H-TiO<sub>2</sub>), despite the insulating properties of L-TiO<sub>2</sub> and H-TiO<sub>2</sub> single layers. Multiple characterizations elucidate that the <i>V<sub>O</sub></i> layer is geometrically confined within 4 unit cells at the interface, along with low-temperature crystallization of upper L-TiO<sub>2</sub> films; this 2D <i>V<sub>O</sub></i> layer is responsible for the formation of in-gap states, promoting photocarrier lifetime (≈300%) and light absorption. These results suggest a synthetic strategy to locally confine functional defects and emphasize how sub-bandgap energy levels in the confined imperfections influence the kinetics of light-driven catalytic reactions.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"10 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143393875","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Zhengqi Xiao, Yang Zou, Zhanxiang Chen, Jingsheng Miao, Yuntao Qiu, Zhongyan Huang, Xiaosong Cao, Xiaojun Peng, Chuluo Yang
The hyperfluorescence (HF) technology holds great promise for the development of high-quality organic light-emitting diodes (OLEDs) for their excellent color purity, high efficiency, and low-efficiency roll-off. Sensitizer plays a crucial role in the performance of HF devices. However, designing sensitizers with simultaneous high photoluminescence quantum yield (PLQY), rapid radiative decay (kr), and fast reverse intersystem crossing rate (kRISC) poses a great challenge, particularly for the thermally activated delayed fluorescence (TADF) sensitizers targeting deep-blue HF device. Herein, by introducing a boron-containing multi-resonance-type acceptor into the multi-tert-butyl-carbazole encapsulated benzene molecular skeleton, two TADF emitters featuring hybridized multi-channel charge-transfer pathways, including short-range multi-resonance, weakened through-bond, and compact face-to-face through-space charge-transfer. Benefiting from the rational molecular design, the proof-of-concept sensitizers exhibit simultaneous rapid kr of 5.3 × 107 s−1, fast kRISC up to 5.9 × 105 s−1, a PQLY of near-unity, as well as ideal deep-blue emission in both solution and film. Consequently, the corresponding deep-blue HF devices not only achieve chromaticity coordinates that fully comply with the latest BT. 2020 standards, but also showcase record-high maximum external quantum efficiencies nearing 40%, along with suppressed efficiency roll-off.
{"title":"Deep-Blue OLEDs with BT. 2020 Blue Gamut, External Quantum Efficiency Approaching 40%","authors":"Zhengqi Xiao, Yang Zou, Zhanxiang Chen, Jingsheng Miao, Yuntao Qiu, Zhongyan Huang, Xiaosong Cao, Xiaojun Peng, Chuluo Yang","doi":"10.1002/adma.202419601","DOIUrl":"https://doi.org/10.1002/adma.202419601","url":null,"abstract":"The hyperfluorescence (HF) technology holds great promise for the development of high-quality organic light-emitting diodes (OLEDs) for their excellent color purity, high efficiency, and low-efficiency roll-off. Sensitizer plays a crucial role in the performance of HF devices. However, designing sensitizers with simultaneous high photoluminescence quantum yield (PLQY), rapid radiative decay (<i>k</i><sub>r</sub>), and fast reverse intersystem crossing rate (<i>k</i><sub>RISC</sub>) poses a great challenge, particularly for the thermally activated delayed fluorescence (TADF) sensitizers targeting deep-blue HF device. Herein, by introducing a boron-containing multi-resonance-type acceptor into the multi-<i>tert</i>-butyl-carbazole encapsulated benzene molecular skeleton, two TADF emitters featuring hybridized multi-channel charge-transfer pathways, including short-range multi-resonance, weakened through-bond, and compact face-to-face through-space charge-transfer. Benefiting from the rational molecular design, the proof-of-concept sensitizers exhibit simultaneous rapid <i>k</i><sub>r</sub> of 5.3 × 10<sup>7</sup> s<sup>−1</sup>, fast <i>k</i><sub>RISC</sub> up to 5.9 × 10<sup>5</sup> s<sup>−1</sup>, a PQLY of near-unity, as well as ideal deep-blue emission in both solution and film. Consequently, the corresponding deep-blue HF devices not only achieve chromaticity coordinates that fully comply with the latest BT. 2020 standards, but also showcase record-high maximum external quantum efficiencies nearing 40%, along with suppressed efficiency roll-off.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"16 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143394034","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The pursuit of sustainable, high-performance organic ultralong room temperature phosphorescence (OURTP) materials with stimulus-responsive properties presents a significant and enticing yet formidable challenge. Herein, an efficient strategy to confining boric acid-based compounds into biomass macrocycle γ-cyclodextrin through multiple interactions is developed, enabling the construction of high-performance and multicolor OURTP doped systems. The synergistic effects of strong hydrogen bonding, C─O─B covalent cross-linking, and host–guest encapsulation significantly suppress non-radiative transition, culminating in an extraordinary lifetime and excellent phosphorescence quantum yield of 4.65 s and 32.8%, respectively, which are far superior to reported biomass RTP materials. Additionally, merging biomass macrocycle with phosphors contributes to multiple stimulus responses, overcoming the inherent limitations of degradation and recycling of organic RTP compounds, and dynamically modulating RTP signals through multiple-stimulus responses, achieving the integration of multifunctional dynamic data processing techniques. This work will provide a direction for new environmentally friendly and potentially commercially available stimulus-responsive OURTP materials.
{"title":"High-Performance Organic Ultralong Room Temperature Phosphorescence Based on Biomass Macrocycle","authors":"Zhenyi He, Jinming Song, Chunli Li, Zizhao Huang, Wenbin Liu, Xiang Ma","doi":"10.1002/adma.202418506","DOIUrl":"https://doi.org/10.1002/adma.202418506","url":null,"abstract":"The pursuit of sustainable, high-performance organic ultralong room temperature phosphorescence (OURTP) materials with stimulus-responsive properties presents a significant and enticing yet formidable challenge. Herein, an efficient strategy to confining boric acid-based compounds into biomass macrocycle γ-cyclodextrin through multiple interactions is developed, enabling the construction of high-performance and multicolor OURTP doped systems. The synergistic effects of strong hydrogen bonding, C─O─B covalent cross-linking, and host–guest encapsulation significantly suppress non-radiative transition, culminating in an extraordinary lifetime and excellent phosphorescence quantum yield of 4.65 s and 32.8%, respectively, which are far superior to reported biomass RTP materials. Additionally, merging biomass macrocycle with phosphors contributes to multiple stimulus responses, overcoming the inherent limitations of degradation and recycling of organic RTP compounds, and dynamically modulating RTP signals through multiple-stimulus responses, achieving the integration of multifunctional dynamic data processing techniques. This work will provide a direction for new environmentally friendly and potentially commercially available stimulus-responsive OURTP materials.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"41 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385875","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pragyan Jha, Nikolai Mukhin, Arup Ghorai, Hamed Morshedian, Richard B. Canty, Fernando Delgado-Licona, Emily E. Brown, Austin J. Pyrch, Felix N. Castellano, Milad Abolhasani
Over the past decade, lead halide perovskite (LHP) nanocrystals (NCs) have attracted significant attention due to their tunable optoelectronic properties for next-generation printed photonic and electronic devices. High-energy photons in the presence of haloalkanes provide a scalable and sustainable pathway for precise bandgap engineering of LHP NCs via photo-induced anion exchange reaction (PIAER) facilitated by in situ generated halide anions. However, the mechanisms driving photo-induced bandgap engineering in LHP NCs remain not fully understood. This study elucidates the underlying PIAER mechanisms of LHP NCs through an advanced microfluidic platform. Additionally, the first instance of a PIAER, transforming CsPbBr3 NCs into high-performing CsPbI3 NCs, with the assistance of a thiol-based additive is reported. Utilizing an intensified photo-flow microreactor accelerates the anion exchange rate 3.5-fold, reducing material consumption 100-fold compared to conventional batch processes. It is demonstrated that CsPbBr3 NCs act as photocatalysts, driving oxidative bond cleavage in dichloromethane and promoting the photodissociation of 1-iodopropane using high-energy photons. Furthermore, it is demonstrated that a thiol-based additive plays a dual role: surface passivation, which enhances the photoluminescence quantum yield, and facilitates the PIAER. These findings pave the way for the tailored design of perovskite-based optoelectronic materials.
{"title":"Photo-Induced Bandgap Engineering of Metal Halide Perovskite Quantum Dots In Flow","authors":"Pragyan Jha, Nikolai Mukhin, Arup Ghorai, Hamed Morshedian, Richard B. Canty, Fernando Delgado-Licona, Emily E. Brown, Austin J. Pyrch, Felix N. Castellano, Milad Abolhasani","doi":"10.1002/adma.202419668","DOIUrl":"https://doi.org/10.1002/adma.202419668","url":null,"abstract":"Over the past decade, lead halide perovskite (LHP) nanocrystals (NCs) have attracted significant attention due to their tunable optoelectronic properties for next-generation printed photonic and electronic devices. High-energy photons in the presence of haloalkanes provide a scalable and sustainable pathway for precise bandgap engineering of LHP NCs via photo-induced anion exchange reaction (PIAER) facilitated by in situ generated halide anions. However, the mechanisms driving photo-induced bandgap engineering in LHP NCs remain not fully understood. This study elucidates the underlying PIAER mechanisms of LHP NCs through an advanced microfluidic platform. Additionally, the first instance of a PIAER, transforming CsPbBr<sub>3</sub> NCs into high-performing CsPbI<sub>3</sub> NCs, with the assistance of a thiol-based additive is reported. Utilizing an intensified photo-flow microreactor accelerates the anion exchange rate 3.5-fold, reducing material consumption 100-fold compared to conventional batch processes. It is demonstrated that CsPbBr<sub>3</sub> NCs act as photocatalysts, driving oxidative bond cleavage in dichloromethane and promoting the photodissociation of 1-iodopropane using high-energy photons. Furthermore, it is demonstrated that a thiol-based additive plays a dual role: surface passivation, which enhances the photoluminescence quantum yield, and facilitates the PIAER. These findings pave the way for the tailored design of perovskite-based optoelectronic materials.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"10 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143394030","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Mechanically stable and structurally homogeneous lithium–electrolyte interfacial layers are crucial in stabilizing lithium (Li) anodes for practical Li metal batteries. Herein, an ultrathin (≈84 nm) and robust artificial protective layer is constructed with reactive two-dimensional (2D) molecular brushes as building blocks. The artificial protective layer can in situ react with underlying Li metal to produce a nanoscale poly(lithium styrenesulfonate)-grafted graphene oxide (GO-g-PSSLi) layer on the outermost surface and an infinite Li–Ag solid solution in the anode. The nanoscale GO-g-PSSLi layer well integrates a large number of single Li-ion conducting PSSLi chains and 2D robust GO backbones, thereby enabling molecular-level homogeneous and fast Li-ion diffusion as well as remarkable mechanical strength. Meanwhile, the simultaneously formed Li–Ag solid solution is beneficial for rapid Li transport in the anode to reduce the Li nucleation barrier and facilitate homogeneous deposition of Li. With such artificial protective layers, a prototype pouch cell with a thin Li metal anode (50 µm) and a high-loading cathode (21.6 mg cm−2) delivers an impressive cycle life of over 350 cycles with 69% capacity retention under harsh conditions. Remarkably, ultrahigh charging power density of 456 W kg−1 and energy density of 325 Wh kg−1 can be simultaneously achieved in an Ah-level pouch cell.
{"title":"Robust Nanoscale Anode Protective Layers toward Fast-Charge High-Energy-Density Lithium Metal Batteries","authors":"Chuanfa Li, Yin Cui, Shenghao Lin, Pengwei Ma, Yiwei Ji, Zongheng Cen, Guofang Yu, Shimei Li, Shaohong Liu, Dingcai Wu","doi":"10.1002/adma.202416377","DOIUrl":"https://doi.org/10.1002/adma.202416377","url":null,"abstract":"Mechanically stable and structurally homogeneous lithium–electrolyte interfacial layers are crucial in stabilizing lithium (Li) anodes for practical Li metal batteries. Herein, an ultrathin (≈84 nm) and robust artificial protective layer is constructed with reactive two-dimensional (2D) molecular brushes as building blocks. The artificial protective layer can in situ react with underlying Li metal to produce a nanoscale poly(lithium styrenesulfonate)-grafted graphene oxide (GO-<i>g</i>-PSSLi) layer on the outermost surface and an infinite Li–Ag solid solution in the anode. The nanoscale GO-<i>g</i>-PSSLi layer well integrates a large number of single Li-ion conducting PSSLi chains and 2D robust GO backbones, thereby enabling molecular-level homogeneous and fast Li-ion diffusion as well as remarkable mechanical strength. Meanwhile, the simultaneously formed Li–Ag solid solution is beneficial for rapid Li transport in the anode to reduce the Li nucleation barrier and facilitate homogeneous deposition of Li. With such artificial protective layers, a prototype pouch cell with a thin Li metal anode (50 µm) and a high-loading cathode (21.6 mg cm<sup>−2</sup>) delivers an impressive cycle life of over 350 cycles with 69% capacity retention under harsh conditions. Remarkably, ultrahigh charging power density of 456 W kg<sup>−1</sup> and energy density of 325 Wh kg<sup>−1</sup> can be simultaneously achieved in an Ah-level pouch cell.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"57 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143385874","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Teng Zhang, Stanislaw Wozniak, Ghazi Sarwat Syed, Piergiulio Mannocci, Matteo Farronato, Daniele Ielmini, Abu Sebastian, Yuchao Yang
In the era of relentless data generation and dynamic information streams, the demand for efficient and robust temporal signal analysis has intensified across diverse domains such as healthcare, finance, and telecommunications. This perspective study explores the unfolding landscape of emerging materials and computing paradigms that are reshaping the way temporal signals are analyzed and interpreted. Traditional signal processing techniques often fall short when confronted with the intricacies of time-varying data, prompting the exploration of innovative approaches. The rise of emerging materials and devices empowers real-time analysis by processing temporal signals in situ, mitigating latency concerns. Through this perspective, the untapped potential of emerging materials and computing paradigms for temporal signal analysis is highlighted, offering valuable insights into both challenges and opportunities. Standing on the cusp of a new era in computing, understanding and harnessing these paradigms is pivotal for unraveling the complexities embedded within the temporal dimensions of data, propelling signal analysis into realms previously deemed inaccessible.
{"title":"Emerging Materials and Computing Paradigms for Temporal Signal Analysis","authors":"Teng Zhang, Stanislaw Wozniak, Ghazi Sarwat Syed, Piergiulio Mannocci, Matteo Farronato, Daniele Ielmini, Abu Sebastian, Yuchao Yang","doi":"10.1002/adma.202408566","DOIUrl":"https://doi.org/10.1002/adma.202408566","url":null,"abstract":"In the era of relentless data generation and dynamic information streams, the demand for efficient and robust temporal signal analysis has intensified across diverse domains such as healthcare, finance, and telecommunications. This perspective study explores the unfolding landscape of emerging materials and computing paradigms that are reshaping the way temporal signals are analyzed and interpreted. Traditional signal processing techniques often fall short when confronted with the intricacies of time-varying data, prompting the exploration of innovative approaches. The rise of emerging materials and devices empowers real-time analysis by processing temporal signals in situ, mitigating latency concerns. Through this perspective, the untapped potential of emerging materials and computing paradigms for temporal signal analysis is highlighted, offering valuable insights into both challenges and opportunities. Standing on the cusp of a new era in computing, understanding and harnessing these paradigms is pivotal for unraveling the complexities embedded within the temporal dimensions of data, propelling signal analysis into realms previously deemed inaccessible.","PeriodicalId":114,"journal":{"name":"Advanced Materials","volume":"12 1","pages":""},"PeriodicalIF":29.4,"publicationDate":"2025-02-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143394037","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":1,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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