Weixi Jiang, Xiaoting Wang, Hongjin An, Xun Guo, Li Chen, Luodan Yu, Yu Chen, Jianli Ren
Prompt removal of apoptotic cells via macrophage-mediated efferocytosis is an emerging approach for atherosclerosis treatment, because these diseased cells directly contribute to vascular inflammation and secondary necrosis in plaques. Despite blocking CD47 can restore impaired efferocytosis by inhibiting “don't eat me” signals, the currently available CD47 antibody (CD47-Ab)-based therapy may accelerate off-target clearance of healthy cells due to the ubiquitous expression of CD47 on viable cells. Here, a peptide-templated nanoassembly (PTna-1) engineered to induce synergistic enhancement of engulfment by macrophages is reported. Through self-assembled polypeptides with multiple functional motifs, the nanoassembly can specifically target p32-overexpressing macrophages and bind to the Ig-V-like domain of SIRPα but not to CD47, thereby normalizing intraplaque efferocytosis and alleviating persistent inflammation. Concurrently, disassembled PTna-1 released manganese porphyrins with photoacoustic/magnetic resonance imaging capability to suppress oxidative stress and synergistically enhance macrophage phagocytosis through the RhoA/ROCK1 pathway. Compared with CD47-Abs, PTna-1 promoted a more significant reduction in lesion area and plaque stabilization without affecting the incidence of anemia in atherosclerotic mice. Proteomic analysis revealed that PTna-1 treatment decreased the expression of inflammation-related proteins in plaques. Overall, these peptide-driven nanoassemblies employing a SIRPα-specific blockade strategy provide a distinct paradigm of pro-efferocytotic therapy for atherosclerosis.
{"title":"Enhanced Macrophages Engulfment by Peptide-Templated Nanoassemblies Targeting SIRPα and Suppressing Oxidative Stress for Atherosclerosis Pro-Efferocytotic Therapy","authors":"Weixi Jiang, Xiaoting Wang, Hongjin An, Xun Guo, Li Chen, Luodan Yu, Yu Chen, Jianli Ren","doi":"10.1002/adfm.202414017","DOIUrl":"https://doi.org/10.1002/adfm.202414017","url":null,"abstract":"Prompt removal of apoptotic cells via macrophage-mediated efferocytosis is an emerging approach for atherosclerosis treatment, because these diseased cells directly contribute to vascular inflammation and secondary necrosis in plaques. Despite blocking CD47 can restore impaired efferocytosis by inhibiting “don't eat me” signals, the currently available CD47 antibody (CD47-Ab)-based therapy may accelerate off-target clearance of healthy cells due to the ubiquitous expression of CD47 on viable cells. Here, a peptide-templated nanoassembly (PTna-1) engineered to induce synergistic enhancement of engulfment by macrophages is reported. Through self-assembled polypeptides with multiple functional motifs, the nanoassembly can specifically target p32-overexpressing macrophages and bind to the Ig-V-like domain of SIRPα but not to CD47, thereby normalizing intraplaque efferocytosis and alleviating persistent inflammation. Concurrently, disassembled PTna-1 released manganese porphyrins with photoacoustic/magnetic resonance imaging capability to suppress oxidative stress and synergistically enhance macrophage phagocytosis through the RhoA/ROCK1 pathway. Compared with CD47-Abs, PTna-1 promoted a more significant reduction in lesion area and plaque stabilization without affecting the incidence of anemia in atherosclerotic mice. Proteomic analysis revealed that PTna-1 treatment decreased the expression of inflammation-related proteins in plaques. Overall, these peptide-driven nanoassemblies employing a SIRPα-specific blockade strategy provide a distinct paradigm of pro-efferocytotic therapy for atherosclerosis.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"243 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142588351","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Zhiwei Chen, Hongru Zhou, Fanhao Kong, Zhaolin Dou, Jingxuan Yang, Min Wang
Photocatalysis has shown power in the valorization of biomass while controlling the selectivity is a long-standing goal and challenge, especially for the complex and reactive bio-polyols. The selectivity control of photocatalytic biopolyols reforming to formic acid (FA) or CO is realized via engineering the electrostatic field on TiO2 semiconductor. The electrostatic field is generated by surface modification with anion adsorbates, which can alter the trap states of photoexcited holes and regulate interfacial hole transfer to the surface-bound species, thereby strongly affecting photocatalytic activity. Taking formic acid dehydration as an example, a shallow trap of photoexcited holes on pristine TiO2 favors the dehydration of FA to CO, while a deep trap of photoexcited holes after introduced anion adsorbates makes FA stable. Based on this result, the selectivity is successfully tuned in the photocatalytic oxidation of biopolyols via controlling electrostatic field. A wide range of biopolyols can be selectively converted into FA or CO. This work presents an effective strategy to manipulate reaction pathways via generating electric field.
光催化技术已在生物质的价值化方面显示出强大的威力，而控制选择性则是一项长期的目标和挑战，尤其是对于复杂和反应性强的生物多元醇而言。光催化生物多元醇重整为甲酸（FA）或一氧化碳的选择性控制是通过在二氧化钛半导体上设计静电场来实现的。静电场是通过阴离子吸附剂的表面改性产生的，它可以改变光激发空穴的阱态，调节界面空穴向表面结合物种的转移，从而强烈影响光催化活性。以甲酸脱水为例，原始二氧化钛上的光激发空穴浅阱有利于甲酸脱水为 CO，而引入阴离子吸附剂后的光激发空穴深阱则使甲酸稳定。在此基础上，通过控制静电场成功地调整了生物多酚光催化氧化过程中的选择性。多种生物多元醇可被选择性地转化为 FA 或 CO。这项工作提出了一种通过产生电场来操纵反应途径的有效策略。
{"title":"Electrostatic Field Regulate Interfacial Hole Transfer for Photocatalytic Valorization of Biopolyols","authors":"Zhiwei Chen, Hongru Zhou, Fanhao Kong, Zhaolin Dou, Jingxuan Yang, Min Wang","doi":"10.1002/adfm.202418154","DOIUrl":"https://doi.org/10.1002/adfm.202418154","url":null,"abstract":"Photocatalysis has shown power in the valorization of biomass while controlling the selectivity is a long-standing goal and challenge, especially for the complex and reactive bio-polyols. The selectivity control of photocatalytic biopolyols reforming to formic acid (FA) or CO is realized via engineering the electrostatic field on TiO<sub>2</sub> semiconductor. The electrostatic field is generated by surface modification with anion adsorbates, which can alter the trap states of photoexcited holes and regulate interfacial hole transfer to the surface-bound species, thereby strongly affecting photocatalytic activity. Taking formic acid dehydration as an example, a shallow trap of photoexcited holes on pristine TiO<sub>2</sub> favors the dehydration of FA to CO, while a deep trap of photoexcited holes after introduced anion adsorbates makes FA stable. Based on this result, the selectivity is successfully tuned in the photocatalytic oxidation of biopolyols via controlling electrostatic field. A wide range of biopolyols can be selectively converted into FA or CO. This work presents an effective strategy to manipulate reaction pathways via generating electric field.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"91 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142588354","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Han Tian, Yanyu Hu, Jiajie Wu, Rixuan Wang, Jing Wang, Xixi Cai, Xu Chen, Yong He, Shaoyun Wang
3D printing of bio-hydrogel scaffolds are widely used in tissue regeneration. However, due to the ultra-soft properties of bio-hydrogels, it is hard to print them precisely. Here, crystal transduction 3D printing with high fidelity is proposed to address this challenge. A phase-transition bio-inks system with beeswax is developed for crystal transduction, which can accelerate energy consumption and induce soft bio-inks to quickly harden during printing. Interestingly, an interconnected porous hydrogel scaffold can be obtained after washing the crystal beeswax. The porous hydrogel scaffold demonstrated excellent biocompatibility and cell proliferation effect in vitro and is free from defense responses and immunogenicity in vivo. Muscle analog porous scaffolds constructed by high-fidelity 3D printing significantly improve the tissue function recovery of rats with muscle defects, compared with the conventional printed hydrogel with a non-matched shape. These structure-performance design rules create exciting opportunities to customize 3D-printed porous hydrogel scaffolds with high fidelity.
{"title":"Crystal Transduction 3D Printing of Bio-Hydrogels with High Fidelity and Order Micro Pores","authors":"Han Tian, Yanyu Hu, Jiajie Wu, Rixuan Wang, Jing Wang, Xixi Cai, Xu Chen, Yong He, Shaoyun Wang","doi":"10.1002/adfm.202415799","DOIUrl":"https://doi.org/10.1002/adfm.202415799","url":null,"abstract":"3D printing of bio-hydrogel scaffolds are widely used in tissue regeneration. However, due to the ultra-soft properties of bio-hydrogels, it is hard to print them precisely. Here, crystal transduction 3D printing with high fidelity is proposed to address this challenge. A phase-transition bio-inks system with beeswax is developed for crystal transduction, which can accelerate energy consumption and induce soft bio-inks to quickly harden during printing. Interestingly, an interconnected porous hydrogel scaffold can be obtained after washing the crystal beeswax. The porous hydrogel scaffold demonstrated excellent biocompatibility and cell proliferation effect in vitro and is free from defense responses and immunogenicity in vivo. Muscle analog porous scaffolds constructed by high-fidelity 3D printing significantly improve the tissue function recovery of rats with muscle defects, compared with the conventional printed hydrogel with a non-matched shape. These structure-performance design rules create exciting opportunities to customize 3D-printed porous hydrogel scaffolds with high fidelity.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"144 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142588355","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sandra M. Estévez, Zhiyong Wang, Tsai-Jung Liu, Gabriel Caballero, Fernando J. Urbanos, Ignacio Figueruelo-Campanero, Julia García-Pérez, Cristina Navío, Miroslav Polozij, Jianjun Zhang, Thomas Heine, Mariela Menghini, Daniel Granados, Xiliang Feng, Renhao Dong, Enrique Cánovas
Understanding charge transport properties of large-area single-layer 2D materials is crucial for the future development of novel optoelectronic devices. In this work, the synthesis and electrical characterization of large-area single-layers of Cu3BHT 2D conjugated coordination polymers are reported. The Cu3BHT are synthesized on the water surface by the Langmuir-Blodgett method and then transferred to SiO2/Si substrates with pre-patterned electrical contacts. Electrical measurements revealed ohmic responses across areas up to ≈1 cm2, with a mean resistance of approximately 53 ± 3 kΩ at a probe separation of 50 µm. Cooling and heating cycles show hysteresis in the electrical response, suggesting different current pathways are formed as the samples underwent structural-chemical changes during temperature sweeps. This hysteresis vanished after several cycles and the conductivity shows a stable exponential behavior as a function of temperature, suggesting that a temperature-dependent tunneling process is governing the conduction mechanism in the analyzed polycrystalline single-layer Cu3BHT samples. These results, together with density functional theory calculations and valence band X-ray photoelectron spectroscopy data suggest that the single-layer samples exhibit a semiconducting rather than a metallic behavior.
{"title":"Electrical Characterization of a Large-Area Single-Layer Cu3BHT 2D Conjugated Coordination Polymer","authors":"Sandra M. Estévez, Zhiyong Wang, Tsai-Jung Liu, Gabriel Caballero, Fernando J. Urbanos, Ignacio Figueruelo-Campanero, Julia García-Pérez, Cristina Navío, Miroslav Polozij, Jianjun Zhang, Thomas Heine, Mariela Menghini, Daniel Granados, Xiliang Feng, Renhao Dong, Enrique Cánovas","doi":"10.1002/adfm.202416717","DOIUrl":"https://doi.org/10.1002/adfm.202416717","url":null,"abstract":"Understanding charge transport properties of large-area single-layer 2D materials is crucial for the future development of novel optoelectronic devices. In this work, the synthesis and electrical characterization of large-area single-layers of Cu<sub>3</sub>BHT 2D conjugated coordination polymers are reported. The Cu<sub>3</sub>BHT are synthesized on the water surface by the Langmuir-Blodgett method and then transferred to SiO<sub>2</sub>/Si substrates with pre-patterned electrical contacts. Electrical measurements revealed ohmic responses across areas up to ≈1 cm<sup>2</sup>, with a mean resistance of approximately 53 ± 3 kΩ at a probe separation of 50 µm. Cooling and heating cycles show hysteresis in the electrical response, suggesting different current pathways are formed as the samples underwent structural-chemical changes during temperature sweeps. This hysteresis vanished after several cycles and the conductivity shows a stable exponential behavior as a function of temperature, suggesting that a temperature-dependent tunneling process is governing the conduction mechanism in the analyzed polycrystalline single-layer Cu<sub>3</sub>BHT samples. These results, together with density functional theory calculations and valence band X-ray photoelectron spectroscopy data suggest that the single-layer samples exhibit a semiconducting rather than a metallic behavior.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"8 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142588326","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hao Li, Jia Bin Niu, Long Gang Tao, Mei Chee Tan, Hong Yee Low
Carbon capture emerges as a pivotal decarbonization technology for addressing global warming challenges. Porous carbons, despite their cost-effectiveness and ease of regeneration for CO2 capture, typically exhibit limited capacity owing to insufficient adsorption sites. Here, nitrogen-doped porous carbons (NPCs) are introduced that overcome the prevalent trade-offs between specific surface area and N-doped content in NPCs fabrication through cascade reactions. The optimized NPC, which features hierarchical porosity ranging from ultra-micropores to macropores, shows a superior CO2 capture capacity of 4.46 mmol g−1, ranking in the top 10% of the reported NPCs. This capacity exceeds that of the NPC fabricated with the conventional method by 58% and surpasses the control porous carbon by 106%. Langmuir adsorption modeling and mathematic correlation analysis revealed that this enhanced capacity is attributed to significantly improved ultra-micropores volume and nitrogen-species content. Moreover, this optimized NPC demonstrates exceptional stability, preserving its adsorption performance over 110 adsorption–desorption cycles under simulated flue gas conditions. This research not only highlights the integration of templating and N-doping within NPCs fabrication but also offers an effective strategy to optimize porosity and nitrogen functionality in carbon materials, advancing beyond conventional methodologies.
{"title":"Cascade Reactions for Enhanced CO2 Capture: Concurrent Optimization of Porosity and N-Doping","authors":"Hao Li, Jia Bin Niu, Long Gang Tao, Mei Chee Tan, Hong Yee Low","doi":"10.1002/adfm.202415441","DOIUrl":"https://doi.org/10.1002/adfm.202415441","url":null,"abstract":"Carbon capture emerges as a pivotal decarbonization technology for addressing global warming challenges. Porous carbons, despite their cost-effectiveness and ease of regeneration for CO<sub>2</sub> capture, typically exhibit limited capacity owing to insufficient adsorption sites. Here, nitrogen-doped porous carbons (NPCs) are introduced that overcome the prevalent trade-offs between specific surface area and N-doped content in NPCs fabrication through cascade reactions. The optimized NPC, which features hierarchical porosity ranging from ultra-micropores to macropores, shows a superior CO<sub>2</sub> capture capacity of 4.46 mmol g<sup>−1</sup>, ranking in the top 10% of the reported NPCs. This capacity exceeds that of the NPC fabricated with the conventional method by 58% and surpasses the control porous carbon by 106%. Langmuir adsorption modeling and mathematic correlation analysis revealed that this enhanced capacity is attributed to significantly improved ultra-micropores volume and nitrogen-species content. Moreover, this optimized NPC demonstrates exceptional stability, preserving its adsorption performance over 110 adsorption–desorption cycles under simulated flue gas conditions. This research not only highlights the integration of templating and N-doping within NPCs fabrication but also offers an effective strategy to optimize porosity and nitrogen functionality in carbon materials, advancing beyond conventional methodologies.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"8 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142588349","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Junze Zhang, Tiandi Chen, Meng Zhu, Jian Lu, Xinlong Liu, Weiwei Sun, Mei Yi So, Bingang Xu
Fiber-based photochromic wearables have attracted growing attention in sustainable photo-patterning information displays, information security encryption, and optical data recording/storage. Molybdenum trioxide (MoO3) is one of the key photochromic materials that possesses good photochromic performance, nevertheless, it faces considerable challenges in preparing photochromic textiles with stable, scalable, and long color-retention properties. In this work, a new kind of fiber-based photochromic wearables is designed and developed by combining cotton fabric with a MoO3-based self-adhesive polymer network and long chain silyl group. The prepared photochromic wearable has exhibited excellent fatigue resistance and favorable reversibility (> 40 cycles), rapid light response (reach color saturation with a UV dose of 60 kJ m−2), outstanding color retention capability (> 90 days), and desirable biocompatibility (cell viability > 100%). In addition, the prepared photochromic textiles could maintain a fast light response and excellent color retention even after experiencing repeated washing (20 cycles). Moreover, the photo-patterning photochromic wearables are verified by resisting the deterioration of acid solution, alkali solution, and sweat (pH 2.0–9.0) as well as keeping clear patterns under sunlight irradiation. As a demonstration of the application, fiber-based photochromic wearables are made and employed for the sustainable applications of rewritable photo-patterning and information security encryption.
{"title":"Scalable, Fast Light-Responsive, and Excellent Color-Retention Fiber-Based Photochromic Wearables for Sustainable Photo-Patterning and Information Security Encryption","authors":"Junze Zhang, Tiandi Chen, Meng Zhu, Jian Lu, Xinlong Liu, Weiwei Sun, Mei Yi So, Bingang Xu","doi":"10.1002/adfm.202415622","DOIUrl":"https://doi.org/10.1002/adfm.202415622","url":null,"abstract":"Fiber-based photochromic wearables have attracted growing attention in sustainable photo-patterning information displays, information security encryption, and optical data recording/storage. Molybdenum trioxide (MoO<sub>3</sub>) is one of the key photochromic materials that possesses good photochromic performance, nevertheless, it faces considerable challenges in preparing photochromic textiles with stable, scalable, and long color-retention properties. In this work, a new kind of fiber-based photochromic wearables is designed and developed by combining cotton fabric with a MoO<sub>3</sub>-based self-adhesive polymer network and long chain silyl group. The prepared photochromic wearable has exhibited excellent fatigue resistance and favorable reversibility (> 40 cycles), rapid light response (reach color saturation with a UV dose of 60 kJ m<sup>−2</sup>), outstanding color retention capability (> 90 days), and desirable biocompatibility (cell viability > 100%). In addition, the prepared photochromic textiles could maintain a fast light response and excellent color retention even after experiencing repeated washing (20 cycles). Moreover, the photo-patterning photochromic wearables are verified by resisting the deterioration of acid solution, alkali solution, and sweat (pH 2.0–9.0) as well as keeping clear patterns under sunlight irradiation. As a demonstration of the application, fiber-based photochromic wearables are made and employed for the sustainable applications of rewritable photo-patterning and information security encryption.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"32 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142588350","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Zhenqian Ma, Jinyue Wang, Zhenliang Hao, Jingjie Dai, Xiangyu Zhu, He Zheng, Xiongjun Liu, Hailong Zhang, Zhaoping Lu
Because of the surge in the power density of electronic devices, there is an urgent need for improvements in the thermal conductivity of packaging materials. Nowadays, epoxy composites supplemented with thermally conductive fillers are widely used for this purpose, but unfortunately, none of them can satisfactorily meet industrial requirements. Herein, this article reports on a novel method to prepare well-shaped and highly ordered graphene-epoxy composite architecture; that is, the epoxy infiltrates into tubular graphene columns that have been restored to the high thermally conductive structure of graphene. As a result, the newly developed graphene-epoxy composite exhibits record-high thermal conductivity of 69.74 W m−1 K−1 with filler content of only 11.22 wt.%. The unprecedentedly high thermal conductivity stems from the construction of thermally conductive channels and restoration of the inherent π–π conjugate structure of graphene. These findings not only offer a breakthrough in packaging materials with significantly enhanced thermal conductivity but also provide a promising avenue for the development of other advanced graphene-added composites.
由于电子设备的功率密度急剧增加，因此迫切需要改善包装材料的导热性能。目前，添加导热填料的环氧树脂复合材料已被广泛应用，但遗憾的是，它们都无法满足工业要求。本文报告了一种制备形状良好且高度有序的石墨烯-环氧复合材料结构的新方法，即环氧渗入管状石墨烯柱中，恢复石墨烯的高导热结构。因此，新开发的石墨烯-环氧复合材料的热导率达到了创纪录的 69.74 W m-1 K-1，而填料含量仅为 11.22 wt.%。前所未有的高导热率源于导热通道的构建以及石墨烯固有的 π-π 共轭结构的恢复。这些发现不仅为具有显著增强导热性的包装材料提供了一个突破口，而且为开发其他添加石墨烯的先进复合材料提供了一个前景广阔的途径。
{"title":"Novel Graphene-Epoxy Composite with Aligned Architecture and Ultrahigh Thermal Conductivity","authors":"Zhenqian Ma, Jinyue Wang, Zhenliang Hao, Jingjie Dai, Xiangyu Zhu, He Zheng, Xiongjun Liu, Hailong Zhang, Zhaoping Lu","doi":"10.1002/adfm.202412534","DOIUrl":"https://doi.org/10.1002/adfm.202412534","url":null,"abstract":"Because of the surge in the power density of electronic devices, there is an urgent need for improvements in the thermal conductivity of packaging materials. Nowadays, epoxy composites supplemented with thermally conductive fillers are widely used for this purpose, but unfortunately, none of them can satisfactorily meet industrial requirements. Herein, this article reports on a novel method to prepare well-shaped and highly ordered graphene-epoxy composite architecture; that is, the epoxy infiltrates into tubular graphene columns that have been restored to the high thermally conductive structure of graphene. As a result, the newly developed graphene-epoxy composite exhibits record-high thermal conductivity of 69.74 W m<sup>−1</sup> K<sup>−1</sup> with filler content of only 11.22 wt.%. The unprecedentedly high thermal conductivity stems from the construction of thermally conductive channels and restoration of the inherent π–π conjugate structure of graphene. These findings not only offer a breakthrough in packaging materials with significantly enhanced thermal conductivity but also provide a promising avenue for the development of other advanced graphene-added composites.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"79 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142588346","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Marvin Skiba, Rebeka R. Reszegi, Yalan Huang, Sathi Roy, Jili Han, Dennis Brückner, Carlos Sanchez-Cano, Ying Zhao, Moustapha Hassan, Neus Feliu, Gerald Falkenberg, Wolfgang J. Parak
Selenium (Se) compounds hold promise as potential therapeutics for cancer due to their diverse biological functions and redox-regulating properties. In this study, the encapsulation of a hydrophobic selenium compound inside 5 µm sized biodegradable polyelectrolyte capsules consisting of poly-L-arginine and dextran is investigated. While the encapsulated form of the compound showed comparable cellular uptake and cytotoxicity as the free drug, e.g. no improved anti-cancer efficacy is achieved, the investigation yielded crucial insights. Utilizing subcellular resolution synchrotron X-ray fluorescence imaging (XFI), the intracellular location of the Se compound is successfully visualized by demonstrating the degradation of the capsules and the following redistribution of the compound, without exogenous labeling. By applying a quantitative fitting approach, the intracellular Se mass is determined to be 0.09 ± 0.01 pg after degradation of the carrier. This highlights the potential of XFI as a powerful tool for tracking intracellular dynamics of metal-based drugs, which may facilitate drug development in the clinic.
硒（Se）化合物具有多种生物功能和氧化还原调节特性，有望成为治疗癌症的潜在药物。在本研究中，研究人员将一种疏水性硒化合物封装在由聚-L-精氨酸和葡聚糖组成的 5 微米大小的可生物降解聚电解质胶囊中。虽然该化合物的封装形式显示出与游离药物相当的细胞摄取和细胞毒性，例如没有提高抗癌功效，但这项研究获得了重要的启示。利用亚细胞分辨率同步加速器 X 射线荧光成像技术（XFI），在没有外源标记的情况下，通过展示胶囊的降解和随后化合物的重新分布，成功地观察到 Se 化合物在细胞内的位置。通过定量拟合方法，确定载体降解后细胞内 Se 的质量为 0.09 ± 0.01 pg。这凸显了 XFI 作为一种追踪金属基药物细胞内动态的强大工具的潜力，可促进临床药物开发。
{"title":"Exploring the Intracellular Distribution of Se Compounds Delivered by Biodegradable Polyelectrolyte Capsules Using X-Ray Fluorescence Imaging","authors":"Marvin Skiba, Rebeka R. Reszegi, Yalan Huang, Sathi Roy, Jili Han, Dennis Brückner, Carlos Sanchez-Cano, Ying Zhao, Moustapha Hassan, Neus Feliu, Gerald Falkenberg, Wolfgang J. Parak","doi":"10.1002/adfm.202408539","DOIUrl":"https://doi.org/10.1002/adfm.202408539","url":null,"abstract":"Selenium (Se) compounds hold promise as potential therapeutics for cancer due to their diverse biological functions and redox-regulating properties. In this study, the encapsulation of a hydrophobic selenium compound inside 5 µm sized biodegradable polyelectrolyte capsules consisting of poly-L-arginine and dextran is investigated. While the encapsulated form of the compound showed comparable cellular uptake and cytotoxicity as the free drug, e.g. no improved anti-cancer efficacy is achieved, the investigation yielded crucial insights. Utilizing subcellular resolution synchrotron X-ray fluorescence imaging (XFI), the intracellular location of the Se compound is successfully visualized by demonstrating the degradation of the capsules and the following redistribution of the compound, without exogenous labeling. By applying a quantitative fitting approach, the intracellular Se mass is determined to be 0.09 ± 0.01 pg after degradation of the carrier. This highlights the potential of XFI as a powerful tool for tracking intracellular dynamics of metal-based drugs, which may facilitate drug development in the clinic.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"13 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142588347","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Pub Date : 2024-11-06DOI: 10.1016/j.ensm.2024.103892
Yingchun Yan, Zheng Liu, Weining Li, Fan Feng, Xinhou Yang, Bin Qi, Min Gong, Zhiyuan Li, Tong Wei, Zhuangjun Fan
Quasi-solid-state electrolytes (QSSEs) are regarded as the most promising alternative for next-generation battery technology due to the compatibility of assemble process and high safety. However, the rational design of solid hosts to ensure the high-efficiency utilization of tiny liquid electrolytes and the deep understanding of ion transport mechanisms at heterogeneous structures are still challenging. Herein, inspired by the ion transport in biological blood vessels, we propose a nitrogen vacancy modified glassy metal-organic framework (MOF) as Na-ion QSSEs host, which shows multilevel ions transport channels, isotropy property, and no grain boundaries. The vascularized glassy MOF enables the reasonable distribution of a small amount of solvent (14 wt.% (solvent as a percentage of QSSE by mass)) in both macro and microenvironments with specific functions, boosting the fast Na-ion transport (1.18 × 10−4 S cm–1, 30°C) and Na-ion transfer number (0.92), and homogeneous Na-ion nucleation/propagation even at -50°C. Meanwhile, the quasi-solid-state Na||Na3V2(PO4)3/C cell demonstrates excellent rate capability and long cycling stability (0.0288% capacity decay per cycle after 500 cycles). The bioinspired design of glassy MOF will shed light on new avenues for the development of energy storage and conversion.
准固态电解质（QSSE）因其组装工艺的兼容性和高安全性，被视为下一代电池技术最有前途的替代品。然而，如何合理设计固态宿主以确保高效利用微小的液态电解质，以及如何深入理解离子在异质结构中的传输机制，仍然是一项挑战。在此，我们受生物血管离子传输的启发，提出了一种氮空位修饰的玻璃态金属有机框架（MOF）作为纳离子 QSSEs 的宿主，它具有多级离子传输通道、各向同性和无晶界等特性。维管化的玻璃质 MOF 使少量溶剂（14 wt.%（溶剂占 QSSE 的质量百分比））在宏观和微观环境中合理分布，并具有特定功能，从而提高了 Na 离子的快速传输（1.18 × 10-4 S cm-1，30°C）和 Na 离子转移数（0.92），即使在 -50°C 下也能实现均匀的 Na 离子成核/扩散。同时，准固态 Na||Na3V2(PO4)3/C电池表现出卓越的速率能力和长期循环稳定性（500 次循环后每次循环的容量衰减为 0.0288%）。玻璃状 MOF 的生物启发设计将为能源存储和转换的发展提供新的途径。
{"title":"Bioinspired Design of Vascularized Glassy Metal-Organic Frameworks Electrolyte for Quasi-Solid-State Sodium Batteries","authors":"Yingchun Yan, Zheng Liu, Weining Li, Fan Feng, Xinhou Yang, Bin Qi, Min Gong, Zhiyuan Li, Tong Wei, Zhuangjun Fan","doi":"10.1016/j.ensm.2024.103892","DOIUrl":"https://doi.org/10.1016/j.ensm.2024.103892","url":null,"abstract":"Quasi-solid-state electrolytes (QSSEs) are regarded as the most promising alternative for next-generation battery technology due to the compatibility of assemble process and high safety. However, the rational design of solid hosts to ensure the high-efficiency utilization of tiny liquid electrolytes and the deep understanding of ion transport mechanisms at heterogeneous structures are still challenging. Herein, inspired by the ion transport in biological blood vessels, we propose a nitrogen vacancy modified glassy metal-organic framework (MOF) as Na-ion QSSEs host, which shows multilevel ions transport channels, isotropy property, and no grain boundaries. The vascularized glassy MOF enables the reasonable distribution of a small amount of solvent (14 wt.% (solvent as a percentage of QSSE by mass)) in both macro and microenvironments with specific functions, boosting the fast Na-ion transport (1.18 × 10<sup>−4</sup> S cm<sup>–1</sup>, 30°C) and Na-ion transfer number (0.92), and homogeneous Na-ion nucleation/propagation even at -50°C. Meanwhile, the quasi-solid-state Na||Na<sub>3</sub>V<sub>2</sub>(PO<sub>4</sub>)<sub>3</sub>/C cell demonstrates excellent rate capability and long cycling stability (0.0288% capacity decay per cycle after 500 cycles). The bioinspired design of glassy MOF will shed light on new avenues for the development of energy storage and conversion.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"13 1","pages":""},"PeriodicalIF":20.4,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142588384","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Zhiyi Guo, Xinsheng Zhu, Liang Xu, Jianxiang Zhu, Xue Zhang, Yang Yang, Nan Song
Bone marrow stem cells (BMSCs)-engineered cartilage (BEC) shows promise for clinically repairing cartilage defects. However, when implanted in immunocompetent large animals, BEC becomes susceptible to ossification due to inflammatory infiltration. To address this, a nanofilm isolation approach is developed to enhance BEC's chondrogenic stability. Tacrolimus (FK506), known for its immunosuppressive effect, is integrated into adipic dihydrazide (ADH)-modified hyaluronic acid (HA), creating an acid-responsive macromolecular prodrug called FK506@HA-ADH. This prodrug is then blended with poly(lactic-co-glycolic acid) (PLGA) to form electrospun FK506@HA/PLGA nanofilm. Goat-derived BMSCs are induced in vitro to form BEC, which is enclosed within the FK506@HA/PLGA nanofilm and subcutaneously implanted in autologous goats. The nanofilm acted as a physical barrier, preventing immunocyte infiltration. Additionally, in response to the acidic environment triggered by inflammation and the gradual degradation of PLGA, the FK506@HA-ADH prodrug is cleaved, releasing FK506 as needed. The released FK506 effectively countered inflammatory cytokines and promoted cartilaginous maturity. These combined mechanisms significantly inhibited BEC hypertrophy and improved its chondrogenic stability within an immunocompetent goat model. This nanofilm-based isolation strategy established an immunosuppressive niche, successfully preventing endochondral ossification and promoting stable cartilage formation in BEC. These advancements are crucial for translating stem cell-based therapies into clinical use for cartilage repair.
{"title":"Immuno-Isolation Strategy with Tacrolimus-Loaded Nanofilm Promotes Stable Stem Cell-Based Cartilage Regeneration","authors":"Zhiyi Guo, Xinsheng Zhu, Liang Xu, Jianxiang Zhu, Xue Zhang, Yang Yang, Nan Song","doi":"10.1002/adfm.202414567","DOIUrl":"https://doi.org/10.1002/adfm.202414567","url":null,"abstract":"Bone marrow stem cells (BMSCs)-engineered cartilage (BEC) shows promise for clinically repairing cartilage defects. However, when implanted in immunocompetent large animals, BEC becomes susceptible to ossification due to inflammatory infiltration. To address this, a nanofilm isolation approach is developed to enhance BEC's chondrogenic stability. Tacrolimus (FK506), known for its immunosuppressive effect, is integrated into adipic dihydrazide (ADH)-modified hyaluronic acid (HA), creating an acid-responsive macromolecular prodrug called FK506@HA-ADH. This prodrug is then blended with poly(lactic-co-glycolic acid) (PLGA) to form electrospun FK506@HA/PLGA nanofilm. Goat-derived BMSCs are induced in vitro to form BEC, which is enclosed within the FK506@HA/PLGA nanofilm and subcutaneously implanted in autologous goats. The nanofilm acted as a physical barrier, preventing immunocyte infiltration. Additionally, in response to the acidic environment triggered by inflammation and the gradual degradation of PLGA, the FK506@HA-ADH prodrug is cleaved, releasing FK506 as needed. The released FK506 effectively countered inflammatory cytokines and promoted cartilaginous maturity. These combined mechanisms significantly inhibited BEC hypertrophy and improved its chondrogenic stability within an immunocompetent goat model. This nanofilm-based isolation strategy established an immunosuppressive niche, successfully preventing endochondral ossification and promoting stable cartilage formation in BEC. These advancements are crucial for translating stem cell-based therapies into clinical use for cartilage repair.","PeriodicalId":18,"journal":{"name":"ACS Macro Letters","volume":"17 1","pages":""},"PeriodicalIF":19.0,"publicationDate":"2024-11-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142588324","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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