Yantong Guo, Xiaoju Yang, Ruixue Sun, Xunliang Hu, Chang Shu, Xuan Yang, Hui Gao, Xiaoyan Wang, Bien Tan
Photocatalytic hydrogen peroxide production from water and oxygen offers a clean and sustainable alternative to the conventional energy-intensive anthraquinone oxidation method. Compared to powdered covalent triazine frameworks (CTFs), the film morphology of CTFs provides better connectivity in 2D, yielding several advantages: more efficient connections between active sites, reduced electron-hole pair recombination, increased resistance to superoxide radical induced corrosion, and decreased light scattering. Leveraging these benefits, it has incorporated dual active sites for both the oxygen reduction reaction (ORR) and the water oxidation reaction (WOR) into a CTF film system. This dual-active CTF film demonstrated an exceptional hydrogen peroxide production rate of 19 460 µmol h⁻¹ m⁻2 after 1 h and 17 830 µmol h⁻¹ m⁻2 after 5 h under visible light irradiation (≥420 nm) without the need for sacrificial agents.
{"title":"A Dual-Active Covalent Triazine Framework Film for Efficient Visible-Light-Driven Hydrogen Peroxide Production.","authors":"Yantong Guo, Xiaoju Yang, Ruixue Sun, Xunliang Hu, Chang Shu, Xuan Yang, Hui Gao, Xiaoyan Wang, Bien Tan","doi":"10.1002/smll.202403743","DOIUrl":"https://doi.org/10.1002/smll.202403743","url":null,"abstract":"<p><p>Photocatalytic hydrogen peroxide production from water and oxygen offers a clean and sustainable alternative to the conventional energy-intensive anthraquinone oxidation method. Compared to powdered covalent triazine frameworks (CTFs), the film morphology of CTFs provides better connectivity in 2D, yielding several advantages: more efficient connections between active sites, reduced electron-hole pair recombination, increased resistance to superoxide radical induced corrosion, and decreased light scattering. Leveraging these benefits, it has incorporated dual active sites for both the oxygen reduction reaction (ORR) and the water oxidation reaction (WOR) into a CTF film system. This dual-active CTF film demonstrated an exceptional hydrogen peroxide production rate of 19 460 µmol h⁻¹ m⁻<sup>2</sup> after 1 h and 17 830 µmol h⁻¹ m⁻<sup>2</sup> after 5 h under visible light irradiation (≥420 nm) without the need for sacrificial agents.</p>","PeriodicalId":228,"journal":{"name":"Small","volume":null,"pages":null},"PeriodicalIF":13.0,"publicationDate":"2024-07-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141553766","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Enmin Hu, Qian Liu, Zishu Qian, Qian Zhong, Junhui He, Shicheng Xu, Tianming Lu, Jin Li, Tao Chen, Wenkun Zhu
Photo-assisted uranium extraction from seawater (UES) is regarded as an efficient technique for uranium resource recovery, yet it currently faces many challenges, such as issues like biofouling resistance, low charge separation efficiency, slow carrier transfer, and a lack of active sites. Based on addressing the above challenges, a novel oxygen-deficient Co3O4-x/g-C3N4 p-n heterojunction is developed for efficient photo-assisted uranium extraction from seawater. Relying on the defect-coupling heterojunction synergistic effect, the redistribution of molecular charge density formed the built-in electric field as revealed by DFT calculations, significantly enhancing the separation efficiency of carriers and accelerating their migration rate. Notably, oxygen vacancies served as capture sites for oxygen, effectively promoting the generation of reactive oxygen species (ROS), thereby significantly improving the photo-assisted uranium extraction performance and antibacterial activity. Thus, under simulated sunlight irradiation with no sacrificial reagent added, Co3O4-x/g-C3N4 extracted a high uranium extraction amount of 1.08 mg g-1 from 25 L of natural seawater after 7 days, which is superior to most reported carbon nitride-based photocatalysts. This study elaborates on the important role of surface defects and inerface engineering strategies in enhancing photocatalytic performance, providing a new approach to the development and design of uranium extraction material from seawater.
{"title":"Unveiling Mechanistic Insight into Accelerating Oxygen Molecule Activation by Oxygen Defects in Co<sub>3</sub>O<sub>4-x</sub>/g-C<sub>3</sub>N<sub>4</sub> p-n Heterojunction for Efficient Photo-Assisted Uranium Extraction from Seawater.","authors":"Enmin Hu, Qian Liu, Zishu Qian, Qian Zhong, Junhui He, Shicheng Xu, Tianming Lu, Jin Li, Tao Chen, Wenkun Zhu","doi":"10.1002/smll.202403105","DOIUrl":"https://doi.org/10.1002/smll.202403105","url":null,"abstract":"<p><p>Photo-assisted uranium extraction from seawater (UES) is regarded as an efficient technique for uranium resource recovery, yet it currently faces many challenges, such as issues like biofouling resistance, low charge separation efficiency, slow carrier transfer, and a lack of active sites. Based on addressing the above challenges, a novel oxygen-deficient Co<sub>3</sub>O<sub>4-x</sub>/g-C<sub>3</sub>N<sub>4</sub> p-n heterojunction is developed for efficient photo-assisted uranium extraction from seawater. Relying on the defect-coupling heterojunction synergistic effect, the redistribution of molecular charge density formed the built-in electric field as revealed by DFT calculations, significantly enhancing the separation efficiency of carriers and accelerating their migration rate. Notably, oxygen vacancies served as capture sites for oxygen, effectively promoting the generation of reactive oxygen species (ROS), thereby significantly improving the photo-assisted uranium extraction performance and antibacterial activity. Thus, under simulated sunlight irradiation with no sacrificial reagent added, Co<sub>3</sub>O<sub>4-x</sub>/g-C<sub>3</sub>N<sub>4</sub> extracted a high uranium extraction amount of 1.08 mg g<sup>-1</sup> from 25 L of natural seawater after 7 days, which is superior to most reported carbon nitride-based photocatalysts. This study elaborates on the important role of surface defects and inerface engineering strategies in enhancing photocatalytic performance, providing a new approach to the development and design of uranium extraction material from seawater.</p>","PeriodicalId":228,"journal":{"name":"Small","volume":null,"pages":null},"PeriodicalIF":13.0,"publicationDate":"2024-07-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141553808","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Hongyan Zhou, Quan Kuang, Jianguo Li, Yan Jin, Yunbo Li, Qinghua Fan, Youzhong Dong, Yanming Zhao
Aqueous nickel-ion batteries (ANIBs) as an emerging energy storage device attracted much attention owing to their multielectron redox reaction and dendrite-free Ni anode, yet their development is hindered by the divalent properties of Ni2+ and the lack of suitable cathode materials. Herein, a hydrated iron vanadate (Fe2V3O10.5∙1.5H2O, FOH) with a preferred orientation along the (200) plane is innovatively proposed and used as cathode material for ANIBs. The FOH cathode exhibits a remarkable capacity of 129.3 mAh g-1 at 50 mA g-1 and a super-high capacity retention of 95% at 500 mA g-1 after 700 cycles. The desirable Ni2+ storage capacity of FOH can be attributed to the preferentially oriented and tunnel structures, which offer abundant reaction active planes and a broad Ni2+ diffusion path, the abundant vacancies and high specific surface area further increase ion storage sites and accelerate ion diffusion in the FOH lattice. Furthermore, the Ni2+ storage mechanism and structural evolution in the FOH cathode are explored through ex situ XRD, ex situ Raman, ex situ XPS and other ex situ characteristics. This work opens a new way for designing novel cathode materials to promote the development of ANIBs.
{"title":"A Novel Hydrated Iron Vanadate Cathode Material for Advanced Aqueous Nickel-Ion Batteries.","authors":"Hongyan Zhou, Quan Kuang, Jianguo Li, Yan Jin, Yunbo Li, Qinghua Fan, Youzhong Dong, Yanming Zhao","doi":"10.1002/smll.202404215","DOIUrl":"https://doi.org/10.1002/smll.202404215","url":null,"abstract":"<p><p>Aqueous nickel-ion batteries (ANIBs) as an emerging energy storage device attracted much attention owing to their multielectron redox reaction and dendrite-free Ni anode, yet their development is hindered by the divalent properties of Ni<sup>2+</sup> and the lack of suitable cathode materials. Herein, a hydrated iron vanadate (Fe<sub>2</sub>V<sub>3</sub>O<sub>10.5</sub>∙1.5H<sub>2</sub>O, FOH) with a preferred orientation along the (200) plane is innovatively proposed and used as cathode material for ANIBs. The FOH cathode exhibits a remarkable capacity of 129.3 mAh g<sup>-1</sup> at 50 mA g<sup>-1</sup> and a super-high capacity retention of 95% at 500 mA g<sup>-1</sup> after 700 cycles. The desirable Ni<sup>2+</sup> storage capacity of FOH can be attributed to the preferentially oriented and tunnel structures, which offer abundant reaction active planes and a broad Ni<sup>2+</sup> diffusion path, the abundant vacancies and high specific surface area further increase ion storage sites and accelerate ion diffusion in the FOH lattice. Furthermore, the Ni<sup>2+</sup> storage mechanism and structural evolution in the FOH cathode are explored through ex situ XRD, ex situ Raman, ex situ XPS and other ex situ characteristics. This work opens a new way for designing novel cathode materials to promote the development of ANIBs.</p>","PeriodicalId":228,"journal":{"name":"Small","volume":null,"pages":null},"PeriodicalIF":13.0,"publicationDate":"2024-07-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141553767","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Juanjuan Liu, Ruijia Sun, Xuan Bao, Jiefu Yang, Yanling Chen, Bijun Tang, Zheng Liu
Fragrance plays a crucial role in the daily lives. Its importance spans various sectors, from therapeutic purposes to personal care, making the understanding and accurate identification of fragrances essential. To fully harness the potential of fragrances, efficient and precise fragrance sensing and identification are necessary. However, current fragrance sensors face several limitations, particularly in detecting and differentiating complex scent profiles with high accuracy. To address these challenges, the use of atom-thin materials in fragrance sensors has emerged as a groundbreaking approach. These atom-thin sensors, characterized by their enhanced sensitivity and selectivity, offer significant improvements over traditional sensing technology. Moreover, the integration of Machine Learning (ML) into fragrance sensing has opened new opportunities in the field. ML algorithms applied to fragrance sensing facilitate advancements in four key domains: accurate fragrance identification, precise discrimination between different fragrances, improved detection thresholds for subtle scents, and prediction of fragrance properties. This comprehensive review delves into the synergistic use of atom-thin materials and ML in fragrance sensing, providing an in-depth analysis of how these technologies are revolutionizing the field, offering insights into their current applications and future potential in enhancing the understanding and utilization of fragrances.
香料在人们的日常生活中发挥着至关重要的作用。它的重要性横跨从治疗到个人护理等各个领域,因此了解和准确识别香味至关重要。要充分利用香味的潜力,就必须进行高效、精确的香味感应和识别。然而,目前的香味传感器面临着一些限制,特别是在高精度地检测和区分复杂的香味特征方面。为了应对这些挑战,在香味传感器中使用原子薄材料已成为一种开创性的方法。这些原子超薄传感器的特点是灵敏度和选择性更强,与传统传感技术相比有显著改进。此外,机器学习(ML)与香味传感的结合也为该领域带来了新的机遇。应用于香味传感的 ML 算法促进了四个关键领域的进步:准确识别香味、精确区分不同香味、提高微妙香味的检测阈值以及预测香味特性。这篇综合评论深入探讨了原子薄材料和 ML 在香味传感中的协同应用,深入分析了这些技术如何在这一领域掀起革命,并深入探讨了它们在增强对香味的理解和利用方面的当前应用和未来潜力。
{"title":"Machine Learning Driven Atom-Thin Materials for Fragrance Sensing.","authors":"Juanjuan Liu, Ruijia Sun, Xuan Bao, Jiefu Yang, Yanling Chen, Bijun Tang, Zheng Liu","doi":"10.1002/smll.202401066","DOIUrl":"https://doi.org/10.1002/smll.202401066","url":null,"abstract":"<p><p>Fragrance plays a crucial role in the daily lives. Its importance spans various sectors, from therapeutic purposes to personal care, making the understanding and accurate identification of fragrances essential. To fully harness the potential of fragrances, efficient and precise fragrance sensing and identification are necessary. However, current fragrance sensors face several limitations, particularly in detecting and differentiating complex scent profiles with high accuracy. To address these challenges, the use of atom-thin materials in fragrance sensors has emerged as a groundbreaking approach. These atom-thin sensors, characterized by their enhanced sensitivity and selectivity, offer significant improvements over traditional sensing technology. Moreover, the integration of Machine Learning (ML) into fragrance sensing has opened new opportunities in the field. ML algorithms applied to fragrance sensing facilitate advancements in four key domains: accurate fragrance identification, precise discrimination between different fragrances, improved detection thresholds for subtle scents, and prediction of fragrance properties. This comprehensive review delves into the synergistic use of atom-thin materials and ML in fragrance sensing, providing an in-depth analysis of how these technologies are revolutionizing the field, offering insights into their current applications and future potential in enhancing the understanding and utilization of fragrances.</p>","PeriodicalId":228,"journal":{"name":"Small","volume":null,"pages":null},"PeriodicalIF":13.0,"publicationDate":"2024-07-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141553772","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Heng Zhang, Junquan Cheng, Xin Xia, Lang Qiu, Feng Liu, Wei Sun, Youcun Bai, Chang Ming Li
Metal phosphides with easy synthesis, controllable morphology, and high capacity are considered as potential anodes for sodium-ion batteries (SIBs). However, the inherent shortcomings of metal phosphating materials, such as conductivity, kinetics, volume strain, etc are not satisfactory, which hinders their large-scale application. Here, a CoP@carbon nanofibers-composite containing rich Co─N─C heterointerface and phosphorus vacancies grown on carbon cloth (CoP1-x@MEC) is synthesized as SIB anode to accomplish extraordinary capacity and ultra-long cycle life. The hybrid composite nanoreactor effectively impregnates defective CoP as active reaction center while offering Co─N─C layer to buffer the volume expansion during charge-discharge process. These vast active interfaces, favored electrolyte infiltration, and a well-structured ion-electron transport network synergistically improve Na+ storage and electrode kinetics. By virtue of these superiorities, CoP1-x@MEC binder-free anode delivers superb SIBs performance including a high areal capacity (2.47 mAh cm-2@0.2 mA cm-2), high rate capability (0.443 mAh cm-2@6 mA cm-2), and long cycling stability (300 cycles without decay), thus holding great promise for inexpensive binder-free anode-based SIBs for practical applications.
金属磷化物具有易于合成、形态可控和容量高等特点,被认为是钠离子电池(SIB)的潜在阳极。然而,金属磷化材料在导电性、动力学、体积应变等方面的固有缺陷并不令人满意,这阻碍了其大规模应用。本文合成了一种 CoP@carbon 纳米纤维复合材料(CoP1-x@MEC)作为 SIB 阳极,该材料含有丰富的 Co─N─C 异质面和生长在碳布上的磷空位(CoP1-x@MEC),可实现超大容量和超长循环寿命。这种混合复合纳米反应器有效地浸渍了有缺陷的 CoP 作为活性反应中心,同时提供 Co─N─C 层以缓冲充放电过程中的体积膨胀。这些广阔的活性界面、有利的电解质渗透和结构良好的离子-电子传输网络协同改善了 Na+ 的存储和电极动力学。凭借这些优势,CoP1-x@MEC 无粘结剂阳极可提供卓越的 SIB 性能,包括高面积容量(2.47 mAh cm-2@0.2 mA cm-2)、高速率能力(0.443 mAh cm-2@6 mA cm-2)和长循环稳定性(300 次循环无衰减),从而为实际应用中的廉价无粘结剂阳极 SIB 带来了巨大希望。
{"title":"Vacancies-Induced Delocalized States Cobalt Phosphide for Binder-Free Anode Toward Stable and High-Rate Sodium-Ion Batteries.","authors":"Heng Zhang, Junquan Cheng, Xin Xia, Lang Qiu, Feng Liu, Wei Sun, Youcun Bai, Chang Ming Li","doi":"10.1002/smll.202403719","DOIUrl":"https://doi.org/10.1002/smll.202403719","url":null,"abstract":"<p><p>Metal phosphides with easy synthesis, controllable morphology, and high capacity are considered as potential anodes for sodium-ion batteries (SIBs). However, the inherent shortcomings of metal phosphating materials, such as conductivity, kinetics, volume strain, etc are not satisfactory, which hinders their large-scale application. Here, a CoP@carbon nanofibers-composite containing rich Co─N─C heterointerface and phosphorus vacancies grown on carbon cloth (CoP<sub>1-x</sub>@MEC) is synthesized as SIB anode to accomplish extraordinary capacity and ultra-long cycle life. The hybrid composite nanoreactor effectively impregnates defective CoP as active reaction center while offering Co─N─C layer to buffer the volume expansion during charge-discharge process. These vast active interfaces, favored electrolyte infiltration, and a well-structured ion-electron transport network synergistically improve Na<sup>+</sup> storage and electrode kinetics. By virtue of these superiorities, CoP<sub>1-x</sub>@MEC binder-free anode delivers superb SIBs performance including a high areal capacity (2.47 mAh cm<sup>-2</sup>@0.2 mA cm<sup>-2</sup>), high rate capability (0.443 mAh cm<sup>-2</sup>@6 mA cm<sup>-2</sup>), and long cycling stability (300 cycles without decay), thus holding great promise for inexpensive binder-free anode-based SIBs for practical applications.</p>","PeriodicalId":228,"journal":{"name":"Small","volume":null,"pages":null},"PeriodicalIF":13.0,"publicationDate":"2024-07-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141553809","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Chun Xie, Kuiting Chen, Zhekun Chen, Yingxin Hu, Linqiang Pan
DNA nanostructures have been utilized to study biological mechanical processes and construct artificial nanosystems. Many application scenarios necessitate nanodevices able to robustly generate large single molecular forces. However, most existing dynamic DNA nanostructures are triggered by probabilistic hybridization reactions between spatially separated DNA strands, which only non-deterministically generate relatively small compression forces (≈0.4 piconewtons (pN)). Here, an intercalator-triggered dynamic DNA origami nanostructure is developed, where large amounts of local binding reactions between intercalators and the nanostructure collectively lead to the robust generation of relatively large compression forces (≈11.2 pN). Biomolecular loads with different stiffnesses, 3, 4, and 6-helix DNA bundles are efficiently bent by the compression forces. This work provides a robust and powerful force-generation tool for building highly chemo-mechanically coupled molecular machines in synthetic nanosystems.
DNA 纳米结构已被用于研究生物机械过程和构建人工纳米系统。许多应用场景都要求纳米装置能够稳健地产生较大的单分子力。然而,现有的大多数动态 DNA 纳米结构都是由空间上分离的 DNA 链之间的概率杂交反应触发的,只能非确定地产生相对较小的压缩力(≈0.4 皮牛顿 (pN))。在这里,我们开发了一种由插层剂触发的动态 DNA 折纸纳米结构,插层剂与纳米结构之间的大量局部结合反应可共同产生相对较大的压缩力(≈11.2 皮牛顿)。具有不同刚度的生物分子负载、3、4 和 6 螺旋 DNA 束都能在压缩力的作用下有效弯曲。这项工作为在合成纳米系统中构建高度化学机械耦合的分子机器提供了一种稳健而强大的力生成工具。
{"title":"A Chemo-Mechanically Coupled DNA Origami Clamp Capable of Generating Robust Compression Forces.","authors":"Chun Xie, Kuiting Chen, Zhekun Chen, Yingxin Hu, Linqiang Pan","doi":"10.1002/smll.202401396","DOIUrl":"https://doi.org/10.1002/smll.202401396","url":null,"abstract":"<p><p>DNA nanostructures have been utilized to study biological mechanical processes and construct artificial nanosystems. Many application scenarios necessitate nanodevices able to robustly generate large single molecular forces. However, most existing dynamic DNA nanostructures are triggered by probabilistic hybridization reactions between spatially separated DNA strands, which only non-deterministically generate relatively small compression forces (≈0.4 piconewtons (pN)). Here, an intercalator-triggered dynamic DNA origami nanostructure is developed, where large amounts of local binding reactions between intercalators and the nanostructure collectively lead to the robust generation of relatively large compression forces (≈11.2 pN). Biomolecular loads with different stiffnesses, 3, 4, and 6-helix DNA bundles are efficiently bent by the compression forces. This work provides a robust and powerful force-generation tool for building highly chemo-mechanically coupled molecular machines in synthetic nanosystems.</p>","PeriodicalId":228,"journal":{"name":"Small","volume":null,"pages":null},"PeriodicalIF":13.0,"publicationDate":"2024-07-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141553765","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Sonodynamic therapy (SDT), featuring noninvasive, deeper penetration, low cost, and repeatability, is a promising therapy approach for deep-seated tumors. However, the general or only utilization of SDT shows low efficiency and unsatisfactory treatment outcomes due to the complicated tumor microenvironment (TME) and SDT process. To circumvent the issues, three feasible approaches for enhancing SDT-based therapeutic effects, including sonosensitizer optimization, strategies for conquering hypoxia TME, and combinational therapy are summarized, with a particular focus on the combination therapy of SDT with other therapy modalities, including chemodynamic therapy, photodynamic therapy, photothermal therapy, chemotherapy, starvation therapy, gas therapy, and immunotherapy. In the end, the current challenges in SDT-based therapy on tumors are discussed and feasible approaches for enhanced therapeutic effects are provided. It is envisioned that this review will provide new insight into the strategic design of high-efficiency sonosensitizer-derived nanotheranostics, thereby augmenting SDT and accelerating the potential clinical transformation.
{"title":"Engineering Sonosensitizer-Derived Nanotheranostics for Augmented Sonodynamic Therapy.","authors":"Fuhong Yang, Jingqi Lv, Wen Ma, Yanling Yang, Xiaoming Hu, Zhen Yang","doi":"10.1002/smll.202402669","DOIUrl":"https://doi.org/10.1002/smll.202402669","url":null,"abstract":"<p><p>Sonodynamic therapy (SDT), featuring noninvasive, deeper penetration, low cost, and repeatability, is a promising therapy approach for deep-seated tumors. However, the general or only utilization of SDT shows low efficiency and unsatisfactory treatment outcomes due to the complicated tumor microenvironment (TME) and SDT process. To circumvent the issues, three feasible approaches for enhancing SDT-based therapeutic effects, including sonosensitizer optimization, strategies for conquering hypoxia TME, and combinational therapy are summarized, with a particular focus on the combination therapy of SDT with other therapy modalities, including chemodynamic therapy, photodynamic therapy, photothermal therapy, chemotherapy, starvation therapy, gas therapy, and immunotherapy. In the end, the current challenges in SDT-based therapy on tumors are discussed and feasible approaches for enhanced therapeutic effects are provided. It is envisioned that this review will provide new insight into the strategic design of high-efficiency sonosensitizer-derived nanotheranostics, thereby augmenting SDT and accelerating the potential clinical transformation.</p>","PeriodicalId":228,"journal":{"name":"Small","volume":null,"pages":null},"PeriodicalIF":13.0,"publicationDate":"2024-07-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141544230","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Laccase is capable of catalyzing a vast array of reactions, but its low redox potential limits its potential applications. The use of photocatalytic materials offers a solution to this problem by converting absorbed visible light into electrons to facilitate enzyme catalysis. Herein, MIL-53(Fe) and NH2-MIL-53(Fe) serve as both light absorbers and enzyme immobilization carriers, and laccase is employed for solar-driven chemical conversion. Electron spin resonance spectroscopy results confirm that visible light irradiation causes rapid transfer of photogenerated electrons from MOF excitation to T1 Cu(II) of laccase, significantly increasing the degradation rate constant of tetracycline (TC) from 0.0062 to 0.0127 min-1. Conversely, there is only minimal or no electron transfer between MOF and laccase in the physical mixture state. Theoretical calculations demonstrate that the immobilization of laccase's active site and its covalent binding to the metal-organic framework surface augment the coupled system's activity, reducing the active site accessible from 27.8 to 18.1 Å. The constructed photo-enzyme coupled system successfully combines enzyme catalysis' selectivity with photocatalysis's high reactivity, providing a promising solution for solar energy use.
{"title":"Enhanced Interfacial Electron Transfer in Photocatalyst-Natural Enzyme Coupled Artificial Photosynthesis System: Tuning Strategies and Molecular Simulations.","authors":"Xiaoxuan Lou, Chen Zhang, Zhiyong Xu, Shengbo Ge, Jian Zhou, Deyu Qin, Fanzhi Qin, Xin Zhang, Zhanhu Guo, Chongchen Wang","doi":"10.1002/smll.202404055","DOIUrl":"https://doi.org/10.1002/smll.202404055","url":null,"abstract":"<p><p>Laccase is capable of catalyzing a vast array of reactions, but its low redox potential limits its potential applications. The use of photocatalytic materials offers a solution to this problem by converting absorbed visible light into electrons to facilitate enzyme catalysis. Herein, MIL-53(Fe) and NH<sub>2</sub>-MIL-53(Fe) serve as both light absorbers and enzyme immobilization carriers, and laccase is employed for solar-driven chemical conversion. Electron spin resonance spectroscopy results confirm that visible light irradiation causes rapid transfer of photogenerated electrons from MOF excitation to T1 Cu(II) of laccase, significantly increasing the degradation rate constant of tetracycline (TC) from 0.0062 to 0.0127 min<sup>-1</sup>. Conversely, there is only minimal or no electron transfer between MOF and laccase in the physical mixture state. Theoretical calculations demonstrate that the immobilization of laccase's active site and its covalent binding to the metal-organic framework surface augment the coupled system's activity, reducing the active site accessible from 27.8 to 18.1 Å. The constructed photo-enzyme coupled system successfully combines enzyme catalysis' selectivity with photocatalysis's high reactivity, providing a promising solution for solar energy use.</p>","PeriodicalId":228,"journal":{"name":"Small","volume":null,"pages":null},"PeriodicalIF":13.0,"publicationDate":"2024-07-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141544231","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Deshuai Kong, Yunmeng Li, Biao Yang, Yaokun Pang, Hua Yuan, Cong Du, Yeqiang Tan
Extrusion-based 3D printing is a facile technology to construct complex structures of hydrogels, especially for tough hydrogels that have shown demonstrated potential in load-bearing materials and tissue engineering. However, 3D-printed hydrogels often possess mechanical properties that do not guarantee their usage in tissue-mimicking, load-bearing components, and motion sensors. This study proposes a novel strategy to construct high-strength and anisotropic Fe3+ cross-linked poly(acrylamide-co-acrylic acid)/sodium alginate double network hydrogels. The semi-flexible sodium alginate chains act as a "conformation regulator" to promote the formation of strong intermolecular interactions between polymer chains and lock the more extended conformation exerted by the pre-stretch, enabling the construction of 3D-printed hydrogel structures with high orientation. The equilibrated anisotropic hydrogel filaments with a water content of 50-60 wt.% exhibit outstanding mechanical properties (tensile strength: 9-44 MPa; elongation at break: 120-668%; Young's modulus: 7-62 MPa; toughness: 26-52 MJ m-3). 3D-printed anisotropic hydrogel structures with high mechanical performance show demonstrated potential as loading-bearing structures and electrodes of flexible triboelectric nanogenerators for versatile human motion sensing.
{"title":"3D-Printed Hydrogels with High-Strength and Anisotropy Mediated by Chain Rigidity.","authors":"Deshuai Kong, Yunmeng Li, Biao Yang, Yaokun Pang, Hua Yuan, Cong Du, Yeqiang Tan","doi":"10.1002/smll.202403052","DOIUrl":"https://doi.org/10.1002/smll.202403052","url":null,"abstract":"<p><p>Extrusion-based 3D printing is a facile technology to construct complex structures of hydrogels, especially for tough hydrogels that have shown demonstrated potential in load-bearing materials and tissue engineering. However, 3D-printed hydrogels often possess mechanical properties that do not guarantee their usage in tissue-mimicking, load-bearing components, and motion sensors. This study proposes a novel strategy to construct high-strength and anisotropic Fe<sup>3+</sup> cross-linked poly(acrylamide-co-acrylic acid)/sodium alginate double network hydrogels. The semi-flexible sodium alginate chains act as a \"conformation regulator\" to promote the formation of strong intermolecular interactions between polymer chains and lock the more extended conformation exerted by the pre-stretch, enabling the construction of 3D-printed hydrogel structures with high orientation. The equilibrated anisotropic hydrogel filaments with a water content of 50-60 wt.% exhibit outstanding mechanical properties (tensile strength: 9-44 MPa; elongation at break: 120-668%; Young's modulus: 7-62 MPa; toughness: 26-52 MJ m<sup>-</sup> <sup>3</sup>). 3D-printed anisotropic hydrogel structures with high mechanical performance show demonstrated potential as loading-bearing structures and electrodes of flexible triboelectric nanogenerators for versatile human motion sensing.</p>","PeriodicalId":228,"journal":{"name":"Small","volume":null,"pages":null},"PeriodicalIF":13.0,"publicationDate":"2024-07-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141544225","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The conductive carbon-based interlayer, as the secondary current collector in the self-dissolving battery system, can effectively capture escaping cathode active materials, inducing deep release of remaining capacity. In the multi-step reactions of Li─S batteries, the environmental tolerance of the conductive carbon-based interlayer to polysulfides determines the inhibition of shuttle effects. Here, a modified metal-organic framework (Mn-ZIF67) is utilized to obtain nitrogen-doped carbon-coated heterogeneous Co-MnO (Co-MnO@NC) with dual catalytic center for the functional interlayer materials. The synergistic coupling mechanism of NC and Co-MnO achieves rapid deposition and conversion of free polysulfide and fragmented active sulfur on the secondary current collector, reducing capacity loss in the cathode. The Li─S battery with Co-MnO@NC/PP separator maintains an initial capacity of 1050 mAh g-1 (3C) and excellent cycle stability (0.056% capacity decay rate). Under extreme testing conditions (S load = 5.82 mg cm-2, E/S = 9.1 µL mg-1), a reversible capacity of 501.36 mAh g-1 is observed after 200 cycles at 0.2 C, showing good further practical reliability. This work demonstrates the advancement application of Co-MnO@NC bimetallic heterojunctions catalysts in the secondary current collector for high-performance Li─S batteries, thereby providing guidance for the development of interlayer in various dissolution systems.
导电碳基中间膜作为自溶电池系统中的二次集流器,可以有效捕捉逸出的正极活性物质,从而诱导剩余容量的深度释放。在锂离子电池的多步反应中,导电碳基中间膜对多硫化物的环境耐受性决定了对穿梭效应的抑制。在此,我们利用改性金属有机框架(Mn-ZIF67)获得了具有双催化中心的氮掺杂碳包覆异质 Co-MnO(Co-MnO@NC)功能性中间膜材料。NC 和 Co-MnO 的协同耦合机制实现了游离多硫化物和碎片活性硫在二次集流体上的快速沉积和转化,从而降低了阴极的容量损失。采用 Co-MnO@NC/PP隔膜的锂离子电池可保持 1050 mAh g-1(3C)的初始容量和出色的循环稳定性(容量衰减率为 0.056%)。在极端测试条件下(S 负载 = 5.82 mg cm-2,E/S = 9.1 µL mg-1),在 0.2 C 下循环 200 次后可观察到 501.36 mAh g-1 的可逆容量,显示了良好的进一步实用可靠性。这项工作证明了 Co-MnO@NC 双金属异质结催化剂在高性能锂离子电池二次集流器中的先进应用,从而为各种溶解体系中夹层的开发提供了指导。
{"title":"A Multifunctional Secondary Based on Heterogeneous Co-MnO@NC for Depth-Induced Deposition and Conversion of Polysulfides in Li─S Batteries.","authors":"Kaiquan He, Hangqi Yang, Xiaowei Wu, Junlong Feng, Pu Hu, Chaoqun Shang","doi":"10.1002/smll.202403419","DOIUrl":"https://doi.org/10.1002/smll.202403419","url":null,"abstract":"<p><p>The conductive carbon-based interlayer, as the secondary current collector in the self-dissolving battery system, can effectively capture escaping cathode active materials, inducing deep release of remaining capacity. In the multi-step reactions of Li─S batteries, the environmental tolerance of the conductive carbon-based interlayer to polysulfides determines the inhibition of shuttle effects. Here, a modified metal-organic framework (Mn-ZIF67) is utilized to obtain nitrogen-doped carbon-coated heterogeneous Co-MnO (Co-MnO@NC) with dual catalytic center for the functional interlayer materials. The synergistic coupling mechanism of NC and Co-MnO achieves rapid deposition and conversion of free polysulfide and fragmented active sulfur on the secondary current collector, reducing capacity loss in the cathode. The Li─S battery with Co-MnO@NC/PP separator maintains an initial capacity of 1050 mAh g<sup>-1</sup> (3C) and excellent cycle stability (0.056% capacity decay rate). Under extreme testing conditions (S load = 5.82 mg cm<sup>-2</sup>, E/S = 9.1 µL mg<sup>-1</sup>), a reversible capacity of 501.36 mAh g<sup>-1</sup> is observed after 200 cycles at 0.2 C, showing good further practical reliability. This work demonstrates the advancement application of Co-MnO@NC bimetallic heterojunctions catalysts in the secondary current collector for high-performance Li─S batteries, thereby providing guidance for the development of interlayer in various dissolution systems.</p>","PeriodicalId":228,"journal":{"name":"Small","volume":null,"pages":null},"PeriodicalIF":13.0,"publicationDate":"2024-07-06","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141544227","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":2,"RegionCategory":"材料科学","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}