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Scaffold-free three-dimensional cartilage regeneration based on cartilaginous organoids bioassembly technology 基于软骨有机体生物组装技术的无支架三维软骨再生技术
IF 13.9 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-21 DOI: 10.1002/agt2.619
Yingying Huo, Zheng Ci, Shiqi Wu, Shaoqing Feng, Yuyan Sun, Genke Li, Yu Liu, Yujie Hua, Yixin Zhang, Guangdong Zhou

Cartilage tissue engineering is a promising strategy to repair damaged tissue and reconstruct organ function, but the scaffold-free cartilage regeneration technology is currently limited in its ability to construct three-dimensional (3D) shapes, maintain the chondrogenic phenotype, and express cartilage-specific extracellular matrix (ECM). Recently, cartilaginous organoids (COs), multicellular aggregates with spheroid architecture, have shown great potential in miniaturized cartilage developmental models in vitro. However, high-efficiency and transferable in vivo organoid-based 3D cartilage regeneration technology for preclinical research needs further exploration. In this study, we develop novel cartilaginous organoids bioassembly (COBA) strategy to achieve scaffold-free 3D cartilage regeneration, which displays batch-to-batch efficiency, structural integration, and functional reconstruction. For underlying molecule mechanism, cellular adhesion proteins significantly regulate cell aggregation and cytoskeleton reorganization to form cartilaginous spheroids, and the hypoxic microenvironment created by high-density cell aggregates synergistically activates hypoxia-inducible factor-1α-mediated glycolytic metabolism reprogramming to maintain the chondrogenic phenotype and promote cartilage-specific ECM deposition. Furthermore, separated COs can integrate into a complete and continuous cartilage tissue through the COBA approach, and thus facilitate raising the nasal dorsa in goats after minimally invasive injection. This study thus demonstrates the promise of COBA technology to achieve scaffold-free 3D cartilage regeneration for organoid-based translational applications.

软骨组织工程是修复受损组织和重建器官功能的一种有前途的策略,但无支架软骨再生技术目前在构建三维(3D)形状、保持软骨表型和表达软骨特异性细胞外基质(ECM)方面能力有限。最近,软骨器官组织(COs)--具有球形结构的多细胞聚集体--在体外微型软骨发育模型中显示出巨大的潜力。然而,用于临床前研究的高效、可转移的体内类器官三维软骨再生技术还需要进一步探索。在这项研究中,我们开发了新型软骨类器官生物组装(COBA)策略来实现无支架三维软骨再生,该策略可实现批次间的高效率、结构整合和功能重建。在基础分子机制方面,细胞粘附蛋白能显著调控细胞聚集和细胞骨架重组以形成软骨球体,而高密度细胞聚集形成的缺氧微环境能协同激活缺氧诱导因子-1α介导的糖代谢重编程,从而维持软骨表型并促进软骨特异性ECM沉积。此外,分离的 COs 可通过 COBA 方法整合成完整、连续的软骨组织,从而在微创注射后促进山羊鼻背的隆起。因此,这项研究证明了 COBA 技术在基于类器官的转化应用中实现无支架三维软骨再生的前景。
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引用次数: 0
Inside Front Cover: Supramolecular phthalocyanine assemblies-enhanced synergistic photodynamic and photothermal therapy guided by photoacoustic imaging 封面内页:光声成像引导下的超分子酞菁组装体--增强型协同光动力和光热疗法
Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-18 DOI: 10.1002/agt2.616
Yuan-Yuan Zhao, Xiaojun Zhang, Zixuan Chen, Yihui Xu, Heejeong Kim, Hyunsun Jeong, You Rim Lee, Jiah Lee, Xingshu Li, Juyoung Yoon

In this work, Yoon and co-workers developed a nanostructured supramolecular phototherapeutic agent based on Förster resonance energy transfer mechanism. Such nanostructured phototherapeutic agent can enable the visualization of a tumor with a photoacoustic signal-to-liver ratio as high as 11.9, and ultimately achieving a notable therapeutic effect in a preclinical model at a low dose through the photodynamic and photothermal synergistic therapy (e514).

在这项工作中,Yoon 及其合作者开发了一种基于佛斯特共振能量转移机制的纳米结构超分子光治疗剂。这种纳米结构的光治疗剂能使肿瘤可视化,光声信号与肝脏的比值高达 11.9,并通过光动力和光热协同疗法,最终在临床前模型中以低剂量实现了显著的治疗效果 (e514)。
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引用次数: 0
Inside Back Cover: Twins-like nanodrugs synchronously transport in blood and coalesce inside tumors for sensitive ultrasound imaging and triggerable penetrative drug delivery 封底内页:类似双胞胎的纳米药物在血液中同步传输并在肿瘤内凝聚,可用于灵敏的超声成像和可触发的穿透性给药
Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-18 DOI: 10.1002/agt2.617
Yujun Cai, Gengjia Chen, Minzhao Lin, Bo Li, Huihai Zhong, Tan Li, Zecong Xiao, Yong Wang, Xintao Shuai

A novel strategy for nanoparticle size enlargement is developed by constructing a pair of similar nanodrugs, referred to as “twins-like nanodrugs (TLNs)”. The TLNs synchronously transport in blood, coalesce inside tumor and achieve particle aggregation for ultrasound-triggerable penetrative drug delivery (e476).

通过构建一对相似的纳米药物,即 "双胞胎类纳米药物(TLNs)",开发出了一种扩大纳米粒子尺寸的新策略。TLNs 可在血液中同步传输,在肿瘤内凝聚并实现粒子聚集,从而实现超声触发的穿透性给药 (e476)。
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引用次数: 0
Front Cover: Near-infrared aggregation-induced emission materials: Bibliometric analysis and their application in biomedical field 封面:近红外聚集诱导发射材料:文献计量分析及其在生物医学领域的应用
Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-18 DOI: 10.1002/agt2.615
Qian He, Meiyiming Wang, Li Zhao, Bin Xu, Wenjing Tian, Liyun Zhang

Aggregation-induced emission (AIE) materials emitting near-infrared (NIR) light offer advantages like deep tissue penetration, minimal background interference, and negligible tissue damage. Consequently, NIR-AIE holds great promise in biomedical applications, including cell and living imaging, photothermal and photodynamic therapy, making it a prominent research focus (e505).

发射近红外(NIR)光的聚集诱导发射(AIE)材料具有组织穿透深、背景干扰小和组织损伤小等优点。因此,近红外诱导发射材料在生物医学应用中大有可为,包括细胞和活体成像、光热和光动力疗法,使其成为一个突出的研究重点(e505)。
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引用次数: 0
Back Cover: A core–shell-structured zeolitic imidazolate framework@cationic antimicrobial agent templated silica nanocomposite for tackling antibiotic resistant bacteria infection 封底:用于应对抗生素耐药菌感染的核壳结构沸石咪唑酸盐框架@阳离子抗菌剂模板化二氧化硅纳米复合材料
Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-18 DOI: 10.1002/agt2.618
Qihui Kan, Yaping Song, Yining Yao, Jun Zhang, He Xian, Dan Cheng, Yue Wang, Liang Mao, Meiyan Wang, Chengzhong Yu

An anti-drug-resistant bacteria core-shell structure is designed, containing antibacterial zeolitic imidazolate framework-8 (ZIF-8) as the core and bactericidal benzalkonium chloride (BAC) templated rough-surface mesostructured silica nanocomposite (RMSN) as the shell. The resultant ZIF-8@RMSN nanocomposite exhibits sustained release of BAC and zinc ions, leading to enhanced antibacterial and biofilm elimination properties against drug-resistant bacterial. In addition, ZIF-8@RMSN modified antibacterial band-aid possesses excellent anti-drug-resistant bacterial infection properties both in vitro and in vivo (e523).

本研究设计了一种抗耐药菌核壳结构,以抗菌沸石咪唑酸框架-8(ZIF-8)为核,以杀菌苯扎氯铵(BAC)模板化粗糙表面介质结构二氧化硅纳米复合材料(RMSN)为壳。由此产生的 ZIF-8@RMSN 纳米复合材料可持续释放 BAC 和锌离子,从而增强了对耐药性细菌的抗菌和消除生物膜的特性。此外,ZIF-8@RMSN 改性抗菌创可贴在体外和体内都具有出色的抗耐药菌感染特性 (e523)。
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引用次数: 0
Aggregation-induced emission (AIE) luminescent materials boosting optical storage into the new era of petabit-level capacity 聚合诱导发射(AIE)发光材料推动光存储进入千万亿次级容量的新时代
Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-18 DOI: 10.1002/agt2.605
Siwei Zhang, Pengfei Zhang, Ben Zhong Tang
<p>The recording of information stands as the most significant milestone in human civilization. Historically, the recording and storage of information have undergone a technological evolution from paintings to carvings, scribing, and digitization. The invention of optical compact discs (CDs) was one of the major landmarks in digital information technology. Over the past half-century, scientists have endeavored to enhance optical storage capacity by improving both optical systems and optical storage materials, as shown in Scheme 1. In terms of commercial products, the storage capacity has increased from 700 MB (CDs) to 27 GB (Blu-ray discs) by optimizing the optical system based on the same optical storage medium (polycarbonate). To surpass the conventional optical diffraction limit, the optical systems have evolved from traditional lasers to nonlinear two-photon absorption (TPA) and stimulated emission depletion (STED), which has minified the laser spot size from microns to approximately tens of nanometers, marking a remarkable achievement. However, luminescent materials are essential to enable TPA and STED technology to be applied in optical storage.</p><p>The traditional photopolymers or photoresists usually possess weak emission, and doped with rare earth phosphors, up-conversion nanoparticles, carbon dots, nanoclusters, and metal nanorods that can lead to enhanced fluorescence intensity, but the inorganic nanoparticles in photopolymers may induce light scattering. Traditional conjugated organic chromophores produce quenching upon solid-state aggregation. The green fluorescent protein (GFP) doped in photoresist achieved a reversibly switchable record and detected sub-diffraction site spacing of approximately 200 nm,<sup>[</sup><span><sup>1</sup></span><sup>]</sup> but the stability of GFP is far from meeting the requirements of optical storage. The above methods only enhance the fluorescence intensity of photopolymer film but cannot improve the fluorescence contrast of recorded and unrecorded areas. Therefore, the fluorescence signal radiated by the super-resolution point is easily submerged in the background noise, and the information cannot be read correctly.</p><p>Writing in Nature, Zhao et al.<sup>[</sup><span><sup>2</sup></span><sup>]</sup> reported that a photoresist film doped with aggregation-induced emission luminogens (AIEgens) enables a volumetric nanoscale optical storage system, achieving an impressive 1.6 petabit super disk.</p><p>The concept of aggregation-induced emission (AIE) was proposed in the year of 2001.<sup>[</sup><span><sup>3</sup></span><sup>]</sup> AIEgens usually have rotors or isomerizable double bonds, resulting in weak or no emission in single molecular states (dilute solution) and enhanced emission in the aggregate form due to the restriction of intramolecular motion (RIM). After more than two decades of development, thousands of AIEgens have been designed and synthesized, and their emissions cover from ultravio
光存储还需要 HPS 在日光和环境条件下的稳定性。此外,HPS 的高透光率、与光刻胶的良好兼容性、灵活性和可加工性也为 100 层体积纳米级光存储系统提供了便利(图 1C)。由于 AIEgens 的荧光特性(包括强度和波长)对微环境的敏感性,相信掺杂 AIEgens 的光聚合物能在光存储领域实现更广泛的应用。此外,具有圆偏振光和室温磷光特性的 AIEgens 可能会为防伪和加密信息存储打开新的窗口。同时,我们也注意到,近年来发展迅速的团簇发光也是光刻胶的发光机制之一。基于簇发光可获得波长可调且量子产率高的荧光,这可能是对传统光刻胶的一种改进,无需任何掺杂即可实现高信噪比。总之,由于新材料和新发射机制的出现,尤其是 AIEgens 和团簇发光,光存储介质的选择性更加丰富,这对提高光存储的容量是一个很好的机会。
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引用次数: 0
Regulating room temperature phosphorescence of carbazole quaternization pyridine in polymer through Hofmeister effect 通过霍夫迈斯特效应调节聚合物中咔唑季铵化吡啶的室温磷光
IF 13.9 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-17 DOI: 10.1002/agt2.611
Runying He, Yun Yang, Qian Zhou, Shasha Chang, Yi Cheng, Xiurong Ma, Yonggang Shi, Liyan Zheng, Qiue Cao

Hofmeister effect is a famous physical chemistry phenomenon that was reported a hundred years ago, which firstly refers to the action of certain salts to decrease the solubility of proteins while others increase. The Hofmeister effect on the luminescent properties of cationic organic fluorophore is still obscure, especially for their room temperature phosphorescence (RTP). Herein, hydrophilic groups (quaternization pyridine) were introduced into carbazole molecules to obtain a series of carbazole derivatives (named CZ-Py+) with different counter anions in the Hofmeister series. These carbazole derivatives displayed tunable fluorescent color from cyan to yellow in the solid state following the Hofmeister sequence and anti-Hofmeister behavior in an aqueous solution. Moreover, RTP material with tunable emission color and lifetime was achieved by doping CZ-Py+ with Hofmeister series anion in polymethyl methacrylate and polyvinyl alcohol, which displayed good performance in time getting information encryption and anti-counterfeiting.

霍夫迈斯特效应是一百年前报道的一种著名的物理化学现象,它首先是指某些盐类会降低蛋白质的溶解度,而另一些盐类则会增加蛋白质的溶解度。霍夫迈斯特效应对阳离子有机荧光团发光特性的影响仍不明显,尤其是对其室温磷光(RTP)的影响。在此,我们在咔唑分子中引入了亲水基团(季胺化吡啶),从而获得了一系列具有不同霍夫迈斯特反阴离子的咔唑衍生物(命名为 CZ-Py+)。这些咔唑衍生物在固态下按照霍夫迈斯特序列显示出从青色到黄色的可调荧光颜色,而在水溶液中则显示出反霍夫迈斯特行为。此外,通过在聚甲基丙烯酸甲酯和聚乙烯醇中掺入霍夫迈斯特系列阴离子 CZ-Py+,实现了具有可调发射颜色和寿命的 RTP 材料,在及时获取信息加密和防伪方面表现出色。
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引用次数: 0
Mechanism research of type I reactive oxygen species conversion based on molecular and aggregate levels for tumor photodynamic therapy 基于分子和聚集体水平的 I 型活性氧转化机制研究,用于肿瘤光动力疗法
IF 13.9 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-17 DOI: 10.1002/agt2.612
Youqin Xu, Yili Xie, Qing Wan, Jianwen Tian, Jing Liang, Jianlong Zhou, Mu Song, Xinke Zhou, Muzhou Teng

Type I photosensitizers (PSs) with the ability to generate reactive oxygen species (ROS) containing superoxide anion and hydroxyl radical have promising application potential for treating hypoxia tumors, but the deep mechanism of type II ROS converts to the type I ROS in the PSs is still unclear, it is urgent to reveal influencing factors about inducing type I ROS generation. Herein, six PSs with aggregation-induced emission properties, which were fabricated with the same electronic acceptor but different electronic donors and “π-bridge”, have been successfully prepared to explore the influencing mechanism of generating superoxide anion and hydroxyl radical from organic PSs. Experimental results discovered two factors containing molecular structure and aggregated environment could decide the ROS efficiency and types of PSs. On the level of designing molecular structure, we discovered that “π-bridge” with a lower energy level of the lowest triplet state could be beneficial for triggering the production of superoxide anion, and electronic donor of triphenylamine was an important factor in producing hydroxyl radical than another donor of dimethylamine. On the level of designing aggregates of PS-based polymeric nanoparticles, bovine serum albumin could improve largely the generation efficiency of superoxide anion. Due to the satisfactory ROS efficiency and better biocompatibility, synthetic PSs showed excellent photodynamic therapy outcomes in vitro/vivo.

I型光敏剂(PSs)能够产生含有超氧阴离子和羟基自由基的活性氧(ROS),在治疗缺氧性肿瘤方面具有广阔的应用前景,但II型ROS在PSs中转化为I型ROS的深层机制尚不清楚,迫切需要揭示诱导I型ROS产生的影响因素。本文成功制备了六种具有聚集诱导发射特性的聚苯乙烯,采用相同的电子受体但不同的电子供体和 "π桥",探讨了有机聚苯乙烯产生超氧阴离子和羟基自由基的影响机制。实验结果发现,分子结构和聚集环境这两个因素可以决定 ROS 的效率和 PSs 的类型。在分子结构设计层面,我们发现最低三重态能级较低的 "π桥 "有利于引发超氧阴离子的产生,三苯胺电子供体比二甲胺供体是产生羟基自由基的重要因素。在设计 PS 聚合物纳米粒子聚集体的层面上,牛血清白蛋白能在很大程度上提高超氧阴离子的生成效率。由于合成 PS 具有令人满意的 ROS 效能和更好的生物相容性,因此在体外/活体光动力疗法中表现出卓越的疗效。
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引用次数: 0
Full-color-tunable chiral aggregation-induced emission fluorophores with tailored propeller chirality and their circularly polarized luminescence 具有定制螺旋桨手性的全色可调手性聚集诱导发射荧光团及其圆偏振发光
IF 13.9 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-14 DOI: 10.1002/agt2.613
Yifan Li, Junhao Liang, Shiwei Fu, Haoxin Huang, Sheng Liu, Lei Wang, Yi Liu

The regulation of emission color, emission efficiency, and asymmetry factor is of great significance for the real applications of circularly polarized luminescent (CPL) materials. Herein, we develop a modular synthetic strategy toward full-color-tunable CPL materials based on chiral macrocyclic aggregation-induced emission (AIE) luminogens via delicate molecular engineering. Modular synthesis of chiral AIEgens with different acceptor moieties has afforded a series of bright solid emitters with tunable emission colors. These chiral cyclic AIEgens have retained high solid-state emission quantum yield and displayed CPL emission from blue to red as nano-aggregates, in liquid crystal matrix and polymer film. The strong acceptor units in the red-emitting chiral AIEgens RBTPE-2CN and SBTPE-2CN have rendered them twisted intramolecular charge transfer properties and solvatochromic luminescence. And polymer matrix with different polarity further facilitates the tuning of CPL emission color from green to red emission. These results have paved a reliable approach toward constructing full-spectra solid-state CPL material.

调节发射颜色、发射效率和不对称系数对于圆偏振发光(CPL)材料的实际应用具有重要意义。在此,我们开发了一种模块化合成策略,通过精细的分子工程,在手性大环聚集诱导发射(AIE)发光体的基础上实现全色可调 CPL 材料。通过模块化合成具有不同受体分子的手性 AIE 原素,我们获得了一系列具有可调发射颜色的明亮固体发光体。这些手性环状 AIEgens 保持了很高的固态发射量子产率,并在液晶基质和聚合物薄膜中以纳米聚集体的形式显示出从蓝色到红色的 CPL 发射。红色发射手性 AIEgens RBTPE-2CN 和 SBTPE-2CN 中的强受体单元使它们具有分子内电荷转移特性和溶解变色发光特性。不同极性的聚合物基质进一步促进了 CPL 发射颜色从绿色到红色的调整。这些结果为构建全光谱固态 CPL 材料铺平了可靠的道路。
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引用次数: 0
A clusteroluminescent supramolecular polymer network constructed by pillararene and its application in information encryption 由支柱烯构建的簇发光超分子聚合物网络及其在信息加密中的应用
IF 13.9 Q1 CHEMISTRY, MULTIDISCIPLINARY Pub Date : 2024-06-14 DOI: 10.1002/agt2.608
Meiru Zhang, Yujie Cheng, Ting Zhang, Bicong Liang, Xuehong Wei, Pi Wang, Danyu Xia, Xuzhou Yan

Clusterization-triggered emissive (CTE) materials have attracted great attention in recent years. The regulation of the emission property of materials with CTE property through supramolecular interactions is an excellent strategy for the construction of smart fluorescent materials. In this work, we have prepared a regulatable supramolecular polymer network with CTE properties through pillararene-based host−guest interactions. The pillar[5]arene-grafted poly(methyl methacrylate) (PMMA) showed a classic CTE character. After adding Brooker's merocyanine-grafted polymer to the solution of the pillar[5]arene-containing PMMA, the supramolecular polymer network gel formed by the host−guest interactions between pillararene and Brooker's merocyanine guest. This supramolecular network showed brighter fluorescence than the pillar[5]arene-grafted PMMA in the solid state. In addition, the fluorescence emission of the supramolecular network can be further regulated by pH conditions. After adding an acid, the Brooker's merocyanine-containing guest polymer was protonated, and the supramolecular network changed to a protonated network through host−guest interactions between protonated Brooker's merocyanine guest and pillararene. Interestingly, the fluorescence was quenched when the supramolecular network turned into the protonated network. After adding a base, the protonated network can convert back to the original network, along with recovery of the fluorescence. Therefore, the regulation of the fluorescence of the supramolecular polymer materials with CTE was successfully realized by pillararene-based host−guest interactions. Furthermore, this tailorable fluorescent supramolecular polymer network system was applied as an information encryption material.

近年来,团簇化触发发射(CTE)材料备受关注。通过超分子相互作用调控具有 CTE 特性的材料的发射特性,是构建智能荧光材料的绝佳策略。在这项工作中,我们通过基于支柱烯的主客体相互作用制备了一种具有 CTE 特性的可调控超分子聚合物网络。柱[5]炔接枝的聚甲基丙烯酸甲酯(PMMA)具有典型的 CTE 特性。在含支柱[5]炔的聚甲基丙烯酸甲酯溶液中加入布鲁克梅洛菁接枝聚合物后,支柱炔与布鲁克梅洛菁客体之间的主客作用形成了超分子聚合物网络凝胶。这种超分子网络在固态下比支柱[5]炔接枝的 PMMA 显示出更亮的荧光。此外,超分子网络的荧光发射还可以通过 pH 值条件进一步调节。加入酸后,含有布鲁克梅洛菁的客体聚合物被质子化,通过质子化的布鲁克梅洛菁客体与支柱烯之间的主客体相互作用,超分子网络变为质子化网络。有趣的是,当超分子网络变成质子化网络时,荧光被淬灭。加入碱后,质子化网络又能转换回原始网络,荧光也随之恢复。因此,基于柱烯的主客体相互作用成功实现了对具有 CTE 的超分子聚合物材料的荧光调节。此外,这种可定制的荧光超分子聚合物网络系统还被用作信息加密材料。
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引用次数: 0
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