Dilruba A. Popy, Yashpal Singh, Yauhen Tratsiak, Abby M. Cardoza, John M. Lane, Luis Stand, Mariya Zhuravleva, Neeraj Rai, Bayram Saparov
{"title":"Inside Front Cover: Stimuli-responsive photoluminescent copper(I) halides for scintillation, anticounterfeiting, and light-emitting diode applications","authors":"Dilruba A. Popy, Yashpal Singh, Yauhen Tratsiak, Abby M. Cardoza, John M. Lane, Luis Stand, Mariya Zhuravleva, Neeraj Rai, Bayram Saparov","doi":"10.1002/agt2.682","DOIUrl":"https://doi.org/10.1002/agt2.682","url":null,"abstract":"<p>Near unity photoluminescence efficiency has been achieved in green emitting (TEP)<sub>2</sub>Cu<sub>2</sub>Br<sub>4</sub> and orange emitting (TEP)<sub>2</sub>Cu<sub>4</sub>Br<sub>6</sub>. In both cases, emission originates from self-trapped excitons localized on the copper(I) halide structural units. The sensitivity of these compounds to the external stimuli coupled with their ultrabright emission allows their consideration for applications such as solid-state lighting, scintillation, sensing, information storage, and anticounterfeiting (e602).\u0000\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure></p>","PeriodicalId":72127,"journal":{"name":"Aggregate (Hoboken, N.J.)","volume":"5 5","pages":""},"PeriodicalIF":13.9,"publicationDate":"2024-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/agt2.682","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142540834","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yang Jiao, Haimang Wang, Xiechuan Weng, Jihang Wang, Ying Li, Jian Shen, Weiwei Zhao, Qing Xi, Hongyu Zhang, Zhenhong Fu
{"title":"Inside Back Cover: Supramolecular self-assembled nanoparticles for targeted therapy of myocardial infarction by enhancing cardiomyocyte mitophagy","authors":"Yang Jiao, Haimang Wang, Xiechuan Weng, Jihang Wang, Ying Li, Jian Shen, Weiwei Zhao, Qing Xi, Hongyu Zhang, Zhenhong Fu","doi":"10.1002/agt2.683","DOIUrl":"https://doi.org/10.1002/agt2.683","url":null,"abstract":"<p>In this study, supramolecular self-assembled nanoparticles were developed with multi-functional properties of macrophage escape, cardiac targeting, and drug release for the treatment of myocardial infarction. The nanoparticles reduced cardiomyocyte apoptosis, alleviated myocardial interstitial fibrosis, and enhanced cardiac function based on the mechanism of the enhancement in mitophagy and alleviation in mitochondrial damage (e563).\u0000\u0000 <figure>\u0000 <div><picture>\u0000 <source></source></picture><p></p>\u0000 </div>\u0000 </figure></p>","PeriodicalId":72127,"journal":{"name":"Aggregate (Hoboken, N.J.)","volume":"5 5","pages":""},"PeriodicalIF":13.9,"publicationDate":"2024-10-20","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/agt2.683","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142540835","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Constructing benzothiadiazole-based donor‒acceptor covalent organic frameworks for efficient photocatalytic H2 evolution","authors":"Yanchang Huang, Bin Gao, Qihang Huang, De-Li Ma, Hongwei Wu, Cheng Qian","doi":"10.1002/agt2.669","DOIUrl":"https://doi.org/10.1002/agt2.669","url":null,"abstract":"<p>Donor‒acceptor covalent organic frameworks (D‒A COFs) have been regarded as promising materials for photocatalytic water splitting because of their tunable band gaps. However, their efficiency is hindered by fast charge recombination and low photostability. Herein, we proposed a donor structural engineering strategy for improving the photocatalytic activity of D‒A COFs to tackle these problems. Two benzothiadiazole-based D‒A COFs (DHU-COF-BB and DHU-COF-BP) with distinct donors were prepared for photocatalytic H<sub>2</sub> evolution reaction (HER). As a comparison, DHU-COF-TB without benzothiadiazole moieties was also designed and synthesized. Impressively, the photocatalytic H<sub>2</sub> production rate of DHU-COF-BB reaches 12.80 mmol g<sup>−1</sup> h<sup>−1</sup> under visible light irradiation (≥420 nm), which was nearly 2.0 and 3.1 times higher than that of DHU-COF-BP (6.47 mmol g<sup>−1</sup> h<sup>−1</sup>) and DHU-COF-TB (4.06 mmol g<sup>−1</sup> h<sup>−1</sup>), respectively. In addition, the apparent quantum efficiency (AQE) of DHU-COF-BB was up to 5.04% at 420 nm. Photocatalytic and electrochemical measurements indicate that the enhanced hydrogen evolution activity of DHU-COF-BB can be ascribed to the introduction of appropriate benzene moiety into the donors, which increases the charge separation efficiency and thereby suppresses the electron‒hole recombination. Density functional theory (DFT) calculations revealed that both triphenylamine and benzothiadiazole units are the main active sites for HER over the DHU-COF-BB. This work provides new insight into the photocatalytic hydrogen production activity of D‒A COFs by a donor structural engineering strategy.</p>","PeriodicalId":72127,"journal":{"name":"Aggregate (Hoboken, N.J.)","volume":"6 1","pages":""},"PeriodicalIF":13.9,"publicationDate":"2024-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/agt2.669","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143111553","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Maryam Shabbir, Atia Atiq, Jiahua Wang, Maria Atiq, Nyla Saeed, Ibrahim Yildiz, Xuehai Yan, Ruirui Xing, Manzar Abbas
{"title":"Metal-coordinated amino acid/peptide/protein-based supramolecular self-assembled nanomaterials for anticancer applications","authors":"Maryam Shabbir, Atia Atiq, Jiahua Wang, Maria Atiq, Nyla Saeed, Ibrahim Yildiz, Xuehai Yan, Ruirui Xing, Manzar Abbas","doi":"10.1002/agt2.672","DOIUrl":"https://doi.org/10.1002/agt2.672","url":null,"abstract":"<p>Biomolecules with metals can form supramolecular nanomaterials through coordination assembly, opening new avenues for cancer theranostics and bringing unique insights into personalized nanomedicine. These biomaterials have been considered versatile and innovative nanoagents due to their structure‒function control, biological nature, and simple preparation methods. This review article summarized the recent developments in multicomponent nanomaterials formed from metal coordination interactions with amino acids, peptides, and proteins, together with anticancer drugs, for cancer theranostics. We discussed the role of functional groups anchored in building blocks for coordination interactions, and subsequently, the types of interactions were examined from a structure‒function perspective. Amino acids with different metals and anticancer drugs forming supramolecular nanomaterials and their anticancer mechanisms were highlighted. Peptides with different metals and anticancer drugs, proteins with metals and anticancer drugs used for material formations, and anticancer activity have been discussed. Ultimately, the conclusion and future outlook for multicomponent supramolecular nanomaterials offer fundamental insights into fabrication design and precision medicine.</p>","PeriodicalId":72127,"journal":{"name":"Aggregate (Hoboken, N.J.)","volume":"6 1","pages":""},"PeriodicalIF":13.9,"publicationDate":"2024-10-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/agt2.672","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143111554","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Programmable light-driven soft actuator enabled by structurally anisotropic liquid crystalline network","authors":"Zhaoping Deng, Xinyu Chen, Xinrui Deng, Jiangmin Yang, Shuai Zhou, Jingyu Chen, Peixiang Wang, Huai Yang, Ruochen Lan","doi":"10.1002/agt2.633","DOIUrl":"https://doi.org/10.1002/agt2.633","url":null,"abstract":"<p>The design and fabrication of advanced soft actuators with programmable actuation are highly desirable in constructing intelligent soft robots. In this work, a programmable light-driven liquid crystalline network (LCN)-based soft actuator was judiciously designed and prepared by constructing structural anisotropy across the thickness of the film. A three-dimensional (3D) deformable LCN actuator was realized by polymerization-induced phase separation of small-molar-weight monomers and polymer networks. The resultant anisotropic LCN displays anisotropic microscale nanoporous architecture across the thickness in addition to uniform alignment at the molecular scale. The actuation behaviors of LCN film are tunable by adjusting the size and distribution of nanopores in LCN bulk via changing polymerization conditions and monomer components. More importantly, the nanoporous LCN film can be harnessed as a promising template to achieve diverse light responsiveness by changing the photothermal dyes via a feasible washing and refilling process, demonstrating a reprogrammable light-driven soft actuator.</p>","PeriodicalId":72127,"journal":{"name":"Aggregate (Hoboken, N.J.)","volume":"6 1","pages":""},"PeriodicalIF":13.9,"publicationDate":"2024-10-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/agt2.633","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143111016","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Shan Wang, Qiang Wang, Yang Lv, Zhe Liu, Kippeum Lee, Dongeun Kim, Miae Won, Jianliang Shen, Jong Seung Kim
{"title":"Fluorescence imaging-guided lipid droplets-localized photodynamic therapy","authors":"Shan Wang, Qiang Wang, Yang Lv, Zhe Liu, Kippeum Lee, Dongeun Kim, Miae Won, Jianliang Shen, Jong Seung Kim","doi":"10.1002/agt2.665","DOIUrl":"https://doi.org/10.1002/agt2.665","url":null,"abstract":"<p>Photodynamic therapy (PDT) has emerged as a promising strategy for cancer treatment due to its non-invasive nature and high specificity toward malignant tissues. In recent years, a variety of protocols have been proposed to improve the PDT efficacy, of which organelle-targeted PDT strategy is supposed to be quite promising. Particularly, lipid droplets (LDs)-localized PDT attracts a lot of interest due to the inherent advantages such as abundant LDs in cancer cells and their close relation with ferroptosis. This review provides a comprehensive summary of the advancements of LDs-localized photosensitizers (PSs) according to their chemical structures and functions. Especially, these PSs are featured with fluorescence emission, thereby facilitating an imaging-guided phototherapy. The review highlights the cytocidal actions of these PSs, such as the cell death pathway and their cytotoxicity. Finally, some unresolved issues and challenges in this domain will be discussed.</p>","PeriodicalId":72127,"journal":{"name":"Aggregate (Hoboken, N.J.)","volume":"6 1","pages":""},"PeriodicalIF":13.9,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/agt2.665","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143110326","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"A new class of organic nanoparticles through hyperbranching and crosslinking","authors":"Haoran Wang, Junyi Gong, Ben Zhong Tang","doi":"10.1002/agt2.668","DOIUrl":"https://doi.org/10.1002/agt2.668","url":null,"abstract":"<p>Brush-modified nanoparticles, created by grafting functional polymers from nanoparticle surfaces, have demonstrated their versatility in various applications.<sup>[</sup><span><sup>1</sup></span><sup>]</sup> Traditionally, these nanoparticle brushes are formed by tethering polymer chains onto surface-modified “inorganic” particles. However, customizing the internal molecular structure of these nanoparticles is quite limited. In contrast, “organic” nanoparticles (oNPs) offer significant potential for incorporating small functional molecules, enabling applications in areas such as luminescence, sensing, and drug delivery.<sup>[</sup><span><sup>2</sup></span><sup>]</sup> Additionally, materials composed of oNPs are less dense, making them suitable for lightweight equipment, for example, for soft robotics. Despite these advantages, realizing oNPs remains a challenge. Most synthetic approaches rely on “bottom-up” methods such as self-assembly. However, in these systems labile interactions can undermine performance and long-term stability under harsh conditions.</p><p>In a recent breakthrough, Matyjaszewski, Bockstaller, and their teams have developed a new class of oNPs by leveraging macromolecular architecture through concurrent hyperbranching and crosslinking, utilizing atom transfer radical polymerization (ATRP) in microemulsion (Figure 1A).<sup>[</sup><span><sup>3</sup></span><sup>]</sup> Unlike previous work on hyperbranched homopolymers such as poly[2-(2-bromoisobutyryloxy)ethyl methacrylate] (PBiBEM),<sup>[</sup><span><sup>4</sup></span><sup>]</sup> the new method introduces copolymerization with ethylene glycol dimethacrylate (EGDMA) to enhance internal rigidity. Within a confined space, these inimer-based oNPs had tunable sizes and mechanical properties through varying crosslinking densities. With BiBEM composition varying from 60 to 90 mol%, the resulting oNPs are spherical macromolecules (<i>M</i><sub>n,MALS</sub> ranged from 2 to 6 million Daltons), with nanometer-scale diameters, uniform distribution, and minimal aggregation after purification. Also, the increasing crosslinker content yielded smaller oNPs (diameters from 17 to 36 nm) with lower dispersity (<i>M</i><sub>w</sub>/<i>M</i><sub>n</sub>), and greater rigidity (Figure 1B). Furthermore, the addition of sodium dodecyl sulfate (SDS) as an anionic cosurfactant improved uniformity, achieving size dispersity below 3% (Figure 1C).</p><p>Due to the high concentration of alkyl bromide ATRP functionality from the inimer BiBEM and the retention of polymer chain-end functionality via ATRP, these oNPs are well suited as effective macroinitiators for surface-initiated ATRP (Figure 1D). Surface grafting of poly(methyl methacrylate) brushes from oNPs demonstrated high grafting density (<i>σ</i> ∼ 0.5 chains nm<sup>−2</sup>), indicating the potential for direct assembly of brush-modified oNPs or their integration into matrix materials. As crosslinking density increased, each oNP was densely d","PeriodicalId":72127,"journal":{"name":"Aggregate (Hoboken, N.J.)","volume":"5 6","pages":""},"PeriodicalIF":13.9,"publicationDate":"2024-10-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/agt2.668","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142859866","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
{"title":"Enhancing antibacterial photodynamic therapy with NIR-activated gold nanoclusters: Atomic-precision size effect on reducing bacterial biofilm formation and virulence","authors":"Chengyu Liu, Tenghui Tian, Yujia Shi, Meiqi Li, Le Hong, Jing Zhou, Jia Liu, Yuan Zhong, Xue Wang, Zhenyu Wang, Xue Bai, Lin Wang, Chunyan Li, Zhennan Wu","doi":"10.1002/agt2.666","DOIUrl":"https://doi.org/10.1002/agt2.666","url":null,"abstract":"<p>Persistent biofilm infections pose a critical health threat with their relentless presence and amplified antibiotic resistance. Traditional antibacterial photodynamic therapy can inhibit bacteria extracellularly but struggles to control biofilm formation and virulence. Thus, there is an urgent need to develop photosensitizers, such as ultra-small gold nanoclusters (AuNCs), that can penetrate biofilms and internalize into bacteria. However, AuNCs still face the challenge of insufficient reactive oxygen species (ROS) production and limited near-infrared light absorption. This study develops a model of indocyanine green (ICG)-sensitized AuNCs with atomic-precision size effect. This approach achieved near-infrared light absorption while inhibiting radiation transitions, thereby regulating the generation of ROS. Notably, different-sized AuNCs (Au<sub>10</sub>NCs, Au<sub>15</sub>NCs, Au<sub>25</sub>NCs) yielded varied ROS types, resulting from different energy level distributions and electron transfer rates. ICG-Au<sub>15</sub>NCs achieved a treatment efficacy of 99.94% against <i>Staphylococcus aureus</i> infections in vitro and significantly accelerated wound healing in vivo. Moreover, this study highlights the unique role of ICG-AuNCs in suppressing quorum sensing, virulence, and ABC transporters compared to their larger counterparts. This strategy demonstrates that atomic-precision size effect of AuNCs paves the way for innovative approaches in antibacterial photodynamic therapy for infection control.</p>","PeriodicalId":72127,"journal":{"name":"Aggregate (Hoboken, N.J.)","volume":"6 1","pages":""},"PeriodicalIF":13.9,"publicationDate":"2024-09-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/agt2.666","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143120430","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ke Wang, Xinwen Ou, Xiaofei Niu, Zhenghao Wang, Fengyan Song, Xiaobin Dong, Wu-jie Guo, Hui-Qing Peng, Zujin Zhao, Jacky W. Y. Lam, Jianwei Sun, Hongkai Wu, Shu-Yan Yu, Fei Li, Ben Zhong Tang
{"title":"Aggregation-induced circularly polarized luminescence and delayed fluorescence enabled by activating high-level reverse intersystem crossing","authors":"Ke Wang, Xinwen Ou, Xiaofei Niu, Zhenghao Wang, Fengyan Song, Xiaobin Dong, Wu-jie Guo, Hui-Qing Peng, Zujin Zhao, Jacky W. Y. Lam, Jianwei Sun, Hongkai Wu, Shu-Yan Yu, Fei Li, Ben Zhong Tang","doi":"10.1002/agt2.667","DOIUrl":"https://doi.org/10.1002/agt2.667","url":null,"abstract":"<p>Circularly polarized luminescence (CPL) materials with delayed fluorescence have attracted much attention due to their ability to efficiently trap triplet state excitons, thereby improving the photoluminescence quantum yields of CPL materials. However, much effort has been normally focused on the utilization of T<sub>1</sub> excitons but seldom on the utilization of higher excited triplet state T<i><sub>n</sub></i> (<i>n</i> > 1) excitons. Rational manipulation of higher excited triplet state T<i><sub>n</sub></i> (<i>n</i> > 1) excitons and suppression of Kasha's rule of CPL materials remains a major challenge. Herein, two gold complex enantiomers ((<i>R</i>/<i>S</i>)-BPAuBC) based on axially chiral binaphthyls and 3,6-Di-tert-butylcarbazole groups are synthesized and systematically investigated. These materials exhibit aggregation-induced circularly polarized delayed fluorescence. Circularly polarized delayed fluorescence was found to be enabled by activating high-level reverse intersystem crossing (hRISC). The anti-Kasha phosphorescence at 77 K proves that the exciton has a large population in the high-lying triplet state T<sub>2</sub>, which allows the effective hRISC process to cross back to the singlet state S<sub>1</sub> and emit delayed fluorescence. In addition, CPL “on–off” switching is further achieved in nanoparticles by acid–base stimulus, showing its potential as an acid–base responsive material.</p>","PeriodicalId":72127,"journal":{"name":"Aggregate (Hoboken, N.J.)","volume":"6 1","pages":""},"PeriodicalIF":13.9,"publicationDate":"2024-09-25","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://onlinelibrary.wiley.com/doi/epdf/10.1002/agt2.667","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"143119451","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"OA","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}