{"title":"Adaptable Invisibility Management Using Kirigami-Inspired Transformable Metamaterials.","authors":"He-Xiu Xu, Mingzhao Wang, Guangwei Hu, Shaojie Wang, Yanzhao Wang, Chaohui Wang, Yixuan Zeng, Jiafang Li, Shuang Zhang, Wei Huang","doi":"10.34133/2021/9806789","DOIUrl":"https://doi.org/10.34133/2021/9806789","url":null,"abstract":"<p><p>Many real-world applications, including adaptive radar scanning and smart stealth, require reconfigurable multifunctional devices to simultaneously manipulate multiple degrees of freedom of electromagnetic (EM) waves in an on-demand manner. Recently, kirigami technique, affording versatile and unconventional structural transformation, has been introduced to endow metamaterials with the capability of controlling EM waves in a reconfigurable manner. Here, we report for a kirigami-inspired sparse meta-architecture, with structural density of 1.5% in terms of the occupation space, for adaptive invisibility based on independent operations of frequency, bandwidth, and amplitude. Based on the general principle of dipolar management via structural reconstruction of kirigami-inspired meta-architectures, we demonstrate reconfigurable invisibility management with abundant EM functions and a wide tuning range using three enantiomers (A, B, and C) of different geometries characterized by the folding angle <i>β</i>. Our strategy circumvents issues of limited abilities, narrow tuning range, extreme condition, and high cost raised by available reconfigurable metamaterials, providing a new avenue toward multifunctional smart devices.</p>","PeriodicalId":520765,"journal":{"name":"Research (Washington, D.C.)","volume":" ","pages":"9806789"},"PeriodicalIF":11.0,"publicationDate":"2021-09-10","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8449819/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39507127","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}
Qingsong Zhang, Yunlong Sun, Haijing Li, Kun Tang, Yu-Wu Zhong, Dong Wang, Yunlong Guo, Yunqi Liu
{"title":"Synthesis of Two-Dimensional C-C Bonded Truxene-Based Covalent Organic Frameworks by Irreversible Brønsted Acid-Catalyzed Aldol Cyclotrimerization.","authors":"Qingsong Zhang, Yunlong Sun, Haijing Li, Kun Tang, Yu-Wu Zhong, Dong Wang, Yunlong Guo, Yunqi Liu","doi":"10.34133/2021/9790705","DOIUrl":"https://doi.org/10.34133/2021/9790705","url":null,"abstract":"<p><p>The synthesis of new C-C bonded two-dimensional (2D) covalent organic frameworks (COFs) is highly desirable. Here, a simple but effective synthetic strategy has been developed using an irreversible Brønsted acid-catalyzed aldol cyclotrimerization reaction by virtue of truxene as a linkage. Nonolefin C-C bonded 2D truxene-based covalent organic frameworks (Tru-COFs) were constructed by polymerization of 1,3,5-triindanonebenzene (TDB). The structure formation was confirmed by wide-angle X-ray scattering, Fourier-transform infrared spectroscopy, and solid-state <sup>13</sup>C CP/MAS NMR. The results showed that the Tru-COFs were porous (645 m<sup>2</sup>/g) and chemically stable. Benzyl methylene in conjugated Tru-COFs more effectively produced photoinduced radicals than the model truxene compound. Due to the radical photoresponsiveness, Tru-COFs were efficient catalysts for photocatalytic oxidation of sulfides. We expect that this will provide a new synthetic methodology to obtain C-C bonded functional 2D COFs.</p>","PeriodicalId":520765,"journal":{"name":"Research (Washington, D.C.)","volume":" ","pages":"9790705"},"PeriodicalIF":11.0,"publicationDate":"2021-09-03","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8435030/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39437631","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}
Yuanyuan Fan, Yingshun Zhou, Meng Lu, Haibin Si, Lu Li, Bo Tang
{"title":"Responsive Dual-Targeting Exosome as a Drug Carrier for Combination Cancer Immunotherapy.","authors":"Yuanyuan Fan, Yingshun Zhou, Meng Lu, Haibin Si, Lu Li, Bo Tang","doi":"10.34133/2021/9862876","DOIUrl":"https://doi.org/10.34133/2021/9862876","url":null,"abstract":"<p><p>Recently, combination immunotherapy, which incorporates the activation of the immune system and inhibition of immune escape, has been proved to be a new powerful strategy for more efficient tumor suppression compared to monotherapy. However, the major challenge is how to integrate multiple immune drugs together and efficiently convey these drugs to tumor sites. Although a variety of nanomaterials have been exploited as carriers for targeting tumor issues and the delivery of multiple drugs, their potential toxicity, immune rejection, and stability are still controversial for clinical application. Here, we proposed endogenic exosomes as drug carriers to deliver two antibodies acting as tumor-targeting molecules and block checkpoint inhibitors with specific response to the tumor microenvironment and costimulatory molecules for further improvement of therapeutic effect. The versatile exosomes exhibit excellent biocompatibility and provide a combination immunotherapy platform with synergistic advantages of activation of immune response and inhibition of immune escape.</p>","PeriodicalId":520765,"journal":{"name":"Research (Washington, D.C.)","volume":" ","pages":"9862876"},"PeriodicalIF":11.0,"publicationDate":"2021-08-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8426567/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39431968","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":"Fast Bulky Anion Conduction Enabled by Free Shuttling Phosphonium Cations.","authors":"Xiaolin Ge, Yubin He, Kaiyu Zhang, Xian Liang, Chengpeng Wei, Muhammad A Shehzad, Wanjie Song, Zijuan Ge, Geng Li, Weisheng Yu, Liang Wu, Tongwen Xu","doi":"10.34133/2021/9762709","DOIUrl":"https://doi.org/10.34133/2021/9762709","url":null,"abstract":"<p><p>Highly conductive anion-exchange membranes (AEMs) are desirable for applications in various energy storage and conversion technologies. However, conventional AEMs with bulky HCO<sub>3</sub> <sup>-</sup> or Br<sup>-</sup> as counterion generally exhibit low conductivity because the covalent bonding restrains the tethered cationic group's mobility and rotation. Here, we report an alternative polyrotaxane AEM with nontethered and free-shuttling phosphonium cation. As proved by temperature-dependent NMR, solid-state NMR, and molecular dynamics simulation, the phosphonium cation possesses a thermally trigged shuttling behavior, broader extension range, and greater mobility, thus accelerating the diffusion conduction of bulky anions. Owing to this striking feature, high HCO<sub>3</sub> <sup>-</sup> conductivity of 105 mS cm<sup>-1</sup> at 90°C was obtained at a relatively lower ion-exchange capacity of 1.17 mmol g<sup>-1</sup>. This study provides a new concept for developing highly conductive anion-exchange membranes and will catalyze the exploration of new applications for polyrotaxanes in ion conduction processes.</p>","PeriodicalId":520765,"journal":{"name":"Research (Washington, D.C.)","volume":" ","pages":"9762709"},"PeriodicalIF":11.0,"publicationDate":"2021-08-31","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8426568/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39431967","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":"Time-Dependent Afterglow from a Single Component Organic Luminogen.","authors":"Tianjia Yang, Yunzhong Wang, Jixuan Duan, Shuangyu Wei, Saixing Tang, Wang Zhang Yuan","doi":"10.34133/2021/9757460","DOIUrl":"https://doi.org/10.34133/2021/9757460","url":null,"abstract":"<p><p>Pure organic luminogens with long-persistent luminescence have been extensively studied, on account of their fundamental research significance and diverse utilizations in anticounterfeiting, bioimaging, encryption, organic light-emitting diodes, chemo-sensing, etc. However, time-dependent color-tunable afterglow is rarely reported, especially for single-component materials. In this work, we reported an organic luminogen with time-dependent afterglow, namely, benzoyleneurea (BEU), with multiple persistent room-temperature phosphorescence (p-RTP) and thermally activated delayed fluorescence (TADF) in single crystals. While the lifetime of TADF is relatively short (~1.2 ms), those for p-RTP are as long as around 369~754 ms. The comparable but different decay rates of diversified p-RTP emissions endow BEU crystals with obvious time-dependent afterglow. The existence of multiple emissions can be reasonably illustrated by the clustering-triggered emission (CTE) mechanism. Single-crystal structure illustrates that the combination of benzene ring and nonconventional chromophores of ureide helps facilitate divergent intermolecular interactions, which contribute to the formation of varying emissive species. Moreover, its methyl- and chloro-substituted derivatives show similar multiple p-RTP emissions. However, no time-dependent afterglows are observed in their crystals, due to the highly approaching lifetimes. The afterglow color variation of BEU crystals grants its applications in advanced anticounterfeiting field and information encryption.</p>","PeriodicalId":520765,"journal":{"name":"Research (Washington, D.C.)","volume":" ","pages":"9757460"},"PeriodicalIF":11.0,"publicationDate":"2021-08-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8422276/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39440066","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}
Guanjie Wang, Min Zhang, Yezhi Guan, Ye Zhang, Xianfang Hong, Chenlong Wei, Pengcheng Zheng, Donghui Wei, Zhenqian Fu, Yonggui Robin Chi, Wei Huang
{"title":"Desymmetrization of Cyclic 1,3-Diketones under <i>N</i>-Heterocyclic Carbene Organocatalysis: Access to Organofluorines with Multiple Stereogenic Centers.","authors":"Guanjie Wang, Min Zhang, Yezhi Guan, Ye Zhang, Xianfang Hong, Chenlong Wei, Pengcheng Zheng, Donghui Wei, Zhenqian Fu, Yonggui Robin Chi, Wei Huang","doi":"10.34133/2021/9867915","DOIUrl":"https://doi.org/10.34133/2021/9867915","url":null,"abstract":"<p><p>Symmetric 1,3-diketones with fluorine or fluorinated substituents on the prochiral carbon remain to be established. Herein, we have developed a novel prochiral fluorinated oxindanyl 1,3-diketone and successfully applied these substrates in carbene-catalyzed asymmetric desymmetrization. Accordingly, a versatile strategy for asymmetric generation of organofluorines with fluorine or fluorinated methyl groups has been developed. Multiple stereogenic centers were selectively constructed with satisfactory outcomes. Structurally diverse enantioenriched organofluorines were generated with excellent results in terms of yields, diastereoselectivities, and enantioselectivities. Notably, exchanging fluorinated methyl groups to fluorine for this prochiral 1,3-diketones leads to switchable stereoselectivity. Mechanistic aspects and origin of stereoselectivity were studied by DFT calculations. Notably, some of the prepared organofluorines demonstrated competitive antibacterial activities.</p>","PeriodicalId":520765,"journal":{"name":"Research (Washington, D.C.)","volume":" ","pages":"9867915"},"PeriodicalIF":11.0,"publicationDate":"2021-08-23","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8422277/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39437635","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":"MA Cation-Induced Diffusional Growth of Low-Bandgap FA-Cs Perovskites Driven by Natural Gradient Annealing.","authors":"Taiyang Zhang, Yuetian Chen, Miao Kan, Shumao Xu, Yanfeng Miao, Xingtao Wang, Meng Ren, Haoran Chen, Xiaomin Liu, Yixin Zhao","doi":"10.34133/2021/9765106","DOIUrl":"https://doi.org/10.34133/2021/9765106","url":null,"abstract":"<p><p>Low-bandgap formamidinium-cesium (FA-Cs) perovskites of FA<sub>1-<i>x</i></sub> Cs <i><sub>x</sub></i> PbI<sub>3</sub> (<i>x</i> < 0.1) are promising candidates for efficient and robust perovskite solar cells, but their black-phase crystallization is very sensitive to annealing temperature. Unfortunately, the low heat conductivity of the glass substrate builds up a temperature gradient within from bottom to top and makes the initial annealing temperature of the perovskite film lower than the black-phase crystallization point (~150°C). Herein, we take advantage of such temperature gradient for the diffusional growth of high-quality FA-Cs perovskites by introducing a thermally unstable MA<sup>+</sup> cation, which would firstly form <i>α</i>-phase FA-MA-Cs mixed perovskites with low formation energy at the hot bottom of the perovskite films in the early annealing stage. The natural gradient annealing temperature and the thermally unstable MA<sup>+</sup> cation then lead to the bottom-to-top diffusional growth of highly orientated <i>α</i>-phase FA-Cs perovskite, which exhibits 10-fold of enhanced crystallinity and reduced trap density (~3.85 × 10<sup>15</sup> cm<sup>-3</sup>). Eventually, such FA-Cs perovskite films were fabricated into stable solar cell devices with champion efficiency up to 23.11%, among the highest efficiency of MA-free perovskite solar cells.</p>","PeriodicalId":520765,"journal":{"name":"Research (Washington, D.C.)","volume":" ","pages":"9765106"},"PeriodicalIF":11.0,"publicationDate":"2021-08-18","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8391048/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39410246","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}
Yao Chen, Dong Yang, Yuchen Gao, Runlai Li, Ke An, Wenjing Wang, Zhanfeng Zhao, Xin Xin, Hanjie Ren, Zhongyi Jiang
{"title":"On-Surface Bottom-Up Construction of COF Nanoshells towards Photocatalytic H<sub>2</sub> Production.","authors":"Yao Chen, Dong Yang, Yuchen Gao, Runlai Li, Ke An, Wenjing Wang, Zhanfeng Zhao, Xin Xin, Hanjie Ren, Zhongyi Jiang","doi":"10.34133/2021/9798564","DOIUrl":"https://doi.org/10.34133/2021/9798564","url":null,"abstract":"<p><p>The rational design of an outer shell is of great significance to promote the photocatalytic efficiency of core-shell structured photocatalysts. Herein, a covalent organic framework (COF) nanoshell was designed and deposited on the cadmium sulfide (CdS) core surface. A typical COF material, TPPA, featuring exceptional stability, was synthesized through interfacial polymerization using 1, 3, 5-triformylphloroglucinol (TP) and p-phenylenediamine (PA) as monomers. The nanoshell endows the CdS@TPPA nanosphere with ordered channels for unimpeded light-harvesting and fast diffusion of reactants/products and well-defined modular building blocks for spatially charge separation. Moreover, the heterojunction formed between CdS and TPPA can further facilitate the effective charge separation at the interface <i>via</i> lower exciton binding energy compared with that of pristine TPPA. By modulating the thickness of TPPA nanoshell, the CdS@TPPA nanosphere photocatalyst with the nanoshell thickness of about 8 ± 1 nm exhibits the highest photocatalytic H<sub>2</sub> evolution of 194.1 <i>μ</i>mol h<sup>-1</sup> (24.3 mmol g<sup>-1</sup> h<sup>-1</sup>, 8 mg), which is superior to most of the reported COF-based photocatalysts. The framework nanoshell in this work may stimulate the thinking about how to design advanced shell architecture in the core-shell structured photocatalysts to achieve coordinated charge and molecule transport.</p>","PeriodicalId":520765,"journal":{"name":"Research (Washington, D.C.)","volume":" ","pages":"9798564"},"PeriodicalIF":11.0,"publicationDate":"2021-08-02","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8356126/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39321061","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":"Stretchable, Rehealable, Recyclable, and Reconfigurable Integrated Strain Sensor for Joint Motion and Respiration Monitoring.","authors":"Chuanqian Shi, Zhanan Zou, Zepeng Lei, Pengcheng Zhu, Guohua Nie, Wei Zhang, Jianliang Xiao","doi":"10.34133/2021/9846036","DOIUrl":"https://doi.org/10.34133/2021/9846036","url":null,"abstract":"<p><p>Cutting-edge technologies of stretchable, skin-mountable, and wearable electronics have attracted tremendous attention recently due to their very wide applications and promising performances. One direction of particular interest is to investigate novel properties in stretchable electronics by exploring multifunctional materials. Here, we report an integrated strain sensing system that is highly stretchable, rehealable, fully recyclable, and reconfigurable. This system consists of dynamic covalent thermoset polyimine as the moldable substrate and encapsulation, eutectic liquid metal alloy as the strain sensing unit and interconnects, and off-the-shelf chip components for measuring and magnifying functions. The device can be attached on different parts of the human body for accurately monitoring joint motion and respiration. Such a strain sensing system provides a reliable, economical, and ecofriendly solution to wearable technologies, with wide applications in health care, prosthetics, robotics, and biomedical devices.</p>","PeriodicalId":520765,"journal":{"name":"Research (Washington, D.C.)","volume":" ","pages":"9846036"},"PeriodicalIF":11.0,"publicationDate":"2021-07-29","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8347367/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39326140","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 Self-Assembly of Gold Nanoarrows via Regioselective Adsorption.","authors":"Cheng Chen, Liheng Zheng, Fucheng Guo, Zheyu Fang, Limin Qi","doi":"10.34133/2021/9762095","DOIUrl":"https://doi.org/10.34133/2021/9762095","url":null,"abstract":"<p><p>Programing the self-assembly of colloidal nanoparticles into predetermined superstructures represents an attractive strategy to realize functional assemblies and novel nanodevices, but it remains a challenge. Herein, gold nanoarrows (GNAs) showing a distinct convex-concave structure were employed as unique building blocks for programmable self-assembly involving multiple assembly modes. Regioselective adsorption of 1,10-decanedithiol on the vertexes, edges, and facets of GNAs allowed for programmable self-assembly of GNAs with five distinct assembly modes, and regioselective blocking with 1-dodecanethiol followed by adsorption of 1,10-decanedithiol gave rise to programmable self-assembly with six assembly modes including three novel wing-engaged modes. The assembly mode was essentially determined by regioselective adsorption of the dithiol linker dictated by the local curvature together with the shape complementarity of GNAs. This approach reveals how the geometric morphology of nanoparticles affects their regioselective functionalization and drives their self-assembly.</p>","PeriodicalId":520765,"journal":{"name":"Research (Washington, D.C.)","volume":" ","pages":"9762095"},"PeriodicalIF":11.0,"publicationDate":"2021-07-28","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"https://www.ncbi.nlm.nih.gov/pmc/articles/PMC8343431/pdf/","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"39314472","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}