The soot emitted during the operation of diesel engine exhaust seriously threatens the human health and environment, so treating diesel engine exhaust is critical. At present, the most effective method for eliminating soot particles is post‐treatment technology. Preparation of economically viable and highly active soot combustion catalysts is a pivotal element of post‐treatment technology. In this study, different single‐metal oxide catalysts with fibrous structures and alkali metal‐modified hollow nanotubular Mn‐based oxide catalysts were synthesized using centrifugal spinning method. Activity evaluation results showed that the manganese oxide catalyst has the best catalytic activity among the prepared single‐metal oxide catalysts. Further research on alkali metal modification showed that doping alkali metals is beneficial for improving the oxidation state of manganese and generating a large number of reactive oxygen species. Combined with the structural effect brought by the hollow nanotube structure, the alkali metal‐modified Mn‐based oxide catalysts exhibit superior catalytic performance. Among them, the Cs‐modified Mn‐based oxide catalyst exhibits the best catalytic performance because of its rich active oxygen species, excellent NO oxidation ability, abundant Mn4+ ions (Mn4+/Mnn+ = 64.78%), and good redox ability. The T10, T50, T90, and CO2 selectivity of the Cs‐modified Mn‐based oxide catalyst were 267°C, 324°C, 360°C, and 97.8%, respectively.
柴油发动机运行过程中排放的烟尘严重威胁人类健康和环境，因此柴油发动机尾气处理至关重要。目前，消除烟尘颗粒最有效的方法是后处理技术。制备经济可行的高活性烟尘燃烧催化剂是后处理技术的关键要素。本研究采用离心纺丝法合成了不同的纤维状单金属氧化物催化剂和碱金属改性空心纳米管锰基氧化物催化剂。活性评价结果表明，在所制备的单金属氧化物催化剂中，氧化锰催化剂的催化活性最好。对碱金属改性的进一步研究表明，掺杂碱金属有利于改善锰的氧化态，产生大量活性氧。结合空心纳米管结构带来的结构效应，碱金属改性的锰基氧化物催化剂表现出优异的催化性能。其中，Cs 改性 Mn 基氧化物催化剂具有丰富的活性氧物种、优异的 NO 氧化能力、丰富的 Mn4+ 离子（Mn4+/Mnn+ = 64.78%）和良好的氧化还原能力，因此催化性能最佳。Cs 改性锰基氧化物催化剂的 T10、T50、T90 和 CO2 选择性分别为 267°C、324°C、360°C 和 97.8%。
{"title":"Facile preparation of alkali metal‐modified hollow nanotubular manganese‐based oxide catalysts and their excellent catalytic soot combustion performance","authors":"Chunlei Zhang, Siyu Gao, Xinyu Chen, Di Yu, Lanyi Wang, Xiaoqiang Fan, Ying Cheng, Xuehua Yu, Zhen Zhao","doi":"10.1002/smo.20240022","DOIUrl":"https://doi.org/10.1002/smo.20240022","url":null,"abstract":"The soot emitted during the operation of diesel engine exhaust seriously threatens the human health and environment, so treating diesel engine exhaust is critical. At present, the most effective method for eliminating soot particles is post‐treatment technology. Preparation of economically viable and highly active soot combustion catalysts is a pivotal element of post‐treatment technology. In this study, different single‐metal oxide catalysts with fibrous structures and alkali metal‐modified hollow nanotubular Mn‐based oxide catalysts were synthesized using centrifugal spinning method. Activity evaluation results showed that the manganese oxide catalyst has the best catalytic activity among the prepared single‐metal oxide catalysts. Further research on alkali metal modification showed that doping alkali metals is beneficial for improving the oxidation state of manganese and generating a large number of reactive oxygen species. Combined with the structural effect brought by the hollow nanotube structure, the alkali metal‐modified Mn‐based oxide catalysts exhibit superior catalytic performance. Among them, the Cs‐modified Mn‐based oxide catalyst exhibits the best catalytic performance because of its rich active oxygen species, excellent NO oxidation ability, abundant Mn4+ ions (Mn4+/Mnn+ = 64.78%), and good redox ability. The T10, T50, T90, and CO2 selectivity of the Cs‐modified Mn‐based oxide catalyst were 267°C, 324°C, 360°C, and 97.8%, respectively.","PeriodicalId":501601,"journal":{"name":"Smart Molecules","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-15","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141644697","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Dudu Li, Mao Ye, Chao Ma, Ning Li, Zhenjie Gu, Z. Qiao
The low porosity of metal‐organic framework glass makes it difficult to prepare membranes with high permeability. To solve this problem, we fabricated a series of self‐supported zeolite glass composite membranes with different 4A zeolite loadings using the abundant pore structure of the zeolite. The 4A zeolite embedded in the zeolite glass composite membrane preserved the ligand bonds and chemical structure. The self‐supported zeolite glass composite membranes exhibited good interfacial compatibility. More importantly, the incorporation of the 4A zeolite significantly improved the CO2 adsorption capacity of the pure agZIF‐62 membranes. In addition, gas separation performance measurements showed that the (agZIF‐62)0.7(4A)0.3 membrane had a permeability of 13,329 Barrer for pure CO2 and an ideal selectivity of 31.7 for CO2/CH4, which exceeded Robeson's upper bound. The (agZIF‐62)0.7(4A)0.3 membrane exhibited good operational stability in the variable pressure test and 48 h long‐term continuous test. This study provides a method for preparing zeolite glass composite membranes.
{"title":"Preparation of a self‐supported zeolite glass composite membrane for CO2/CH4 separation","authors":"Dudu Li, Mao Ye, Chao Ma, Ning Li, Zhenjie Gu, Z. Qiao","doi":"10.1002/smo.20240009","DOIUrl":"https://doi.org/10.1002/smo.20240009","url":null,"abstract":"The low porosity of metal‐organic framework glass makes it difficult to prepare membranes with high permeability. To solve this problem, we fabricated a series of self‐supported zeolite glass composite membranes with different 4A zeolite loadings using the abundant pore structure of the zeolite. The 4A zeolite embedded in the zeolite glass composite membrane preserved the ligand bonds and chemical structure. The self‐supported zeolite glass composite membranes exhibited good interfacial compatibility. More importantly, the incorporation of the 4A zeolite significantly improved the CO2 adsorption capacity of the pure agZIF‐62 membranes. In addition, gas separation performance measurements showed that the (agZIF‐62)0.7(4A)0.3 membrane had a permeability of 13,329 Barrer for pure CO2 and an ideal selectivity of 31.7 for CO2/CH4, which exceeded Robeson's upper bound. The (agZIF‐62)0.7(4A)0.3 membrane exhibited good operational stability in the variable pressure test and 48 h long‐term continuous test. This study provides a method for preparing zeolite glass composite membranes.","PeriodicalId":501601,"journal":{"name":"Smart Molecules","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141656259","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Prostate‐specific membrane antigen (PSMA) is known to be overexpressed in prostate cancer (PCa). The development of precise and rapid imaging technologies to monitor PSMA is crucial for early diagnosis and therapy. Fluorescence imaging in the second near‐infrared window (NIR‐II) has emerged as a powerful tool for real‐time tracking and in vivo visualization, offering high sensitivity and resolution. However, there is a lack of stable, bright and easy‐to‐implement NIR‐II fluorescent probes for PSMA targeting. Herein, we presented a PSMA‐targeting NIR‐II fluorescent probe FC‐PSMA based on π‐conjugated crossbreeding dyed strategy that affords high stability, large extinction coefficient, and good brightness. As demonstrated, FC‐PSMA displayed a high fluorescence quantum yield in fetal bovine serum (FBS). Following intravenous injection of FC‐PSMA, the tumor‐to‐normal ratio of fluorescence intensity steadily increased over time, reaching a peak at 48 h (tumor‐to‐leg ratio = 12.16 ± 0.90). This advancement enables precise identification of PC through NIR‐II fluorescence imaging, facilitating high‐performance guidance for prostate cancer resection surgery.
{"title":"“Crossbreeding” NIR‐II flavchromene for PSMA‐positive prostate cancer detection and image‐guided surgery","authors":"Jialiang Huang, Yongkang Yao, Liao Zhang, Chenxu Yan, Zhiqian Guo","doi":"10.1002/smo.20240020","DOIUrl":"https://doi.org/10.1002/smo.20240020","url":null,"abstract":"Prostate‐specific membrane antigen (PSMA) is known to be overexpressed in prostate cancer (PCa). The development of precise and rapid imaging technologies to monitor PSMA is crucial for early diagnosis and therapy. Fluorescence imaging in the second near‐infrared window (NIR‐II) has emerged as a powerful tool for real‐time tracking and in vivo visualization, offering high sensitivity and resolution. However, there is a lack of stable, bright and easy‐to‐implement NIR‐II fluorescent probes for PSMA targeting. Herein, we presented a PSMA‐targeting NIR‐II fluorescent probe FC‐PSMA based on π‐conjugated crossbreeding dyed strategy that affords high stability, large extinction coefficient, and good brightness. As demonstrated, FC‐PSMA displayed a high fluorescence quantum yield in fetal bovine serum (FBS). Following intravenous injection of FC‐PSMA, the tumor‐to‐normal ratio of fluorescence intensity steadily increased over time, reaching a peak at 48 h (tumor‐to‐leg ratio = 12.16 ± 0.90). This advancement enables precise identification of PC through NIR‐II fluorescence imaging, facilitating high‐performance guidance for prostate cancer resection surgery.","PeriodicalId":501601,"journal":{"name":"Smart Molecules","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-07-04","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141679498","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Conductive polymer hydrogels (CPHs) are promising in cutting-edge applications including bioelectronics and tissue engineering. However, the precise regulation of the spatial distribution of the conductive polymer (CP) in the hydrogel network is still an issue for designing a smart material. Herein, we propose a facile method for preparing CPH-based smart materials by controlling the distribution of Fe3+ initiator with UV light irradiation. Thus, designable polypyrrole (PPy) conductive patterns in the polyvinyl alcohol/sodium alginate (PVA/SA) semi-interpenetrating hydrogel network are demonstrated by controlling the concentration of Fe3+ ions coordinated with carboxylate groups. Depending on the irradiation time, the reduction of Fe3+ to Fe2+ occurs in different extents. As a result, the controllable polymerization of pyrrole only initiated by Fe3+ is achieved to form desirable CPH patterns, which are confirmed by the characterization results of Fourier transform infrared spectrometry, X-ray photoelectron spectroscopy, and scanning electron microscopy. Moreover, the developed hydrogel with PPy patterns is illustrated for the application in smart conductive circuit and information encryption. The simple procedure and the controllable conductive patterning of the proposed method make it a promising route in developing smart hydrogel materials, which can be extended to other Fe3+ initiated CP patterns.
{"title":"Designable polypyrrole pattern in hydrogel achieved by photo-controllable concentration of Fe3+ initiator","authors":"Xinyu Zhao, Huidong Xu, Zhao-Tie Liu, Guo Li, Jinqiang Jiang, Zhong-Wen Liu","doi":"10.1002/smo.20240015","DOIUrl":"https://doi.org/10.1002/smo.20240015","url":null,"abstract":"Conductive polymer hydrogels (CPHs) are promising in cutting-edge applications including bioelectronics and tissue engineering. However, the precise regulation of the spatial distribution of the conductive polymer (CP) in the hydrogel network is still an issue for designing a smart material. Herein, we propose a facile method for preparing CPH-based smart materials by controlling the distribution of Fe<sup>3+</sup> initiator with UV light irradiation. Thus, designable polypyrrole (PPy) conductive patterns in the polyvinyl alcohol/sodium alginate (PVA/SA) semi-interpenetrating hydrogel network are demonstrated by controlling the concentration of Fe<sup>3+</sup> ions coordinated with carboxylate groups. Depending on the irradiation time, the reduction of Fe<sup>3+</sup> to Fe<sup>2+</sup> occurs in different extents. As a result, the controllable polymerization of pyrrole only initiated by Fe<sup>3+</sup> is achieved to form desirable CPH patterns, which are confirmed by the characterization results of Fourier transform infrared spectrometry, X-ray photoelectron spectroscopy, and scanning electron microscopy. Moreover, the developed hydrogel with PPy patterns is illustrated for the application in smart conductive circuit and information encryption. The simple procedure and the controllable conductive patterning of the proposed method make it a promising route in developing smart hydrogel materials, which can be extended to other Fe<sup>3+</sup> initiated CP patterns.","PeriodicalId":501601,"journal":{"name":"Smart Molecules","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-27","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"142249113","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Daipeng Huang, Jikai Yin, Yang Zou, Haiqiao Huang, Saran Long, Wen Sun, Jianjun Du, Jiangli Fan, Xiaojun Peng
As a novel drug development paradigm, selective activation of prodrugs provides the potential for precise tumor chemotherapy, thereby presenting an opportunity for advancing cancer treatment. The combination of photodynamic therapy (PDT) and prodrug can enhance the therapeutic efficacy while simultaneously enabling real‐time monitoring of drug distribution and release. However, the tumor hypoxia microenvironment and the frequent high‐dose administration of prodrugs significantly impede therapeutic efficacy and escalate treatment‐related risks. Herein, a tumor microenvironment‐specific release prodrug is constructed, termed NBS‐2S‐5FU. Under the influence of glutathione (GSH), NBS‐2S‐5FU undergoes activation, leading to the release of photosensitizer NBS and chemotherapeutic agent 5‐FU derivatives. Under irradiation, NBS produces sufficient superoxide radical () while 5‐FU derivatives inhibit DNA biosynthesis, thereby effectively suppressing tumor growth at low doses. Subsequent in vivo studies utilizing NBS‐2S‐5FU liposomes exhibit outstanding anti‐cancer effectiveness. This study highlights a promising direction for advancing combined prodrugs that integrate PDT and chemotherapy.
{"title":"A self‐reinforced activatable photosensitizer prodrug enabling synergistic photodynamic and chemotherapy","authors":"Daipeng Huang, Jikai Yin, Yang Zou, Haiqiao Huang, Saran Long, Wen Sun, Jianjun Du, Jiangli Fan, Xiaojun Peng","doi":"10.1002/smo.20240005","DOIUrl":"https://doi.org/10.1002/smo.20240005","url":null,"abstract":"As a novel drug development paradigm, selective activation of prodrugs provides the potential for precise tumor chemotherapy, thereby presenting an opportunity for advancing cancer treatment. The combination of photodynamic therapy (PDT) and prodrug can enhance the therapeutic efficacy while simultaneously enabling real‐time monitoring of drug distribution and release. However, the tumor hypoxia microenvironment and the frequent high‐dose administration of prodrugs significantly impede therapeutic efficacy and escalate treatment‐related risks. Herein, a tumor microenvironment‐specific release prodrug is constructed, termed NBS‐2S‐5FU. Under the influence of glutathione (GSH), NBS‐2S‐5FU undergoes activation, leading to the release of photosensitizer NBS and chemotherapeutic agent 5‐FU derivatives. Under irradiation, NBS produces sufficient superoxide radical () while 5‐FU derivatives inhibit DNA biosynthesis, thereby effectively suppressing tumor growth at low doses. Subsequent in vivo studies utilizing NBS‐2S‐5FU liposomes exhibit outstanding anti‐cancer effectiveness. This study highlights a promising direction for advancing combined prodrugs that integrate PDT and chemotherapy.","PeriodicalId":501601,"journal":{"name":"Smart Molecules","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-14","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141342414","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ruize Jiang, Huilin Wang, Li Liu, Baokang Geng, Xiang Chu, Yi Shi, Xiao Wang, Shuyan Song, Hongjie Zhang
Three‐way catalysts are widely used to control criterion pollutant emissions from the increasing gasoline engines. With the stringent requirements of automotive pollutant emission standards in various countries, Rh has become an irreplaceable component of three‐way catalysts due to its superior NOx elimination, high N2 selectivity, and simultaneous elimination of CO and hydrocarbons. In this review, we systematically review the recent development of Rh‐based three‐way catalysts in terms of potential supports and effective active center construction strategies. We further summarize the key role of Rh metal in the three‐way catalytic mechanism and reaction kinetics. Finally, we conclude the current challenges and future opportunities facing Rh‐based catalysts. It is believed that based on the deep understanding of Rh‐based three‐way catalysts, the design of Rh‐based catalysts with good low‐temperature catalytic performance and low cost is expected to be realized in the future.
{"title":"Recent progress of Rh‐based three‐way catalysts","authors":"Ruize Jiang, Huilin Wang, Li Liu, Baokang Geng, Xiang Chu, Yi Shi, Xiao Wang, Shuyan Song, Hongjie Zhang","doi":"10.1002/smo.20240004","DOIUrl":"https://doi.org/10.1002/smo.20240004","url":null,"abstract":"Three‐way catalysts are widely used to control criterion pollutant emissions from the increasing gasoline engines. With the stringent requirements of automotive pollutant emission standards in various countries, Rh has become an irreplaceable component of three‐way catalysts due to its superior NOx elimination, high N2 selectivity, and simultaneous elimination of CO and hydrocarbons. In this review, we systematically review the recent development of Rh‐based three‐way catalysts in terms of potential supports and effective active center construction strategies. We further summarize the key role of Rh metal in the three‐way catalytic mechanism and reaction kinetics. Finally, we conclude the current challenges and future opportunities facing Rh‐based catalysts. It is believed that based on the deep understanding of Rh‐based three‐way catalysts, the design of Rh‐based catalysts with good low‐temperature catalytic performance and low cost is expected to be realized in the future.","PeriodicalId":501601,"journal":{"name":"Smart Molecules","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141356397","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Photodynamic therapy (PDT) has become a promising method for tumor treatment due to its non‐invasive and high spatiotemporal selectivity. However, PDT is still hindered by reactive oxygen species deficiency, because solid tumors feature a hypoxic microenvironment. PDT combined with hypoxia‐activated chemotherapy drugs can effectively induce tumor death, overcoming the limitations of the sole PDT for the fight against hypoxia. Herein, we designed a nanosystem (PCe6AZOM) that enhances the release of hypoxia‐activated drugs (AZOM) by PDT. Under hypoxic conditions, the azo bond of AZOM is cleaved by azo reductase, releasing highly cytotoxic AZOM and resulting in a significant increase in intratumor drug concentration. Meanwhile, the commercial photosensitizer Ce6 can aggravate the oxygen‐poor state during the PDT process and further cause more AZOM release. Moreover, the cascade reactions in the nanosystem could activate singlet oxygen and enhance drug release through 660 nm light laser irradiation, contributing to more effective induction of tumor apoptosis and tumor growth retardation in vitro and in vivo.
{"title":"Photodynamic therapy promotes hypoxia‐activated nitrogen mustard drug release","authors":"Ran Wang, Maomao He, Zongwei Zhang, Tian Qiu, Yue Xi, Xiaolong Zeng, Jiangli Fan, Wen Sun, Xiaojun Peng","doi":"10.1002/smo.20240010","DOIUrl":"https://doi.org/10.1002/smo.20240010","url":null,"abstract":"Photodynamic therapy (PDT) has become a promising method for tumor treatment due to its non‐invasive and high spatiotemporal selectivity. However, PDT is still hindered by reactive oxygen species deficiency, because solid tumors feature a hypoxic microenvironment. PDT combined with hypoxia‐activated chemotherapy drugs can effectively induce tumor death, overcoming the limitations of the sole PDT for the fight against hypoxia. Herein, we designed a nanosystem (PCe6AZOM) that enhances the release of hypoxia‐activated drugs (AZOM) by PDT. Under hypoxic conditions, the azo bond of AZOM is cleaved by azo reductase, releasing highly cytotoxic AZOM and resulting in a significant increase in intratumor drug concentration. Meanwhile, the commercial photosensitizer Ce6 can aggravate the oxygen‐poor state during the PDT process and further cause more AZOM release. Moreover, the cascade reactions in the nanosystem could activate singlet oxygen and enhance drug release through 660 nm light laser irradiation, contributing to more effective induction of tumor apoptosis and tumor growth retardation in vitro and in vivo.","PeriodicalId":501601,"journal":{"name":"Smart Molecules","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141356546","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
The fabrication of precisely patterned polymers at the nanoscale is of critical importance. We have previously succeeded in creating various nanopatterned polymers with nanoscale resolution through the use of in situ atom transfer radical polymerization (ATRP) techniques on deoxyribonucleic acid (DNA) origami. However, separating nanopatterned polymers from the origami template without damaging the origami presents a significant challenge, thereby increasing costs and limiting the development of applications involving nanopatterned polymers. Here, we achieved spatially and temporally controlled release of DNA origami templates through photo‐regulation by incorporating azobenzene‐modified DNA into the initiator. Under UV exposure, azobenzene isomerization rapidly induces the disassociation of patterned polymers from the origami template at ambient temperatures, without damaging the DNA origami. Additionally, the released origami template can be reused as a template for the cyclic production of nanopatterned polymers. This method provides a pathway for the large‐scale production of patterned polymers at reduced costs and facilitates dynamic control over the polymer‐DNA complex, with potential applications in both the biomedical and chemical fields.
制造纳米级精确图案聚合物至关重要。此前，我们通过在脱氧核糖核酸（DNA）折纸上使用原位原子转移自由基聚合（ATRP）技术，成功地制造出了各种具有纳米级分辨率的纳米图案聚合物。然而，如何在不损坏折纸的情况下将纳米图案化聚合物从折纸模板中分离出来是一个巨大的挑战，从而增加了成本，限制了纳米图案化聚合物的应用开发。在这里，我们将偶氮苯修饰的 DNA 加入到引发剂中，通过光调节实现了 DNA 折纸模板在空间和时间上的可控释放。在紫外线照射下，偶氮苯异构化可在环境温度下迅速诱导图案化聚合物与折纸模板分离，而不会损坏 DNA 折纸。此外，释放出的折纸模板可作为模板重复使用，循环生产纳米图案聚合物。这种方法为降低成本大规模生产图案化聚合物提供了途径，并有利于对聚合物-DNA 复合物进行动态控制，有望应用于生物医学和化学领域。
{"title":"Precision fabrication of polymer nanostructures on recyclable DNA template","authors":"Zi'an Lin, Xuemei Xu, Yiwei Shi, Yuzhou Wu","doi":"10.1002/smo.20240006","DOIUrl":"https://doi.org/10.1002/smo.20240006","url":null,"abstract":"The fabrication of precisely patterned polymers at the nanoscale is of critical importance. We have previously succeeded in creating various nanopatterned polymers with nanoscale resolution through the use of in situ atom transfer radical polymerization (ATRP) techniques on deoxyribonucleic acid (DNA) origami. However, separating nanopatterned polymers from the origami template without damaging the origami presents a significant challenge, thereby increasing costs and limiting the development of applications involving nanopatterned polymers. Here, we achieved spatially and temporally controlled release of DNA origami templates through photo‐regulation by incorporating azobenzene‐modified DNA into the initiator. Under UV exposure, azobenzene isomerization rapidly induces the disassociation of patterned polymers from the origami template at ambient temperatures, without damaging the DNA origami. Additionally, the released origami template can be reused as a template for the cyclic production of nanopatterned polymers. This method provides a pathway for the large‐scale production of patterned polymers at reduced costs and facilitates dynamic control over the polymer‐DNA complex, with potential applications in both the biomedical and chemical fields.","PeriodicalId":501601,"journal":{"name":"Smart Molecules","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-11","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141356906","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Yuanyu Tang, E. Pang, Pan Zhu, Qiuxia Tan, Shaojing Zhao, Benhua Wang, Chaoyi Yao, Xiangzhi Song, Minhuan Lan
Sonodynamic therapy (SDT) is a novel cancer treatment type showing the advantages of high tissue penetration ability, non‐invasion, low systemic toxicity, and high selectivity. However, SDT depends on ultrasound (US) irradiation; once US is turned off, the sonosensitizer will stop producing reactive oxygen species (ROS). Moreover, most sonosensitizers generate oxygen‐dependent ROS, that is, singlet oxygen (1O2), significantly limiting the therapeutic effect of SDT in treating deep and hypoxic tumor. Therefore, combining SDT with other treatment modalities is essential. Here, we designed and synthesized a series of cisplatin‐coordinated copolythiophenes (CPT‐Pts), simultaneously generating 1O2, superoxide anion, and hydroxyl radicals for synergistic chemotherapy and SDT of tumor. The sonodynamic toxicity and cytotoxicity of CPT‐Pts were accurately regulated by tuning the monomer ratio of the polythiophene. This copolymerization strategy avoids the side effects originating from the high‐dose chemotherapy drug while making up for limiting SDT relying on ultrasonic activation, effectively inhibiting cancer cells and tumors.
{"title":"Cisplatin‐coordinated copolythiophene for synergistic chemotherapy and sonodynamic therapy of tumor","authors":"Yuanyu Tang, E. Pang, Pan Zhu, Qiuxia Tan, Shaojing Zhao, Benhua Wang, Chaoyi Yao, Xiangzhi Song, Minhuan Lan","doi":"10.1002/smo.20240003","DOIUrl":"https://doi.org/10.1002/smo.20240003","url":null,"abstract":"Sonodynamic therapy (SDT) is a novel cancer treatment type showing the advantages of high tissue penetration ability, non‐invasion, low systemic toxicity, and high selectivity. However, SDT depends on ultrasound (US) irradiation; once US is turned off, the sonosensitizer will stop producing reactive oxygen species (ROS). Moreover, most sonosensitizers generate oxygen‐dependent ROS, that is, singlet oxygen (1O2), significantly limiting the therapeutic effect of SDT in treating deep and hypoxic tumor. Therefore, combining SDT with other treatment modalities is essential. Here, we designed and synthesized a series of cisplatin‐coordinated copolythiophenes (CPT‐Pts), simultaneously generating 1O2, superoxide anion, and hydroxyl radicals for synergistic chemotherapy and SDT of tumor. The sonodynamic toxicity and cytotoxicity of CPT‐Pts were accurately regulated by tuning the monomer ratio of the polythiophene. This copolymerization strategy avoids the side effects originating from the high‐dose chemotherapy drug while making up for limiting SDT relying on ultrasonic activation, effectively inhibiting cancer cells and tumors.","PeriodicalId":501601,"journal":{"name":"Smart Molecules","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-07","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141374665","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
Ilse M. Welleman, Carlijn L. F. van Beek, Ioana Belcin, A. Schulte, Rudi A J O Dierckx, B. L. Feringa, H. Boersma, W. Szymański
In recent years, the use of light to selectively and precisely activate drugs has been developed along the fundamental concepts of photopharmacology. One of the key methods in this field relies on transiently silencing the drug activity with photocleavable protecting groups (PPGs). To effectively utilize light‐activated drugs in future medical applications, physicians will require a reliable method to assess whether light penetrates deep enough into the tissues to activate the photoresponsive theragnostic agents. Here, we describe the development and evaluation of magnetic resonance (MR) imaging agents that allow for the detection of light penetration and drug activation in the tissues using non‐invasive whole‐body magnetic resonance imaging (MRI) and chemical exchange saturation transfer (CEST)‐MRI modalities. The approach relies on the use of PPG‐protected MR contrast agents, which upon irradiation with light change their imaging signal. A Gadolinium(III)‐based MRI contrast agent is presented that undergoes a significant change in relaxivity (25%) upon uncaging, providing a reliable indicator of light‐induced cargo release. Additionally, we introduce the first light‐responsive CEST‐MRI imaging agent, enabling positive signal enhancement (off‐to‐on) upon light activation, offering a novel approach to visualize the activation of photoactive agents in living tissues. This research provides a proof‐of‐principle for the non‐invasive, whole‐body imaging of light penetration and drug activation with high temporal resolution characteristic of MR methods.
{"title":"Towards medical imaging of drug photoactivation: Development of light responsive magnetic resonance imaging and chemical exchange saturation transfer contrast agents","authors":"Ilse M. Welleman, Carlijn L. F. van Beek, Ioana Belcin, A. Schulte, Rudi A J O Dierckx, B. L. Feringa, H. Boersma, W. Szymański","doi":"10.1002/smo.20230029","DOIUrl":"https://doi.org/10.1002/smo.20230029","url":null,"abstract":"In recent years, the use of light to selectively and precisely activate drugs has been developed along the fundamental concepts of photopharmacology. One of the key methods in this field relies on transiently silencing the drug activity with photocleavable protecting groups (PPGs). To effectively utilize light‐activated drugs in future medical applications, physicians will require a reliable method to assess whether light penetrates deep enough into the tissues to activate the photoresponsive theragnostic agents. Here, we describe the development and evaluation of magnetic resonance (MR) imaging agents that allow for the detection of light penetration and drug activation in the tissues using non‐invasive whole‐body magnetic resonance imaging (MRI) and chemical exchange saturation transfer (CEST)‐MRI modalities. The approach relies on the use of PPG‐protected MR contrast agents, which upon irradiation with light change their imaging signal. A Gadolinium(III)‐based MRI contrast agent is presented that undergoes a significant change in relaxivity (25%) upon uncaging, providing a reliable indicator of light‐induced cargo release. Additionally, we introduce the first light‐responsive CEST‐MRI imaging agent, enabling positive signal enhancement (off‐to‐on) upon light activation, offering a novel approach to visualize the activation of photoactive agents in living tissues. This research provides a proof‐of‐principle for the non‐invasive, whole‐body imaging of light penetration and drug activation with high temporal resolution characteristic of MR methods.","PeriodicalId":501601,"journal":{"name":"Smart Molecules","volume":null,"pages":null},"PeriodicalIF":0.0,"publicationDate":"2024-06-01","publicationTypes":"Journal Article","fieldsOfStudy":null,"isOpenAccess":false,"openAccessPdf":"","citationCount":null,"resultStr":null,"platform":"Semanticscholar","paperid":"141234986","PeriodicalName":null,"FirstCategoryId":null,"ListUrlMain":null,"RegionNum":0,"RegionCategory":"","ArticlePicture":[],"TitleCN":null,"AbstractTextCN":null,"PMCID":"","EPubDate":null,"PubModel":null,"JCR":null,"JCRName":null,"Score":null,"Total":0}
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