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Singlet Oxygen Generation in Dark-Hypoxia by Catalytic Microenvironment-Tailored Nanoreactors for NIR-II Fluorescence-Monitored Chemodynamic Therapy

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Angewandte Chemie (International ed. in English) 2021年第27期60卷 15006-15012页

作者： Tao Chen Peidong Hou Yafei Zhang Rujiang Ao Lichao Su Yifan Jiang Yuanli Zhang Huilan Cai Jun Wang Qiushui Chen Jibin Song Lisen Lin Huanghao Yang Xiaoyuan Chen MOE Key Laboratory for Analytical Science of Food Safety and Biology College of Chemistry Fuzhou University Fuzhou 350108 China. Departments of Diagnostic Radiology Chemical and Biomolecular Engineering and Biomedical Engineering Yong Loo Lin School of Medicine and Faculty of Engineering National University of Singapore Singapore 117597 Singapore. Clinical Imaging Research Centre Centre for Translational Medicine Yong Loo Lin School of Medicine National University of Singapore Singapore 117599 Singapore. Nanomedicine Translational Research Program NUS Center for Nanomedicine Yong Loo Lin School of Medicine National University of Singapore Singapore 117597 Singapore.

Singlet oxygen ( O ) has a potent anticancer effect, but photosensitized generation of O is inhibited by tumor hypoxia and limited light penetration depth. Despite the potential of chemodynamic therapy (CDT) to circumvent these issues by exploration of O -producing catalysts, engineering efficient CDT agents is still a formidable challenge since most catalysts require specific pH to function and become inactivated upon chelation by glutathione (GSH). Herein, we present a catalytic microenvironment-tailored nanoreactor (CMTN), constructed by encapsulating MoO catalyst and alkaline sodium carbonate within liposomes, which offers a favorable pH condition for MoO -catalyzed generation of O from H O and protects MoO from GSH chelation owing to the impermeability of liposomal lipid membrane to ions and GSH. H O and O can freely cross the liposomal membrane, allowing CMTN with a built-in NIR-II ratiometric fluorescent O sensor to achieve monitored tumor CDT.

关键词： NIR-II ratiometric fluorescence catalytic microenvironment chemodynamic therapy nanoreactors singlet oxygen

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Controlled synthetic chirality in macroscopic assemblies of carbon nanotubes

arXiv

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arXiv 2023年

作者： Doumani, Jacques Lou, Minhan Dewey, Oliver Hong, Nina Fan, Jichao Baydin, Andrey Yomogida, Yohei Yanagi, Kazuhiro Pasquali, Matteo Saito, Riichiro Kono, Junichiro Gao, Weilu Department of Electrical and Computer Engineering Rice University HoustonTX United States Applied Physics Graduate Program Smalley–Curl Institute Rice University HoustonTX United States Department of Electrical and Computer Engineering The University of Utah Salt Lake CityUT United States Carbon Hub Rice University HoustonTX United States Department of Chemical and Biomolecular Engineering Rice University HoustonTX United States J.A. Woollam Co. Inc. LincolnNE United States Smalley–Curl Institute Rice University HoustonTX United States Department of Physics Tokyo Metropolitan University Tokyo Japan Department of Chemistry Rice University HoustonTX United States Department of Materials Science and NanoEngineering Rice University HoustonTX United States Department of Physics Tohoku University Sendai Japan Department Physics and Astronomy Rice University HoustonTX United States

There is an emerging recognition that successful utilization of chiral degrees of freedom can bring new scientific and technological opportunities to diverse research areas. Hence, methods are being sought for creating artificial matter with controllable chirality in an uncomplicated and reproducible manner. Here, we report the development of two straightforward methods for fabricating wafer-scale chiral architectures of ordered carbon nanotubes (CNTs) with tunable and giant circular dichroism (CD). Both methods employ simple approaches, (i) mechanical rotation and (ii) twist-stacking, based on controlled vacuum filtration and do not involve any sophisticated nanofabrication processes. We used a racemic mixture of CNTs as the starting material, so the intrinsic chirality of chiral CNTs is not responsible for the observed chirality. In particular, by controlling the stacking angle and handedness in (ii), we were able to maximize the CD response and achieve a record-high deep-ultraviolet ellipticity of 40 ± 1 mdeg/nm. Our theoretical simulations using the transfer matrix method reproduce the salient features of the experimentally observed CD spectra and further predict that a film of twist-stacked CNTs with an optimized thickness will exhibit an ellipticity as high as 150 mdeg/nm. The created wafer-scale objects represent a new class of synthetic chiral matter consisting of ordered quantum wires whose macroscopic properties are governed by nanoscopic electronic signatures such as van Hove singularities. These artificial structures with engineered chirality will not only provide playgrounds for uncovering new chiral phenomena but also open up new opportunities for developing high-performance chiral photonic and optoelectronic devices. © 2023, CC BY.

关键词： Carbon nanotubes

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Monitoring and dynamically controlling glucose uptake rate and central metabolism

Nature Chemical Engineering

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Nature Chemical engineering 2025年 1-13页

作者： Dongqin Ding Yaru Zhu Danyang Bai Tongxin Wan Dawei Zhang Sang Yup Lee Tianjin Institutes of Industrial Biotechnology Chinese Academy of Sciences Tianjin P. R. China National Technology Innovation Center of Synthetic Biology Tianjin P. R. China University of Chinese Academy of Sciences Beijing P. R. China College of Biotechnology Engineering Tianjin University of Science and Technology Tianjin P. R. China Department of Chemical and Biomolecular Engineering (BK21 four program) Korea Advanced Institute of Science and Technology (KAIST) 291 Daehak-ro Yuseong-gu Daejeon Republic of Korea

The rate of glucose import directly affects the maximum possible flux of central carbon metabolism. However, few tools can directly monitor the cellular glucose uptake rate. Here we report the development of a set of programmable bifunctional glucose uptake rate biosensors (GURBs) for real-time monitoring of glucose uptake rate, which enable the dynamic activation and inhibition of glucose uptake and central metabolism inEscherichia coli. These genetic circuits are used to monitor the glucose uptake rates of strains under different culture conditions. Also, feedback-loop control systems are designed to make cells rely on the glucose uptake rate to tune the target metabolic modules, resulting in a substantial increase of the titers ofl-tryptophan, riboflavin andd-lactic acid. The glucose-uptake-rate-responsive genetic circuits developed in this study will serve as an effective tool for the dynamic control of glucose uptake and central metabolism.

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DNA origami technology for biomedical applications: Challenges and opportunities

MedComm - Biomaterials and Applications

引用

MedComm - Biomaterials and Applications 2023年第2期2卷

作者： Li, Ling Nie, Shihong Du, Ting Zhao, Jiaxuan Chen, Xiaoyuan West China School of Public Health West China Fourth Hospital and State Key Laboratory of Biotherapy Sichuan University Chengdu China Department of Radiation Oncology Cancer Center West China Hospital Sichuan University Chengdu China Non-coding RNA and Drug Discovery Key Laboratory of Sichuan Province Chengdu Medical College Chengdu China Departments of Diagnostic Radiology Surgery Chemical and Biomolecular Engineering and Biomedical Engineering Yong Loo Lin School of Medicine and Faculty of Engineering National University of Singapore Singapore Singapore Clinical Imaging Research Centre Centre for Translational Medicine Yong Loo Lin School of Medicine National University of Singapore Singapore Singapore Nanomedicine Translational Research Program NUS Center for Nanomedicine Yong Loo Lin School of Medicine National University of Singapore Singapore Singapore Institute of Molecular and Cell Biology Agency for Science Technology and Research (A*STAR) Singapore Singapore

DNA origami, a promising branch of structural DNA technology, refers to the technique of folding a single-stranded DNA scaffold into well-defined nanostructures. In recent years, DNA origami nanostructures have shown considerable promise in a variety of biomedical applications, owing to their biodegradability, unique programmability, and addressability. Despite their popularity, the biomedical application of DNA origami techniques, which exploits their unique programmability and addressability, is rare in previous studies. Most recently, mounting evidence has demonstrated the robustness of DNA origami nanostructures in the spatial organization of functional components at the nanoscale in the biomedical field. These examples provide typical paradigms to fully realize the potential of DNA origami techniques by taking advantage of their unique programmability and addressability. This minireview summarizes the recent advancements of DNA origami techniques in biosensing, biocatalysis, and drug delivery, and the representative examples using DNA origami nanostructures for the spatial organization of functional molecules with nanometric precision are highlighted. We further discuss the possible limitations and challenges for in vivo applications, including stability issues and potential immunogenicity, and finally, propose some strategies to overcome these obstacles to fully realize the potential of DNA origami techniques in biomedical applications. © 2023 The Authors. MedComm – Biomaterials and Applications published by John Wiley & Sons Australia, Ltd on behalf of Sichuan International Medical Exchange & Promotion Association (SCIMEA).

关键词： biocatalysis biosensing DNA nanotechnology DNA origami

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A facile strategy for the preparation of end-capped and cross-linkable poly(propylene carbonate) with high performance

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Advanced Industrial and engineering Polymer Research 2019年第4期2卷 161-166页

作者： Song, Pengfei Ran, Baocheng Shang, Yingqi Kang, Li Chen, Yalun Sun, Luyi College of Chemistry and Chemical Engineering Gansu International Scientific and Technological Cooperation Base of Water-Retention Chemical Functional Materials Key Laboratory of Eco-functional Polymer Materials of the Ministry of Education Key Laboratory of Eco-environmental Polymer Materials of Gansu Province Northwest Normal University Lanzhou730070 China Polymer Program Institute of Materials Science Department of Chemical & Biomolecular Engineering University of Connecticut StorrsCT06269 United States

Itaconic anhydride (IAn) was firstly used for the modification of poly(propylene carbonate) (PPC) by solution blending following with the direct heating treatment, producing end-capped and cross-linkable PPC (PECPPC) with high performance. The reaction of PPC with IAn was detailed investigated and the structure of PECPPC was identified by FTIR and 1H NMR. A facile strategy including end-capping and cross-linking can be developed to improve the performance of PPC. Differential scanning calorimetry (DSC) and thermogravimetric analysis (TGA) measurements revealed that the glass transition temperature (Tg) and thermal decomposition temperature (Td) of PECPPCs are all much higher than those of PPC and increased with the increasing content of IAn. Tensile tests also showed the huge enhancement on the mechanical properties of PPC with the end-capping and cross-linking techniques, and the highest tensile strength of PECPPC4 is 37.5 MPa. Furthermore, ECPPC4 exhibits high hydrolysis rate in phosphate buffer solution (PBS) than that of PPC. It is demonstrated that the strategy with the combination of end-capping and cross-linking is efficient for the perfect modification of PPC with IAn. © 2019 Kingfa SCI. & TECH. CO., LTD.

关键词： Differential scanning calorimetry

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Correction: Influence of shape on crystal structure and optical properties of heterocyclic conjugated molecules

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Journal of Materials Chemistry C 2025年第10期13卷 5385-5385页

作者： Elisa Guzmán Yu Yan Peter Müller Justin Amengual Chung-Hao Liu Mu-Ping Nieh Department of Chemistry Tufts University 62 Talbot Ave Medford MA 02155 USA Department of Chemistry Massachusetts Institute of Technology Cambridge MA 02139 USA Polymer Program Institute of Materials Science University of Connecticut 25 King Hill Road Storrs CT 06269-3136 USA Department of Chemical & Biomolecular Engineering University of Connecticut – Storrs 97 North Eagleville Road Unit 3136 Storrs CT-06269-3136 USA

Correction for ‘Influence of shape on crystal structure and optical properties of heterocyclic conjugated molecules’ by Elisa Guzmán et al., J. Mater. Chem. C, 2025, 13, 954–962, https://***/10.1039/D4TC03509G.

Correction for ‘Influence of shape on crystal structure and optical properties of heterocyclic conjugated molecules’ by Elisa Guzmán et al., J. Mater. Chem. C, 2025, 13, 954–962, https://***/10.1039/D4TC03509G.

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Full Crystallographic Imaging of Hexagonal Boron Nitride Monolayers with Phonon-Enhanced Sum-Frequency Microscopy

arXiv

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arXiv 2025年

作者： Mueller, Niclas S. Fellows, Alexander P. John, Ben Naclerio, Andrew E. Carbogno, Christian Gharagozloo-Hubmann, Katayoun Baláž, Damián Kowalski, Ryan A. Heenen, Hendrik H. Scheurer, Christoph Reuter, Karsten Caldwell, Joshua D. Wolf, Martin Kidambi, Piran R. Thämer, Martin Paarmann, Alexander Department of Physical Chemistry Fritz-Haber-Institute of the Max-Planck-Society Berlin14195 Germany Department of Chemical and Biomolecular Engineering Vanderbilt University NashvilleTN37235 United States Theory Department Fritz-Haber-Institute of the Max-Planck-Society Berlin14195 Germany Department of Physics Freie Universität Berlin Berlin14195 Germany Department of Mechanical Engineering Vanderbilt University NashvilleTN37235 United States Interdisciplinary Materials Science Program Vanderbilt University NashvilleTN37235 United States

Hexagonal boron nitride (hBN) is an important 2D material for van der Waals heterostructures, single photon emitters, and infrared nanophotonics. The optical characterization of mono- and few-layer samples of hBN however remains a challenge as the material is almost invisible optically. Here we introduce phase-resolved sum-frequency microscopy as a technique for imaging monolayers of hBN grown by chemical vapor deposition (CVD) and visualize their crystal orientation. A combination of femtosecond mid-infrared (IR) and visible laser pulses is used for sum-frequency generation (SFG), which is imaged in a wide-field optical microscope. The IR laser resonantly excites a phonon of hBN that leads to an ~800-fold enhancement of the SFG intensity, making it possible to image large 100x100 µm2 sample areas in less than 1 s. Implementing heterodyne detection in combination with azimuthal rotation of the sample further provides full crystallographic information. Through combined knowledge of topography and crystal orientation, we find that triangular domains of CVD-grown monolayer hBN have nitrogen-terminated zigzag edges. Overall, SFG microscopy can be used as an ultra-sensitive tool to image crystal structure, strain, stacking sequences, and twist angles, and is applicable to the wide range of van der Waals structures, where location and identification of monolayer regions and interfaces with broken inversion symmetry is of paramount importance. © 2025, CC BY.

关键词： Van der Waals forces

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Influence of compatibilizer and carbon nanotubes on mechanical, electrical, and barrier properties of PTT/ABS blends

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Advanced Industrial and engineering Polymer Research 2019年第3期2卷 121-125页

作者： Braga, Natália F. LaChance, Anna Marie Liu, Bin Sun, Luyi Passador, Fabio R. Technology Laboratory of Polymers and Biopolymers Federal University of São Paulo São José dos CamposSP12231-280 Brazil Polymer Program Institute of Materials Science University of Connecticut StorrsCT06269 United States Department of Chemical and Biomolecular Engineering University of Connecticut StorrsCT06269 United States Beijing Key Laboratory of Electrochemical Process and Technology for Materials College of Materials Science and Engineering Beijing University of Chemical Technology Beijing100029 China Department of Biomedical Engineering University of Connecticut StorrsCT06269 United States

Composites based on poly (trimethylene terephthalate) (PTT)/acrylonitrile butadiene styrene (ABS) blend with maleic anhydride grafted PTT (PTT-g-MA) as a compatibilizer and carbon nanotubes (CNTs) as reinforcers were prepared via melt-mixing, and the mechanical, electrical, and barrier properties of the as-fabricated composites were evaluated. Scanning electron microscopy (SEM) characterization of the cross-section of the composites after tensile test showed improved phase stability in the presence of the compatibilizer PTT-g-MA. The toughness of the composites was also improved with the addition of the compatibilizer and CNTs. Electrical conductivity tests were carried out and the results showed that CNT-reinforced composite exhibited significantly increased conductivity. Since barrier properties are very sensitive to structural changes, the oxygen transmission rate (OTR) of the composites was measured and the results showed that the composites possess a much high oxygen barrier compared to that of the neat PTT or ABS. © 2019 Kingfa SCI. & TECH. CO., LTD.

关键词： Carbon nanotubes

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Correction to: Pincus blob elasticity in an intrinsically disordered protein

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The European Physical Journal E 2023年第12期46卷 1-1页

作者： Truong, Hoang P. Morgan, Ian L. Koren, Gil Avinery, Ram Beck, Roy Saleh, Omar A. Materials Department University of California Santa Barbara USA Biomolecular Science and Engineering Program University of California Santa Barbara USA The Raymond and Beverly Sackler School of Physics and Astronomy and The Center for Nanoscience and Nanotechnology Tel Aviv University Tel Aviv Israel The Center of Physics and Chemistry of Living Systems Tel Aviv University Tel Aviv Israel Physics Department University of California Santa Barbara USA

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Responsive self-assembly of tectoRNAs with loop-receptor interactions from the tetrahydrofolate (THF) riboswitch

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NUCLEIC ACIDS RESEARCH 2019年第12期47卷 6439-6451页

作者： Mitchell, Charles Polanco, Julio A. DeWald, Laura Kress, Dustin Jaeger, Luc Grabow, Wade W. Department of Chemistry and Biochemistry Seattle Pacific University Seattle WA 918119-1997 USA Department of Chemistry and Biochemistry Biomolecular Science and Engineering Program University of California Santa Barbara CA 93106-9510 USA Department of Chemistry and Biochemistry Seattle Pacific University Seattle WA 918119-1997 USA Department of Chemistry and Biochemistry Seattle Pacific University Seattle WA 918119-1997 USA Department of Chemistry and Biochemistry Biomolecular Science and Engineering Program University of California Santa Barbara CA 93106-9510 USA Correspondence may also be addressed to Luc Jaeger. Tel: +1 805 893 3628 Email: jaeger@chem.ucsb.edu Department of Chemistry and Biochemistry Seattle Pacific University Seattle WA 918119-1997 USA To whom correspondence should be addressed. Tel: +1 206 281 2016 Email: grabow@spu.edu

Naturally occurring RNAs are known to exhibit a high degree of modularity, whereby specific structural modules (or motifs) can be mixed and matched to create new molecular architectures. The modular nature of RNA also affords researchers the ability to characterize individual structural elements in controlled synthetic contexts in order to gain new and critical insights into their particular structural features and overall performance. Here, we characterized the binding affinity of a unique loop-receptor interaction found in the tetrahydrofolate (THF) riboswitch using rationally designed self-assembling tectoRNAs. Our work suggests that the THF loop-receptor interaction has been fine-tuned for its particular role as a riboswitch component. We also demonstrate that the thermodynamic stability of this interaction can be modulated by the presence of folinic acid, which induces a local structural change at the level of the loop-receptor. This corroborates the existence of a THF binding site within this tertiary module and paves the way for its potential use as a THF responsive module for RNA nanotechnology and synthetic biology.

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