Nanoscale probing of electron-regulated structural transitions in silk proteins by near-field IR imaging and nano-spectroscopy

Qin, Nan; Zhang, Shaoqing; Jiang, Jianjuan; Corder, Stephanie N. Gilbert; Qian, Zhi‐Gang; Zhou, Zhitao; Lee, Woonsoo; Liu, Keyin; Wang, Xiaohan; Li, Xinxin; Shi, Zhifeng; Mao, Ying; Bechtel, Hans A.; Martin, Michael; Xia, Xiao-Xia; Marelli, Benedetto; Kaplan, David L.; Omenetto, Fiorenzo G.; Liu, Mengkun; Tao, Tiger H.

doi:10.1038/ncomms13079

Cited by 90 publications

(72 citation statements)

References 40 publications

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“…The amide band positions (I, II, II) of samples from day 3 and day 7 were quite similar and of low intensity (indistinct peaks), characteristic of a random coil main conformation (1644 cm -1 and 1640 cm -1 for amide I, 1532 cm -1 and 1540 cm -1 for amide II and 1232 cm -1 and 1228 cm -1 for amide III, respectively) [ 45 , 46 ]. At day 14, all the amide signature bands shift towards higher frequency, especially those of amide I and amide II (1650 cm -1 for amide I, 1546 cm -1 for amide II and 1256 for amide III), which is a characteristic of the β-sheet structure [ 48 , 49 ]. Therefore, these results suggest that the natural conformational changes of the native SF can also spontaneously occur on the SF hydrogels over time.…”

Section: Resultsmentioning

confidence: 99%

Rapidly responsive silk fibroin hydrogels as an artificial matrix for the programmed tumor cells death

et al. 2018

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Timely and spatially-regulated injectable hydrogels, able to suppress growing tumors in response to conformational transitions of proteins, are of great interest in cancer research and treatment. Herein, we report rapidly responsive silk fibroin (SF) hydrogels formed by a horseradish peroxidase (HRP) crosslinking reaction at physiological conditions, and demonstrate their use as an artificial biomimetic three-dimensional (3D) matrix. The proposed SF hydrogels presented a viscoelastic nature of injectable hydrogels and spontaneous conformational changes from random coil to β-sheet conformation under physiological conditions. A human neuronal glioblastoma (U251) cell line was used for screening cell encapsulation and in vitro evaluation within the SF hydrogels. The transparent random coil SF hydrogels promoted cell viability and proliferation up to 10 days of culturing, while the crystalline SF hydrogels converted into β-sheet structure induced the formation of TUNEL-positive apoptotic cells. Therefore, this work provides a powerful tool for the investigation of the microenvironment on the programed tumor cells death, by using rapidly responsive SF hydrogels as 3D in vitro tumor models.

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Section: Resultsmentioning

confidence: 99%

Rapidly responsive silk fibroin hydrogels as an artificial matrix for the programmed tumor cells death

et al. 2018

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“…Silk principally consists of antiparallel β‐sheets that are stacked together to create a highly ordered β‐sheet nanocrystals which are implanted in amorphous matrix consisting of 3 1 helices and few β‐turns (Figure S1, Supporting Information) . Additionally, β‐nanocrystals reinforce the biomacromolecular chains by forming interlocks between the chains which allows the amorphous domains to stretch significantly upon stretching .…”

Section: Introductionmentioning

confidence: 99%

Silk nano‐discs: A natural material for cancer therapy

et al. 2018

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The article demonstrates the crystalline silk nano‐discs (CSNs), with well‐controlled morphology, which upon magnetization, yields magnetic crystalline silk nano‐discs, making both prominent alternatives for replacing metal templates such as gold, silver, and so on in therapeutics and implants. The isolated β‐sheet‐rich discotic CSNs have ~50 nm diameter, high crystallinity (> 90%), and are insoluble but provide good dispersibility and stability in aqueous solutions. The melt blending‐cum‐electrospinning of functionalized CSN with poly(lactic acid) results in biocompatible nanofiber‐based scaffolds having in vitro cell cytocompatibility with improved cell adhesion and proliferation. The assessment of release behavior of curcumin, a naturally occurring anticancer drug, shows sustained release over 25 days exhibiting effective cytotoxicity against human cervical cancer cells. Further, combined effect of curcumin and hyperthermia reduced the cell growth by ~63%. Alignment of CSN‐derived magnetic nanoparticles due to effective fiber drawing process during electrospinning could improve cytocompatibility against BHK‐21 cells, and therefore efficacy for cancer therapy.

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“…Because of its well‐known outstanding biocompatibility, ease of functionalization, controllable water‐solubility, and tunable degradation rate, the silk film substrate can be functionalized for controllable drug release applications. [ 35 ] As a proof of concept, the drug‐loaded therapeutic MM‐devices can serve as a skin patch for real‐time monitoring and in situ treatment with controlled drug release, providing new building blocks for constructing multifunctional biosensors for biomedical applications. [ 36 ]…”

Section: Figurementioning

confidence: 99%

Implantable, Degradable, Therapeutic Terahertz Metamaterial Devices

Sun

Zhou

Zhong

et al. 2020

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Artificially structured metamaterials (MMs) exhibit engineered responses at designed frequencies and offer new functions that are not readily available in nature. [1,2] Compared with conven tional materials whose characteristics are mainly derived from Metamaterial (MM) sensors and devices, usually consisting of artificially structured composite materials with engineered responses that are mainly determined by the unit structure rather than the bulk properties or composition, offer new functionalities not readily available in nature. A set of implantable and resorbable therapeutic MM devices at terahertz (THz) frequencies are designed and fabricated by patterning magnesium split ring resonators on drug-loaded silk protein substrates with controllable device degradation and drug release rates. To demonstrate proof-of-concept, a set of silk-based, antibiotics-loaded MM devices, which can serve as degradable antibacterial skin patches with capabilities to monitor drug-release in real time are fabricated. The extent of drug release, which correlates with the degradation of the MM skin patch, can be monitored by analyzing the resonant responses in reflection during degradation using a portable THz camera. Animal experiments are performed to demonstrate the in vivo degradation process and the efficacy of the devices for antibacterial treatment. Thus, the implantable and resorbable therapeutic MM devices do not need to be retrieved once implanted, providing an appealing alternative for in-vivo sensing and in situ treatment applications.

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Nanoscale probing of electron-regulated structural transitions in silk proteins by near-field IR imaging and nano-spectroscopy

Cited by 90 publications

References 40 publications

Rapidly responsive silk fibroin hydrogels as an artificial matrix for the programmed tumor cells death

Rapidly responsive silk fibroin hydrogels as an artificial matrix for the programmed tumor cells death

Silk nano‐discs: A natural material for cancer therapy

Implantable, Degradable, Therapeutic Terahertz Metamaterial Devices

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