Intrinsically Fluorescent Silks from Silkworms Fed with Rare-Earth Upconverting Phosphors

Zheng, Xiaoting; Zhao, Menglu; Zhang, Huihui; Fan, Suna; Shao, Huili; Hu, Xuechao; Zhang, Yaopeng

doi:10.1021/acsbiomaterials.8b00986

Cited by 34 publications

(13 citation statements)

References 42 publications

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“…[ 7,8 ] Therefore, feeding silkworms with nontoxic, biocompatible, environmental benign, highly luminescent, and low‐cost substances seems to be the optimal strategy to produce fluorescent silk. [ 9–11 ]…”

Section: Introductionmentioning

confidence: 99%

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Mulberry‐Leaves‐Derived Red‐Emissive Carbon Dots for Feeding Silkworms to Produce Brightly Fluorescent Silk

2022

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luminescent, and low-cost substances seems to be the optimal strategy to produce fluorescent silk. [9][10][11] Carbon dots (CDs) are the most competitive candidates for the above target, because they have shown outstanding biocompatibility and superior fluorescence in previous research such as bioimaging, [12,13] drug delivery, [14,15] and photothermal therapy. [16,17] In fact, many CDs are made from biomass, which guarantees the biosafety, low price, and green chemistry in CDs production. [18] In comparison with fluorescent organic dyes, rare earth nanoparticles, and semiconductor quantum dots, CDs would be the optimal choice for feeding silkworms. In 2019, blue-emissive CDs were first employed to feed silkworms, which produced blue-emissive silk with enhanced mechanical properties. [19] In the same year, blue-emissive CDs, CdSe/ZnS quantum dots, and rhodamine were fed to silkworms which produced the corresponding blue, green and red fluorescent silk, respectively. [20] By far, CDs-derived fluorescent silk with longer emission wavelengths has not been reported yet. The reasons lie in the state of the art for CDs. On one hand, there are only a few reports about red-emissive CDs with both high quantum yield (QY) and narrow emission peaks, and even fewer red-emissive CDs that could be made in a large scale at low cost. [21][22][23][24][25][26][27][28][29][30][31][32][33][34][35] On the other, hydrophilic CDs are quickly discharged from the silkworm body and are not suitable for dyeing silkworms, while hydrophobic CDs are apt to accumulate excessively in the body and cause serious harm to silkworms, [10] because most of the hydrophobic CDs are made from aromatic compounds at present. [31,36] Therefore, it is really a challenge to synthesize hydrophobic red-emissive CDs from cheap biomass, which must adhere to the body and the silk of silkworms safely for a long time.After screening many routes and carbon sources, we find a green and sustainable approach to prepare deep-red-emissive CDs (R-CDs) from mulberry leaves. The as-prepared CDs have a main emission peak at 676 nm with a shoulder at 725 nm, possessing an full width at half maximum (FWHM) of 20 nm and QY of 73%. They are the brightest deep-red-emissive CDs so far to our knowledge. Since their strong red fluorescence can be observed by naked eyes under a wide range of excitation wavelengths from UV to red, even in the sunlight, the R-CDs-fed silkworms can be monitored under the visible light irradiation safely. During several months' observation, these R-CDs-fed Fluorescent silk has promising applications in dazzling textiles, biological engineering, and medical products, but the natural Bombyx mori silk has almost no fluorescence. Here carbon dots (CDs) made from mulberry leaves are reported, which have a strong near-infrared fluorescence with absolute quantum yield of 73% and a full width at half maximum of 20 nm. After feeding with such CDs, silkworms exhibit bright red fluorescence, grow healthily, cocoon normally, and turn to moths finally. The cocoons are ...

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Section: Introductionmentioning

confidence: 99%

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Mulberry‐Leaves‐Derived Red‐Emissive Carbon Dots for Feeding Silkworms to Produce Brightly Fluorescent Silk

2022

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“…It has been widely used in the biomedical field, textile industry, and even as an engineering material due to its favorable biocompatibility, controllable biodegradability, lustrous appearance, and excellent mechanical properties [ 1 , 2 , 3 , 4 ]. Various functional components, such as fluorescent proteins [ 5 ], rare-earth upconverting phosphors [ 6 ], antimicrobial agents [ 7 , 8 ], metal ions [ 9 ], metal and semiconductor nanodroplets [ 10 , 11 ], and graphene quantum dots [ 12 , 13 , 14 ], have been used to intrinsically produce functionalized silks. Extrinsic and intrinsic functionalization approaches have been used to improve the performance of silk.…”

Section: Introductionmentioning

confidence: 99%

Feeding Alginate-Coated Liquid Metal Nanodroplets to Silkworms for Highly Stretchable Silk Fibers

Gao

Zheng

et al. 2022

Nanomaterials

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In this study, we fed the larval of Bombyx mori silkworms with nanodroplets of liquid metal (LM) coated with microgels of marine polysaccharides to obtain stretchable silk. Alginate-coated liquid metal nanodroplets (LM@NaAlg) were prepared with significant chemical stability and biocompatibility. This study demonstrates how the fed LM@NaAlg acts on the as-spun silk fiber. We also conducted a series of characterizations and steered molecular dynamics simulations, which showed that the LM@NaAlg additions impede the conformation transition of silk fibroins from the random coil and α-helix to the β-sheet by the formation of hydrogen bonds between LM@NaAlg and the silk fibroins, thus enhancing the elongation at the breakpoints in addition to the tensile properties. The intrinsically highly stretchable silk showed outstanding mechanical properties compared with regular silk due to its 814 MPa breaking strength and a breaking elongation of up to 70%—the highest reported performance so far. We expect that the proposed method can expand the fabrication of multi-functional silks.

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“…The use of Ln-doped fibers in photonics is well-known, and several studies have reported that the presence of lanthanides can confer photochromic, luminescent and fluorescent properties as well as up-conversion ability to fibers. Examples could be Eu +3 or Dy +3 strontium aluminate luminescent fibers produced by a special spinning technology, with the substrate of polyester, nylon, or polypropylene resin ( Guo et al, 2011 ), fluorescent Pr +3 and Dy +3 -doped Chalcogenide fibers ( Chahal et al, 2016 ), Er +3 /Yb +3 /Tm +3 tri-doped tellurite glass microsphere coupled by tapered fibers ( Liu et al, 2020 ), fluorescent silks obtained from silkworms fed with rare-earth upconverting phosphors ( Zheng et al, 2018 ). Moreover, Ln-doped fibers have been employed in the production of lasers (amplifiers rare-earth-doped silica and fluorozirconate fibers, particularly erbium-doped fibers) ( Digonnet, 2001 ) and smart Dy +3 and Eu +3 doped stimuli-responsive textiles ( Shen et al, 2021 ).…”

Section: Introductionmentioning

confidence: 99%

Bombyx mori Silk Fibroin Regeneration in Solution of Lanthanide Ions: A Systematic Investigation

Rizzo

Presti

Giannini

et al. 2021

Front. Bioeng. Biotechnol.

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Silk Fibroin (SF) obtained from Bombyx mori is a very attractive biopolymer that can be useful for many technological applications, from optoelectronics and photonics to biomedicine. It can be processed from aqueous solutions to obtain many scaffolds. SF dissolution is possible only with the mediation of chaotropic salts that disrupt the secondary structure of the protein. As a consequence, recovered materials have disordered structures. In a previous paper, it was shown that, by modifying the standard Ajisawa’s method by using a lanthanide salt, CeCl3, as the chaotropic agent, it is possible to regenerate SF as a fibrous material with a very ordered structure, similar to that of the pristine fiber, and doped with Ce+3 ions. Since SF exhibits a moderate fluorescence which can be enhanced by the incorporation of organic molecules, ions and nanoparticles, the possibility of doping it with lanthanide ions could be an appealing approach for the development of new photonic systems. Here, a systematic investigation of the behavior of degummed SF in the presence of all lanthanide ions, Ln+3, is reported. It has been found that all lanthanide chlorides are chaotropic salts for solubilizing SF. Ln+3 ions at the beginning and the end of the series (La+3, Pr+3, Er+3, Tm+3, Yb+3, Lu+3) favor the reprecipitation of fibrous SF as already found for Ce+3. In most cases, the obtained fiber preserves the morphological and structural features of the pristine SF. With the exception of SF treated with La+3, Tm+3, and Lu+3, for all the fibers re-precipitated a concentration of Ln+3 between 0.2 and 0.4% at was measured, comparable to that measured for Ce+3-doped SF.

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Intrinsically Fluorescent Silks from Silkworms Fed with Rare-Earth Upconverting Phosphors

Cited by 34 publications

References 42 publications

Mulberry‐Leaves‐Derived Red‐Emissive Carbon Dots for Feeding Silkworms to Produce Brightly Fluorescent Silk

Mulberry‐Leaves‐Derived Red‐Emissive Carbon Dots for Feeding Silkworms to Produce Brightly Fluorescent Silk

Feeding Alginate-Coated Liquid Metal Nanodroplets to Silkworms for Highly Stretchable Silk Fibers

Bombyx mori Silk Fibroin Regeneration in Solution of Lanthanide Ions: A Systematic Investigation

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