Pressing-Induced Caking: A General Strategy to Scale-Span Molecular Self-Assembly

Jin, Hongjun; Xie, Mengqi; Wang, Wenkai; Jiang, Lingxiang; Wang, Chang; Sun, Yue; Xu, Limin; Zang, Shihao; Huang, Jianbin; Yan, Yun; Jiang, Lei

doi:10.31635/ccschem.020.201900088

Cited by 25 publications

(42 citation statements)

References 37 publications

(38 reference statements)

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“…With increasing the environmental humidity, the physically adsorbed water would bond preferably with the ionic groups of PLL and OL 58 , which weakens the electrostatic interaction between them. As a result, the PLL chains would swell, and the hydrogen bonding between the clusteroluminogens is destroyed.…”

Section: Discussionmentioning

confidence: 99%

“…Herein, we report a case of CPL generated from purely organic CTE using the strategy of solid-phase molecular self-assembly (SPMSA) proposed by us 58 – 60 . In this strategy, a precipitate composed of a pair of oppositely charged polyelectrolyte and amphiphile was first generated in water, and further subjected to mild mechanical pressure to facilitate the merging of nanometer-sized hydrophobic domains into mesophases.…”

Section: Introductionmentioning

confidence: 99%

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Generating circularly polarized luminescence from clusterization‐triggered emission using solid phase molecular self-assembly

Liao

Zang

et al. 2021

Nat Commun

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Purely-organic clusterization‐triggered emission (CTE) has displayed promising abilities in bioimaging, chemical sensing, and multicolor luminescence. However, it remains absent in the field of circularly polarized luminescence (CPL) due to the difficulties in well-aligning the nonconventional luminogens. We report a case of CPL generated with CTE using the solid phase molecular self-assembly (SPMSA) of poly-L-lysine (PLL) and oleate ion (OL), that is, the macroscopic CPL supramolecular film self-assembled by the electrostatic complex of PLL/OL under mechanical pressure. Well-defined interface charge distribution, given by lamellar mesophases of OL ions, forces the PLL chains to fold regularly as a requirement of optimal electrostatic interactions. Further facilitated by hydrogen bonding, the through-space conjugation (TSC) of orderly aligned electron-rich O and N atoms leads to CTE-based CPL, which is capable of transferring energy to an acceptor via a Förster resonance energy transfer (FRET) process, making it possible to develop environmentally friendly and economic CPL from sustainable and renewable materials.

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Section: Discussionmentioning

confidence: 99%

Section: Introductionmentioning

confidence: 99%

Generating circularly polarized luminescence from clusterization‐triggered emission using solid phase molecular self-assembly

Liao

Zang

et al. 2021

Nat Commun

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“…In this way, the clusteroluminogens are aligned on the surface of the 2D OL bilayers. With increasing the environmental humidity, the physically adsorbed water would bond preferably with the ionic groups of PLL and OL 44 , with weakens the electrostatic interaction between them. As a result, the PLL chains would swell, and the hydrogen bonding between the clusteroluminogens was destroyed.…”

Section: Discussionmentioning

confidence: 99%

“…It still remains an insurmountable challenge to align the clusteroluminogens in a CTE system. Herein, we report the first case of CPL generated from CTE using the strategy of solid phase molecular self-assembly (SPMSA) proposed by us [44][45][46] . In this strategy, a precipitate composed of a pair of oppositely charged polyelectrolyte and amphiphile was first generated in water, which was further subjected to mild mechanical pressure to facilitate merging of the nanometer-sized hydrophobic domains into mesophases.…”

Section: Introductionmentioning

confidence: 99%

Generating Circularly Polarized Light from Clustering‐Triggered Emission Using Solid Phase Molecular Self-Assembly

Liao¹,

Zang²,

Wu³

et al. 2021

Preprint

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Clustering-triggered emission (CTE) has displayed promising abilities in bioimaging, chemical sensing, and multicolor luminescence. However, it remains absent in the field of circularly polarized emission (CPL) due to the difficulties in well-aligning the nonconventional luminogens. We report the first case of CPL generated with CTE using the solid phase molecular self-assembly(SPMSA) of poly-L-lysine(PLL) and sodium oleate (OL). Under mechanical pressure, the electrostatic complex of PLL/OL form supramolecular film in which the OL ions self-assemble into lamellar mesophases bridged by the PLL chains. Since the OL mesophases are very alike giant 2D rigid supramolecular polymers with well-defined surface charge distribution, the PLL chains are forced to fold regularly as a requirement of optimal electrostatic interaction. Further facilitated by hydrogen bonding, the O and N atoms that form through space conjugation aligned orderly on the 2D surface, leading to CTE-based CPL. The CTE-based CPL is in analogy with conventional emission, which is capable to transfer its energy to a donor via a FRET process, making it possible to develop environmental friendly and economic CPL from sustained and renewable materials.

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“…[37][38][39][40][41][42] However, the fabrication of robust biological fibers by the introduction of DOPA is rarely reported. In this context, by a combination of those supramolecular interactions, [43][44][45][46] it is possible to manipulate the mechanical properties of protein fibers in a flexible way. Therefore, it becomes an attractive goal to design and fabricate mechanically strong protein fibers by utilizing a DOPA-based strategy.…”

Section: Introductionmentioning

confidence: 99%

Proteinaceous Fibers with Outstanding Mechanical Properties Manipulated by Supramolecular Interactions

Sun

Wang

et al. 2021

CCS Chem

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Proteinaceous fibers based on spidroins have attracted widespread attention due to their lightweight and mechanically strong properties. Presently, mechanical modulation is mainly dependent on the ultrahigh molecular weight of recombinant proteins. This makes it difficult to construct and express the target proteins. It is thus significant to develop alternative strategies for the fabrication of robust biological fibers. Herein, we demonstrate one new type of engineered protein fibers using electrostatic complexation of the cationic elastins and anionic dihydroxyphenylalanine surfactants. Interestingly, the mechanical performance of the resulting fibers can be modulated by multiple supramolecular interactions in the system including electrostatic force, hydrogen bonding, metal coordination, cation-π and other aromatic interactions. Consequently, significant alternation of the fibers' breaking strength (from 32 to 160 MPa), Young's modulus (from 0.8 to 17 GPa), and toughness (from 1.2 to 99 MJ•m −3 ) has been achieved. Moreover, the fibers exhibit high plasticity; for example, the formation of different helical structures, and strong fluorescence after the introduction of Tb chelation. Therefore, this study offers new strategies for the mechanical regulation of engineered protein fibers.

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Pressing-Induced Caking: A General Strategy to Scale-Span Molecular Self-Assembly

Cited by 25 publications

References 37 publications

Generating circularly polarized luminescence from clusterization‐triggered emission using solid phase molecular self-assembly

Generating circularly polarized luminescence from clusterization‐triggered emission using solid phase molecular self-assembly

Generating Circularly Polarized Light from Clustering‐Triggered Emission Using Solid Phase Molecular Self-Assembly

Proteinaceous Fibers with Outstanding Mechanical Properties Manipulated by Supramolecular Interactions

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