scholarly journals Multiscale structural control of linked metal–organic polyhedra gel by aging-induced linkage-reorganization

2021 ◽  
Vol 12 (38) ◽  
pp. 12556-12563
Author(s):  
Zaoming Wang ◽  
Christian Villa Santos ◽  
Alexandre Legrand ◽  
Frederik Haase ◽  
Yosuke Hara ◽  
...  

By a controlled post-synthetic aging process, we demonstrate a protocol to induce the linkage reorganization in metal–organic polyhedra-linked gel networks, leading to the control of gel structures over multiple length scales and their properties.

2021 ◽  
Author(s):  
Zaoming Wang ◽  
Christian Villa Santos ◽  
alexandre legrand ◽  
Frederik Haase ◽  
Yosuke Hara ◽  
...  

Assembly of permanently porous metal-organic cages with functional polymers forms soft supramolecular networks featuring both porosity and processability. However, the amorphous nature of such soft materials complicates their characterization and thus limits structural control. Here we demonstrated that aging is an effective strategy to control the hierarchical network of supramolecular gels, which are assembled from organic ligands as linkers and metal-organic polyhedra (MOP) as junctions. Normally, the initial gel formation by rapid gelation leads to a kinetically trapped structure with low controllability. Through a controlled post-synthetic aging process, we show that it is possible to tune the network of the linked MOP gel over multiple length scales. This process allows control on the molecular-scale rearrangement of interlinking MOPs, mesoscale fusion of colloidal particles and macroscale densification of the whole colloidal network. In this work we elucidate the relationships between the gel properties, such as porosity and rheology, and their hierarchical structures, which suggest that porosity measurement can be used as a powerful tool to characterize the microscale structural transition of the amorphous gels. This aging strategy can be applied in other supramolecular polymer systems particularly containing kinetically controlled structures and shows an opportunity to engineer the structure and porosity of amorphous porous soft materials for further applications.


2021 ◽  
Author(s):  
Zaoming Wang ◽  
Christian Villa Santos ◽  
alexandre legrand ◽  
Frederik Haase ◽  
Yosuke Hara ◽  
...  

Assembly of permanently porous metal-organic cages with functional polymers forms soft supramolecular networks featuring both porosity and processability. However, the amorphous nature of such soft materials complicates their characterization and thus limits structural control. Here we demonstrated that aging is an effective strategy to control the hierarchical network of supramolecular gels, which are assembled from organic ligands as linkers and metal-organic polyhedra (MOP) as junctions. Normally, the initial gel formation by rapid gelation leads to a kinetically trapped structure with low controllability. Through a controlled post-synthetic aging process, we show that it is possible to tune the network of the linked MOP gel over multiple length scales. This process allows control on the molecular-scale rearrangement of interlinking MOPs, mesoscale fusion of colloidal particles and macroscale densification of the whole colloidal network. In this work we elucidate the relationships between the gel properties, such as porosity and rheology, and their hierarchical structures, which suggest that porosity measurement can be used as a powerful tool to characterize the microscale structural transition of the amorphous gels. This aging strategy can be applied in other supramolecular polymer systems particularly containing kinetically controlled structures and shows an opportunity to engineer the structure and porosity of amorphous porous soft materials for further applications.


CrystEngComm ◽  
2021 ◽  
Author(s):  
Xin Zhou ◽  
Yan Ren ◽  
Hongzhen Li ◽  
Xiaoqin Zhou ◽  
Shilong Hao ◽  
...  

The nano-/microstructured energetic materials (EMs) often display a unique combination of low-sensitivity and high-stability, but their structural control across multiple-length scales has proven difficult. Here, a polyvinyl pyrrolidone (PVP) polymer-directed...


Biomaterials ◽  
2014 ◽  
Vol 35 (21) ◽  
pp. 5472-5481 ◽  
Author(s):  
Elizabeth A. Zimmermann ◽  
Bernd Gludovatz ◽  
Eric Schaible ◽  
Björn Busse ◽  
Robert O. Ritchie

2016 ◽  
Vol 26 (16) ◽  
pp. 2609-2616 ◽  
Author(s):  
Pim van der Asdonk ◽  
Hans C. Hendrikse ◽  
Marcos Fernandez-Castano Romera ◽  
Dion Voerman ◽  
Britta E. I. Ramakers ◽  
...  

CIRP Annals ◽  
2012 ◽  
Vol 61 (1) ◽  
pp. 99-102 ◽  
Author(s):  
Rachid M'Saoubi ◽  
Tommy Larsson ◽  
José Outeiro ◽  
Yang Guo ◽  
Sergey Suslov ◽  
...  

Author(s):  
William F Sherman ◽  
Mira Asad ◽  
Anna Grosberg

Abstract Through a variety of mechanisms, a healthy heart is able to regulate its structure and dynamics across multiple length scales. Disruption of these mechanisms can have a cascad- ing effect, resulting in severe structural and/or functional changes that permeate across different length scales. Due to this hierarchical structure, there is interest in understand- ing how the components at the various scales coordinate and influence each other. However, much is unknown regarding how myofibril bundles are organized within a densely packed cell and the influence of the subcellular components on the architecture that is formed. To elucidate potential factors influencing cytoskeletal development, we proposed a compu- tational model that integrated interactions at both the cel- lular and subcelluar scale to predict the location of indi- vidual myofibril bundles that contributed to the formation of an energetically favorable cytoskeletal network. Our model was tested and validated using experimental metrics derived from analyzing single cell cardiomyocytes. We demonstrated that our model-generated networks were capable of repro- ducing the variation observed in experimental cells at different length scales as a result of the stochasticity inher- ent in the different interaction between the various cellu- lar components. Additionally, we showed that incorporat- ing length-scale parameters resulted in physical constraints that directed cytoskeletal architecture towards a structurally consistent motif. Understanding the mechanisms guiding the formation and organization of the cytoskeleton in individual cardiomyocytes can aid tissue engineers towards developing functional cardiac tissue.


RSC Advances ◽  
2016 ◽  
Vol 6 (99) ◽  
pp. 97399-97403 ◽  
Author(s):  
Rui Kuang ◽  
Luyi Zheng ◽  
Ethan Cottrill ◽  
Ning Pan ◽  
Yanhui Chi ◽  
...  

A hierarchical porous MOF nanocrystal, hpCuL (L = 2,4,6-tris(3,5-dicarboxylatephenylamino)-1,3,5-triazine) was prepared via a facile gel-aging process. This nanocomposite exhibits high catalytic activity and stability for the reduction of 4-nitrophenol.


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