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1.
Nanoscale ; 13(4): 2720-2727, 2021 Feb 04.
Article in English | MEDLINE | ID: mdl-33498078

ABSTRACT

Graphene Oxides (GOs) have been frequently employed as fillers in polymer-based applications. While GO is known to nucleate polymer crystallization in GO-polymer composites reinforcing the mechanical properties of semicrystalline polymers, its counter effect on how polymer crystallization can alter the microstructure of GO has rarely been systematically studied yet. In this work, we study the GO nematic liquid crystal (LC) phase during polymer crystallization focusing on their hierarchical structures by employing in situ small/wide-angle X-ray scattering/diffraction (SAXS/WAXD) techniques. We found that GO LC and polymer crystals co-exist in the GO/polymer complex, where the overall liquid crystallinity is influenced by polymer crystallization. While polymer crystallizes in bulk or at the interface depending on the cooling rate, the interfacial crystallization of poly(ethylene glycol) (PEG) on GO improves both GO alignment and orientation of PEG crystal. This work provides an opportunity to develop a hierarchical structure of GO-based crystalline polymer nanocomposites, whose directionality can be controlled by polymer crystallization under proper cooling rates.

2.
Nat Commun ; 11(1): 5032, 2020 Oct 06.
Article in English | MEDLINE | ID: mdl-33024113

ABSTRACT

Unzipping of the basal plane offers a valuable pathway to uniquely control the material chemistry of 2D structures. Nonetheless, reliable unzipping has been reported only for graphene and phosphorene thus far. The single elemental nature of those materials allows a straightforward understanding of the chemical reaction and property modulation involved with such geometric transformations. Here we report spontaneous linear ordered unzipping of bi-elemental 2D MX2 transition metal chalcogenides as a general route to synthesize 1D nanoribbon structures. The strained metallic phase (1T') of MX2 undergoes highly specific longitudinal unzipping owing to the self-linearized oxygenation at chalcogenides. Stable dispersions of 1T' MoS2 nanoribbons with widths of 10-120 nm and lengths up to ~4 µm are produced in water. Edge abundant 1T' MoS2 nanoribbons reveal the hidden potential of idealized electrocatalysis for hydrogen evolution reactions at a competitive level with the precious Pt catalyst.

3.
Nat Commun ; 11(1): 5532, 2020 Oct 27.
Article in English | MEDLINE | ID: mdl-33110099

ABSTRACT

An amendment to this paper has been published and can be accessed via a link at the top of the paper.

4.
ACS Cent Sci ; 6(7): 1105-1114, 2020 Jul 22.
Article in English | MEDLINE | ID: mdl-32724845

ABSTRACT

Graphene fibers (GFs) are promising elements for flexible conductors and energy storage devices, while translating the extraordinary properties of individual graphene sheets into the macroscopically assembled 1D structures. We report that a small amount of water addition to the graphene oxide (GO) N-methyl-2-pyrrolidone (NMP) dispersion has significant influences on the mesophase structures and physical properties of wet-spun GFs. Notably, 2 wt % of water successfully hydrates GO flakes in NMP dope to form a stable graphene oxide liquid crystal (GOLC) phase. Furthermore, 4 wt % of water addition causes spontaneous planarization of wet-spun GFs. Motivated from these interesting findings, we develop highly electroconductive and mechanically strong flat GFs by introducing highly crystalline electrochemically exfoliated graphene (EG) in the wet-spinning of NMP-based GOLC fibers. The resultant high-performance hybrid GFs can be sewn on cloth, taking advantage of the mechanical robustness and high flexibility.

5.
Adv Mater ; : e1803267, 2018 Aug 08.
Article in English | MEDLINE | ID: mdl-30088842

ABSTRACT

Inspired by mussel adhesive polydopamine (PDA), effective reinforcement of graphene-based liquid crystalline fibers to attain high mechanical and electrical properties simultaneously is presented. The two-step defect engineering, relying on bioinspired surface polymerization and subsequent solution infiltration of PDA, addresses the intrinsic limitation of graphene fibers arising from the folding and wrinkling of graphene layers during the fiber-spinning process. For a clear understanding of the mechanism of PDA-induced defect engineering, interfacial adhesion between graphene oxide sheets is straightforwardly analyzed by the atomic force microscopy pull-off test. Subsequently, PDA could be converted into an N-doped graphitic layer within the fiber structure by a mild thermal treatment such that mechanically strong fibers could be obtained without sacrificing electrical conductivity. Bioinspired graphene-based fiber holds great promise for a wide range of applications, including flexible electronics, multifunctional textiles, and wearable sensors.

6.
ACS Nano ; 11(9): 9424-9434, 2017 09 26.
Article in English | MEDLINE | ID: mdl-28783312

ABSTRACT

We report graphene@polymer core-shell fibers (G@PFs) composed of N and Cu codoped porous graphene fiber cores uniformly coated with semiconducting polymer shell layers with superb electrochemical characteristics. Aqueous/organic interface-confined polymerization method produced robust highly crystalline uniform semiconducting polymer shells with high electrical conductivity and redox activity. When the resultant core-shell fibers are utilized for fiber supercapacitor application, high areal/volume capacitance and energy densities are attained along with long-term cycle stability. Desirable combination of mechanical flexibility, electrochemical properties, and facile process scalability makes our G@PFs particularly promising for portable and wearable electronics.

7.
ACS Appl Mater Interfaces ; 9(1): 1021-1028, 2017 Jan 11.
Article in English | MEDLINE | ID: mdl-27966907

ABSTRACT

Cost effective scalable method for uniform film formation is highly demanded for the emerging applications of 2D transition metal dichalcogenides (TMDs). We demonstrate a reliable and fast interfacial self-assembly of TMD thin films and their heterostructures. Large-area 2D TMD monolayer films are assembled at air-water interface in a few minutes by simple addition of ethyl acetate (EA) onto dilute aqueous dispersions of TMDs. Assembled TMD films can be directly transferred onto arbitrary nonplanar and flexible substrates. Precise thickness controllability of TMD thin films, which is essential for thickness-dependent applications, can be readily obtained by the number of film stacking. Most importantly, complex structures such as laterally assembled 2D heterostructures of TMDs can be assembled from mixture solution dispersions of two or more different TMDs. This unusually fast interfacial self-assembly could open up a novel applications of 2D TMD materials with precise tunability of layer number and film structures.

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