bstract
Large-scale production of two-dimensional nanomaterials have being promising potential applications in various fields such as; electronic devices, transistors, energy storage devices and catalysis, drug delivery carrier, biosensor, bimolecular imaging, resulting from they have various unique electronic, optical, mechanical and chemical properties. In here, A simple, reliable and effective sonicated-liquid phase exfoliation method for direct exfoliation of hexagonal boron nitride (h-BN) and tungsten diselenide (WSe2) into few-layered nanosheets has been successfully developed by employing a low molecular weight adenine functionalized poly propylene glycol diacrylate supramolecular polymer (A-PPG) which formed with noncovalent assembly of hydrogen bond networks upon association of monomers. pH/temperature dual-responsive BN-APPG was fabricated for well controllable, rapid, effective drug delivery carrier. To exfoliate bulk layered materials with supramolecular polymers, adenine end-capped supramolecular polymer A-PPG was synthesized as exfoliation and stabilization agent using Michael addition reaction of adenine with PPG diacrylate. A-PPG self-assembled into either long-range ordered lamellar or micelle-like structures on the surface of ultrathin h-BN and WSe2 nanosheet because of the noncovalent interactions between A-PPG and nanosheets. Particularly, the number of exfoliated nanosheets exfoliation could be controlled by adjusting the amount of A-PPG incorporated and sonication time. Single layer BN nanosheets exhibited ordered hexagonal lattice microstructure whereas single layer WSe2 nanosheets is unique as it is chemically homogeneous, but exhibits both a semiconducting 2H crystal structure and metallic 1T phase corresponding to honey comb and ordered hexagonal microstructure respectively. A-PPG has the capacity to form two different lamellar morphology such as contracted and extended lamellar microstructures on the surface of coexisted metallic 1T-phase and semiconducting 2H-phase WSe2 nanosheets, respectively due to different physiochemical, electrical and optical properties of the two phase of WSe2 sheet. Dark brown (WSe2) and white (BN) THF/water dispersion solution were observed after sonication at room temperature and no obvious signs of precipitation for long time, implying the stability of dispersed nanosheets with the attachment of A-PPG which act as a strong stabilizing against aggregation and re-stacking of single/few-layer nanosheets, also indicating self-assembled of A-PPG used to manipulate the physical and morphological properties of exfoliated ultrathin nanosheets. These newly developed BN/A-PPG and WSe2/A-PPG nanocomposites exhibited excellent liquid–solid phase transition behavior and few-layer thickness with good dispersion, which means that they could store thermal energy (heat) while heating and release heat while freezing. Thermal stability and reliability behavior of A-PPG was improved with increasing the loading amount of BN or WSe2 nanosheets due to the optimum thermal stability of those nanosheets and self-assemble structure-forming capacity of A-PPG supramolecular polymer. A-PPG-functionalized BN nanosheets was nontoxic and biocompatibility against murine macrophage cell line, RAW 264.7 and human breast adenocarcinoma cell line,
MCF 7 Cell using the MTT assay indicated that the synthesized APPG–BN nanosheets were suitable for use as drug carriers up to high concentration. A-PPG displayed a well-defined phase transition behavior at its lower critical solution temperature (LCST), however, increasing the concentration of the composite, the LCST of the BN/A-PPG composite significantly reduced. Hence, the BN/A-PPG revealed temperature responsive behavior as function temperature change. In addition, the pH-responsible behavior of BN/A-PPG have been confirmed based on protonation/deprotonation behavior and particle size variation in different pH value. Overall, pH and temperature responsive behavior of multifunctional BN/A-PPG composite may be controlled by the tuning its composition, can be a novel multi-functional nanoscale material provide access to dual pH/temperature-responsive well control drug delivery system. Then, Doxorubicin (DOX) was used as a model anticancer drug to investigate the loading and temperature/pH-dependent triggered drug-releasing behavior of BN/A-PPG complexes. It was observed that the loading capacities of DOX on BN/A-PPG all increased as the function of DOX concentrations and reaches 36.17 % at DOX concentration. DOX loading mechanism over the hetrostructure of BN/A-PPG composite can be confirmed which is electrostatic interaction between positively charged adsorbent and negatively positive surface. In addition, strong specific π−π stacking between aromatic rings of DOX and aromatic BN nanosheets as well as hydrogen bonding between their functional groups possibly occurred. DOX releasing was investigated at different pH and temperature. Then, the controlled drug-release behavior of DOX@ BN/A-PPG complexes, which display an optimistic, rapid, well controllable and effective dox releasing capability. The newly developed method of producing exfoliated WSe2/BN provides a useful conceptual and potential framework for developing WSe2/BN-based multifunctional nanocomposites to extend their application for the next generation of transistors, energy storage devices and catalysis, drug delivery carrier, biosensor, bimolecular imaging, thermoconductive devices and solution-processed semiconductors devices. Particularly, the newly developed dual pH and temperature-responsive BN/A-PPG nanocarrier has highly promising potential for controlled release drug delivery systems.

Abstract
Large-scale production of two-dimensional nanomaterials have being promising potential applications in various fields such as; electronic devices, transistors, energy storage devices and catalysis, drug delivery carrier, biosensor, bimolecular imaging, resulting from they have various unique electronic, optical, mechanical and chemical properties. In here, A simple, reliable and effective sonicated-liquid phase exfoliation method for direct exfoliation of hexagonal boron nitride (h-BN) and tungsten diselenide (WSe2) into few-layered nanosheets has been successfully developed by employing a low molecular weight adenine functionalized poly propylene glycol diacrylate supramolecular polymer (A-PPG) which formed with noncovalent assembly of hydrogen bond networks upon association of monomers. pH/temperature dual-responsive BN-APPG was fabricated for well controllable, rapid, effective drug delivery carrier. To exfoliate bulk layered materials with supramolecular polymers, adenine end-capped supramolecular polymer A-PPG was synthesized as exfoliation and stabilization agent using Michael addition reaction of adenine with PPG diacrylate. A-PPG self-assembled into either long-range ordered lamellar or micelle-like structures on the surface of ultrathin h-BN and WSe2 nanosheet because of the noncovalent interactions between A-PPG and nanosheets. Particularly, the number of exfoliated nanosheets exfoliation could be controlled by adjusting the amount of A-PPG incorporated and sonication time. Single layer BN nanosheets exhibited ordered hexagonal lattice microstructure whereas single layer WSe2 nanosheets is unique as it is chemically homogeneous, but exhibits both a semiconducting 2H crystal structure and metallic 1T phase corresponding to honey comb and ordered hexagonal microstructure respectively. A-PPG has the capacity to form two different lamellar morphology such as contracted and extended lamellar microstructures on the surface of coexisted metallic 1T-phase and semiconducting 2H-phase WSe2 nanosheets, respectively due to different physiochemical, electrical and optical properties of the two phase of WSe2 sheet. Dark brown (WSe2) and white (BN) THF/water dispersion solution were observed after sonication at room temperature and no obvious signs of precipitation for long time, implying the stability of dispersed nanosheets with the attachment of A-PPG which act as a strong stabilizing against aggregation and re-stacking of single/few-layer nanosheets, also indicating self-assembled of A-PPG used to manipulate the physical and morphological properties of exfoliated ultrathin nanosheets. These newly developed BN/A-PPG and WSe2/A-PPG nanocomposites exhibited excellent liquid–solid phase transition behavior and few-layer thickness with good dispersion, which means that they could store thermal energy (heat) while heating and release heat while freezing. Thermal stability and reliability behavior of A-PPG was improved with increasing the loading amount of BN or WSe2 nanosheets due to the optimum thermal stability of those nanosheets and self-assemble structure-forming capacity of A-PPG supramolecular polymer. A-PPG-functionalized BN nanosheets was nontoxic and biocompatibility against murine macrophage cell line, RAW 264.7 and human breast adenocarcinoma cell line,
MCF 7 Cell using the MTT assay indicated that the synthesized APPG–BN nanosheets were suitable for use as drug carriers up to high concentration. A-PPG displayed a well-defined phase transition behavior at its lower critical solution temperature (LCST), however, increasing the concentration of the composite, the LCST of the BN/A-PPG composite significantly reduced. Hence, the BN/A-PPG revealed temperature responsive behavior as function temperature change. In addition, the pH-responsible behavior of BN/A-PPG have been confirmed based on protonation/deprotonation behavior and particle size variation in different pH value. Overall, pH and temperature responsive behavior of multifunctional BN/A-PPG composite may be controlled by the tuning its composition, can be a novel multi-functional nanoscale material provide access to dual pH/temperature-responsive well control drug delivery system. Then, Doxorubicin (DOX) was used as a model anticancer drug to investigate the loading and temperature/pH-dependent triggered drug-releasing behavior of BN/A-PPG complexes. It was observed that the loading capacities of DOX on BN/A-PPG all increased as the function of DOX concentrations and reaches 36.17 % at DOX concentration. DOX loading mechanism over the hetrostructure of BN/A-PPG composite can be confirmed which is electrostatic interaction between positively charged adsorbent and negatively positive surface. In addition, strong specific π−π stacking between aromatic rings of DOX and aromatic BN nanosheets as well as hydrogen bonding between their functional groups possibly occurred. DOX releasing was investigated at different pH and temperature. Then, the controlled drug-release behavior of DOX@ BN/A-PPG complexes, which display an optimistic, rapid, well controllable and effective dox releasing capability. The newly developed method of producing exfoliated WSe2/BN provides a useful conceptual and potential framework for developing WSe2/BN-based multifunctional nanocomposites to extend their application for the next generation of transistors, energy storage devices and catalysis, drug delivery carrier, biosensor, bimolecular imaging, thermoconductive devices and solution-processed semiconductors devices. Particularly, the newly developed dual pH and temperature-responsive BN/A-PPG nanocarrier has highly promising potential for controlled release drug delivery systems.

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