Elsevier

Diamond and Related Materials

Volume 69, October 2016, Pages 166-176
Diamond and Related Materials

Study on the reinforcing effect of nanodiamond particles on the mechanical, thermal and antibacterial properties of cellulose acetate membranes

https://doi.org/10.1016/j.diamond.2016.08.014Get rights and content

Highlights

  • Cellulose acetate (CA)/nanodiamond (NDs) nanocomposite membrane was fabricated.

  • The reinforcement effect of NDs was theoretically and experimentally investigated.

  • A strong interfacial adhesion between CA and neat as well as functionalized NDs was achieved.

  • Fabricated nanocomposite membranes exhibited good thermal and antibacterial properties.

Abstract

The aim of this study was to determine the impact of detonation nanodiamond (DND) on the mechanical, thermal and antibacterial properties of cellulose acetate (CA) membrane. In order to achieve an efficient dispersion of DNDs in the polymeric matrix, they were functionalized via heat treatment. Different amounts of raw and functionalized DND; 0 to 0.75 wt.%, were added to the CA and various structural and characterization analyses such as scanning electron microscopy (SEM), transmission electron microscopy (TEM), thermal gravimetric analysis (TGA) and Fourier transform infrared (FTIR) were also carried out. Mechanical strength analysis revealed that both raw and carboxylated DND have great influence on the mechanical behavior of CA membrane particularly at 0.5 wt.% of nanoparticles (NPs) content. Application of Pukanszky's model for tensile strength and micromechanical models for tensile modulus revealed that strong interfacial interaction and thick interphase region are formed around the NPs. In addition, the TGA results showed that the incorporation of 0.5 wt.% of the DND and DND-COOH improved the thermal stability of the CA membrane. The antibacterial tests confirmed that the nanocomposite membranes containing DND-COOH displayed greater antibacterial enhancement against Escherichia coli (E. coli) and Staphylococcus aureus (S. aureus).

Introduction

Membrane separation technology is one of the most efficient methods in separation science and processes due to its low energy consumption, easy scale-up, less or no use of chemicals, and absence of any harmful by-product formation [1]. Polymeric membranes have many advantages such as straightforward pore forming mechanism, higher flexibility, smaller footprints required for installation and considerably low costs with respect to inorganic membranes or metal frameworks, which make them more convenient for a wide range of applications in large scales especially in water reclamation and wastewater treatment processes [2]. Cellulose acetate (CA) is one of the foremost among polymer membranes which has been widely used in separation processes and has been nominated as one of the most applicable polymers in preparation of membranes, due to its high hydrophilicity, high biocompatibility, non-toxic nature, good desalting, high potential flux and relatively low cost [1], [3], [4]. However, narrow temperature range (maximum 30 °C), high biofouling and microbial degradation tendency, poor mechanical and chemical stability in both acidic and basic solutions are considered as its main disadvantages, which demands for efficient modification [4].

Due to the rapid growth of nanotechnology, fabrication of nanocomposite membranes has shown great impact and efficient performance in the past decades. In this regard, the role of various nanoparticles (NPs) on the engineering features of polymeric nanocomposite membranes has been extensively examined, in many cases significant improvement in mechanical, thermal and antifouling properties has been explored. However, the effective and uniform dispersion of NPs is still a challenging subject for researchers which is greatly influenced by the intraparticle interactions. It is well known that the uniform dispersion of NPs throughout the polymeric matrix and strong interfacial bonding between the NPs and the matrix are major factors that improved the mechanical and thermal properties of membranes [4], [5], [6], [7], [8], [9].

Several researches have been particularly carried out on the impact of NPs on the modification of CA based membranes [4], [6], [10], [11], [12], [13], [14], [15]. According to these studies, at high concentration of nanoparticles e.g. silver (AgNO3), polyhedral oligomeric silsesquioxane (POSS), and organically modified montmorillonite (OMMt), the mechanical and thermal properties of CA membrane decreased due to the agglomeration of NPs as well as the weak interaction between polymer and NPs. Also, the interfacial interaction between NPs and CA matrix played a crucial role in improvement of matrix properties [6], [13], [14].

Carbon-based nanomaterials are potentially useful due to their unique physical and chemical properties. Among them, detonation nanodiamond (DND) particles with a diamond core (sp3 carbon-carbon bond) that is covered with multiple functional groups including carboxylic acids, hydroxyl, ketones, ethers, and lactones, are favored for many direct applications or post modification [16], [17]. Due to the interesting characteristics of DND such as hydrophilicity [16], [18], [19], antibacterial activity [20], [21], biocompatibility [22], [23], [24], [25], [26], chemical stability [22], thermal stability [23] non-toxicity [22], [23], [27], superior hardness and mechanical properties, resistance to harsh environments [22], [28] and ease of surface functionalization [23], [29], it is predicted that it can be potentially used as reinforcement filler in fabrication of nanocomposite materials. The non-diamond carbon from DND surface can be easily removed via thermal or acid treatments and some desirable functional groups, such as carboxyl groups can be easily formed, which could be beneficial to dispersion capability of DND, especially in polar media [23], [30], [31].

To the best of our knowledge, literature does not report any document regarding the application of DNDs in fabrication of polymeric nanocomposite membranes. Excellent mechanical and thermal properties, very high specific surface area and the presence of hydrophilic functional groups on the DND surface make it an interesting and good choice to be used as reinforcement agent in CA matrix to overcome the inherent disadvantages of CA membrane. DNDs have recently emerged as an important focus in the development of antibacterial and antibiofilm forming agents [32]. Some materials with antibacterial activity such as silver more recently concern about the cytotoxic effects, aggregation and loss of antibacterial activity [33]. In this case, DND can be used as a new effective agent against bacteria and prevent the biodegradability of CA membrane.

In order to improve the mechanical, thermal and antibacterial properties of CA membrane, in this work, DND embedded CA nanocomposite membranes with various amounts of the DND contents NPs were fabricated via phase inversion method. Since the mechanical and thermal properties of the nanocomposite membranes depend on interaction between the polymer matrix and the NPs as well as on uniform dispersion NPs in polymer matrix, raw DNDs were functionalized via thermal treatment to create carboxyl groups on the surface of the DND. Fabricated membranes were analyzed by applying experimental methods such as mechanical tests, scanning electron microscopy (SEM), transmission electron microscopy (TEM), thermal gravimetric analysis (TGA) and Fourier transform infrared (FTIR) spectroscopy. Two and three phase theoretical models were also utilized to investigate the impact of DND on embedded CA membranes.

Section snippets

Materials

Cellulose acetate (Mn = 30,000), was used as polymer material to prepare the CA membrane, supplied by Sigma-Aldrich (Germany). The DNDs procured from Nabond Technology Co., Ltd., China, having phase purity higher than 98% and average diameter of 5 nm, providing a specific surface area of about 300 m2 g 1. N-N-dimethylformamide (DMF, 99.8%, Merck) and deionized (DI) water were used as solvent and non-solvent, respectively.

Surface functionalization of DND via thermal oxidation

Due to the fact that the oxidation of carbon-based materials removes organic

FTIR analysis of DND treatment and membranes

The surface chemistry of the raw and thermally treated nanodiamonds; DND and DND-COOH, respectively, was determined by FTIR spectra. As shown in Fig. 1, in case of DNDs, the absorption peaks at 2922 and 2860 cm 1 correspond to the asymmetric and symmetric stretching vibration of Csingle bondH band, respectively. Also, the absorption bands at 1341 cm 1 can be attributed to the deformation vibration of Csingle bondH band in alkyl group [41]. The absorption peak at 3423 cm 1 corresponds to the stretching vibration of Osingle bondH,

Conclusions

In this study, the effect of detonation detnanodiamond (DND) and heat treated DND (DND-COOH) on the mechanical, thermal and antibacterial properties of CA membrane was studied. Phase inversion process with DMF as solvent was used to prepare flat sheet membranes. The presence of small amount of DND and DND-COOH particles in the membrane can significantly improve the mechanical, thermal and antibacterial properties of the membrane. The main conclusions are listed as follows:

  • (1)

    SEM images of the

Acknowledgement

The authors gratefully acknowledge the financial support from Sahand University of Technology with grant number of 30/15975.

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      Citation Excerpt :

      The functionalization of ND surfaces could lead to the excellent dispersion of ND in their matrixes, thus produced a positive effect on thermal properties of substrate [180,182]. Compared with aforementioned works [181], Etemadi et al. [182] highlighted that the ND-COOH with good dispersion obviously improved thermal stability of the cellulose acetate membrane. Beyond that, the PDA modified ND (ND-PDA) provided the significant impacts in enhancing thermal properties of the PVA composites [180].

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