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PUBLISHED ; We report on the modification of graphene oxide (GO) with polyvinylalcohol (PVA) leading to the mechanical improvement of GO based materials. First, GO was covalently functionalised with PVA by esterification of carboxylic groups on GO with hydroxyl groups of PVA resulting in functionalised f-(PVA)GO. This was carried out for PVA of six different molecular weights. This functionalised graphene oxide could be formed into a paper-like material by vacuum filtration. Papers prepared from f-(PVA)GO showed significant increases in mechanical properties compared to those prepared with GO or with simple mixtures of GO and PVA. The best performance was achieved for PVA functional groups with molecular weights between 50 and 150 kg/mol. Improvements in Young?s moduli of 60% and tensile strength of 400% were observed relative to GO-only paper. The improved mechanical properties are attributed to enhanced inter-flake stress transfer due to the covalently bonded PVA. Second, functionalised f-(PVA)GO was used as filler in PVA-based composites. The application of a pre-selection method allowed the use of only the largest functionalised f-(PVA)GO flakes. This resulted in substantially reinforced PVA-f-(PVA)GO composites. Both modulus and strength increased by 40% relative to the pure polymer for f-(PVA)GO loadings below 0.3 vol.%. ; The authors would like to acknowledge Science Foundation Ireland, (grant number 07/IN.7/I1772), Spanish Ministry of Science and Innovation (MICINN) under project MAT2010-15026, Spanish Research Council CSIC under project 201080E124 and the Government of Aragon (DGA) under Project DGA-T66 CNN. M.C. thanks MICINN for her PhD contract and funding for research stay at TCD under FPI Programme BES-2008-003503.

We report on the modification of graphene oxide (GO) with poly(vinyl alcohol) (PVA) leading to the mechanical improvement of GO based materials. First, GO was covalently functionalised with PVA by esterification of carboxylic groups on GO with hydroxyl groups of PVA resulting in functionalised f-(PVA)GO. This was carried out for PVA of six different molecular weights. This functionalised graphene oxide could be formed into a paper-like material by vacuum filtration. Papers prepared from f-(PVA)GO showed significant increases in mechanical properties compared to those prepared with GO or with simple mixtures of GO and PVA. The best performance was achieved for PVA functional groups with molecular weights between 50 and 150 kg/mol. Improvements in Young's moduli of 60% and tensile strength of 400% were observed relative to GO-only paper. The improved mechanical properties are attributed to enhanced inter-flake stress transfer due to the covalently bonded PVA. Second, functionalised f-(PVA)GO was used as filler in * Corresponding author. Tel/Fax: +34 976 73-3977 / -3318. E-mail address: wmaser@icb.csic.es (W.K. Maser) 2 PVA-based composites. The application of a pre-selection method allowed the use of only the largest functionalised f-(PVA)GO flakes. This resulted in substantially reinforced PVA-f-(PVA)GO composites. Both modulus and strength increased by 40% relative to the pure polymer for f- (PVA)GO loadings below 0.3 vol.%. ; The authors would like to acknowledge Science Foundation Ireland, (grant number 07/IN.7/I1772), Spanish Ministry of Science and Innovation (MICINN) under project MAT2010-15026, Spanish Research Council CSIC under project 201080E124 and the Government of Aragon (DGA) under Project DGA-T66 CNN. M.C. thanks MICINN for her PhD contract and funding for research stay at TCD under FPI Programme BES-2008-003503. ; Peer reviewed