Natural rubber (NR) has restricted its application due to its potential for thermal- and oil-resistant materials. The weakness of NR can be eliminated by chemical modification to enhance aging properties. Formic acid and hydrogen peroxide have been used to prepare partially epoxidized natural rubber (ENR) in the latex state. Its residual unsaturated units were then modified using hydrazine and hydrogen peroxide to obtain hydrogenated ENR (HENR). 1H-NMR characterized the resulting products. NR and modified NRs were compounded and then vulcanized using a conventional milling process. This paper compares NR, ENR having 49.5% epoxide group content, and HENR having 49.5% epoxide group content and 24% hydrogenation degree in terms of tensile, thermal, oil, and ozone properties. Morphology and lifetime prediction were studied. Overall results show that the tensile strength of the HENR composite (14.7 MPa) was 79 and 71% lower than that of ENR (18.6 MPa) and NR (20.8 MPa) composites, respectively. In contrast, the modulus at 100% elongation of the HENR composite (2.0 MPa) was 167 and 200% higher than that of ENR (1.2 MPa) and NR (1.0 MPa) composites, respectively. Morphological studies of the tensile fractured surface of the vulcanizates, using scanning electron microscopy, confirmed a shift from ductility failure to brittle with the presence of the epoxide groups and low unsaturated bonds in the backbone chain. The results demonstrated that HENR could act as an ideal material, providing better thermal, oil, and ozone resistances while maintaining the mechanical properties of the rubber. The kinetic analyses of the thermal degradation of NR, ENR, and HENR were studied using thermogravimetric analysis (TGA) at three heating rates. Kissinger–Akahira–Sunose (KAS) was employed to calculate the activation energy (E a). The obtained data were used to predict the lifetime under the established temperature range and 0.05 conversion level. Overall, the results represented that HENR had a longer lifetime than NR and ENR for a temperature range between 25 and 200 °C, indicating that HENR had excellent thermal stability than NR and ENR. Therefore, the HENR should extend the applications to include gaskets and seals, especially for the automotive and oil industries.

Epoxidized natural rubber (ENR) with 50% mol of epoxide groups was synthesized using performic acid generated from the reaction of formic acid/hydrogen peroxide in latex form followed by hydrogenation using diimide generated from hydrazine (N 2 H 4 ) and hydrogen peroxide (H 2 O 2 ) with boric acid (H 3 BO 3 ) as a catalyst. The resulting products (hydrogenated epoxidized natural rubber, HENR) were characterized by proton nuclear magnetic resonance spectroscopy ( 1 H-NMR), gel testing, transmission electron microscopy (TEM), differential scanning calorimetry (DSC), and thermogravimetric analysis (TGA). The effects of reaction parameters such as N 2 H 4 amount, H 2 O 2 amount, H 3 BO 3 amount, gelatin amount, reaction time, and reaction temperature on the percentage of hydrogenation degree and gel content were investigated. The transmission electron micrographs of the particles confirmed a core/shell structure consisting of a highly unsaturated concentration region as the core encapsulated by a low carbon–carbon double bond concentration region as the shell, which indicated that the rubber particle seemed to be modified from the outer layer to the center of the rubber particle. Overall, the data showed that an increase in the amount of the individual chemicals, reaction time, and temperature increased the hydrogenation degree. However, a higher level of gelatin retarded an increase in the percentage of hydrogenation degree. As the hydrogenation degree increased, the gel content increased due to the ether linkage and the crosslinking reaction triggered through hydroxyl radicals. From DSC measurements, the glass transition temperatures of hydrogenated products increased above those of original rubbers. The thermal stability of hydrogenated products was improved, demonstrated by a decomposition temperature shift to a higher temperature than ENR, as shown by the results from the thermogravimetric analysis. Therefore, the hydrogenated ENR (HENR) exhibited good thermal stability, which could extend the applications of ENR in the automotive and oil industries.