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The algae-derived bio-binder (ADBB) from hydrothermal liquefaction has been reported to be an effective and sustainable new alternative to petroleum-based curing agents for epoxy resin. However, there is still room for the epoxy/ADBB system to attain the comprehensive mechanical performance of conventional epoxy-based nanocomposites, typically reinforced with surface-functionalized nanofillers (e.g., glass nanoparticles (GNPs)) by petroleum-based silane coupling agents. Herein, we explored the use of ADBB as an innovative surface-modifying agent to functionalize GNPs and evaluated the potential of ADBB surface-functionalized GNPs (ADBB-GNPs) as a reinforcing agent in the epoxy/ADBB matrix nanocomposite by comparing them to pristine GNPs and (3-aminopropyl) triethoxysilane (APTES) (a popular silane coupling agent) surface-modified GNPs (APTES-GNPs). The surface functionalization of GNPs with ADBB was carried out and characterized by scanning electron microscopy (SEM), dynamic light scattering (DLS), and Fourier-transform infrared spectroscopy (FTIR). Material performance including tensile, flexural, and Izod impact properties and thermal properties of the resulting epoxy/ADBB nanocomposites were investigated by corresponding ASTM mechanical test standards and thermogravimetric analysis (TGA). Our results revealed that the ADBB is a sustainable and effective surface-modifying agent that can functionalize GNPs. The obtained ADBB-GNPs significantly improved the mechanical performance of the epoxy/ADBB system at ultra-low loading (0.5 wt.%) by up to 42% and the maximum decomposition rate temperature increased from 419 °C to 422 °C, both of which outperformed APTES-GNPs. This research sheds light on developing sustainable surface-modifying agents for nanofillers to create high-performance sustainable polymer composite materials. 

We report a transformative epoxy system with a microalgae-derived bio-binder from hydrothermal liquefaction processing (HTL). The obtained bio-binder not only served as a curing agent for conventional epoxy resin (e.g., EPON 862), but also acted as a modifying agent to enhance the thermal and mechanical properties of the conventional epoxy resin. This game-changing epoxy/bio-binder system outperformed the conventional epoxy/hardener system in thermal stability and mechanical properties. Compared to the commercial EPON 862/EPIKURE W epoxy product, our epoxy/bio-binder system (35 wt.% bio-binder addition with respect to the epoxy) increased the temperature of 60% weight loss from 394 °C to 428 °C and the temperature of maximum decomposition rate from 382 °C to 413 °C, while the tensile, flexural, and impact performance of the cured epoxy improved in all cases by up to 64%. Our research could significantly impact the USD 38.2 billion global market of the epoxy-related industry by not only providing better thermal and mechanical performance of epoxy-based composite materials, but also simultaneously reducing the carbon footprint from the epoxy industry and relieving waste epoxy pollution. 

Algae is a promising sustainable feedstock for the generation of bio-crude oil, which is a sustainable alternative to fossil fuels, through the thermochemical process of hydrothermal liquefaction (HTL). However, this process also generates carbon particles (algae-derived carbon, ADC) as a significant byproduct. Herein, we report a brand-new and value-added use of ADC particles as a reinforcing agent for epoxy matrix composites (EMCs). ADC particles were synthesized through HTL processing of Chlorella vulgaris (a green microalgae) and characterized for morphology, average size, specific surface area, porosity, and functional groups. The ADC particles were subsequently integrated into a representative epoxy resin (EPON 862) as a reinforcing filler at loading levels of 0.25%, 0.5%, 1%, and 2% by weight. The tensile, flexural, and Izod impact properties, as well as the thermal stability, of the resulting EMCs were evaluated. It is revealed that the ADC particles are a sustainable and effective reinforcing agent for EMCs at ultra-low loading. Specifically, the ADC-reinforced EMC with 1 wt.% ADC showed improvements of ~24%, ~30%, ~31%, and ~57% in tensile strength, Young’s modulus, elongation at break, and work of fracture (WOF), respectively, and improvements of ~10%, ~37%, ~24%, and ~39% in flexural strength, flexural modulus, flexural elongation at break, and flexural WOF, respectively, as well as an improvement of ~54% in Izod impact strength, compared to those corresponding properties of neat epoxy. In the meantime, the thermal decomposition temperatures at 60% and 80% weight loss of the abovementioned ADC-reinforced EMC increased from 410 °C to 415 °C and from 448 °C to 515 °C in comparison with those of neat epoxy. This study highlighted the potential of sustainable ADC particles as a reinforcing agent in the field of polymer matrix composite materials, which represented a novel and sustainable approach that would mitigate greenhouse gas remission and reduce reliance on nonrenewable reinforcing fillers in the polymer composite industry. 

Epoxy is the most prevalent thermosetting resin in the field of polymer composite materials. There has been a growing interest in the development of bio-based epoxy resins as a sustainable alternative to conventional petrochemical epoxy resins. Advances in this field in recent years have included the use of various renewable resources, such as vegetable oils, lignin, and sugars, as direct precursors to produce bio-based epoxy resins. In the meantime, bio-oils have been produced via the decomposition of biomass through thermochemical conversion and mainly being used as renewable liquid fuels. It is noteworthy that bio-oils can be used as a sustainable resource to produce epoxy resins. This review addresses research progress in producing bio-oil-based epoxy resins from thermochemical processing techniques including organic solvent liquefaction, fast pyrolysis, and hydrothermal liquefaction. The production of bio-oil from thermochemical processing and its use to inject sustainability into epoxy resins are discussed. Herein, we intend to provide an overall picture of current attempts in the research area of bio-oil-based epoxy resins, reveal their potential for sustainable epoxy resins, and stimulate research interests in green/renewable materials.