To expand the applications of graphene-based materials to biogas purification, a series of reduced graphene oxide aerogels (rGOAs) were prepared from industrial grade graphene oxide using a simple hydrothermal method. The influences of the hydrothermal preparation temperature on the textural properties, hydrophobicity and physisorption behavior of the rGOAs were investigated using a range of physical and spectroscopic techniques. The results showed that the rGOAs had a macro-porous three-dimensional network structure. Raising the hydrothermal treatment temperature reduced the number of oxygen-containing groups, whereas the specific surface area (SBET), micropore volume (Vmicro) and water contact angle values of the rGOAs all increased. The dynamic adsorption properties of the rGOAs towards hexamethyldisiloxane (L2) increased with increasing hydrothermal treatment temperature and the breakthrough adsorption capacity showed a significant linear association with SBET, Vmicro and contact angle. There was a significant negative association between the breakthrough time and inlet concentration of L2, and the relationship could be reliably predicted with a simple empirical formula. L2 adsorption also increased with decreasing bed temperature. Saturated rGOAs were readily regenerated by a brief heat-treatment at 100 °C. This study has demonstrated the potential of novel rGOA for applications using adsorbents to remove siloxanes from biogas.
The utilisation of activated porous carbon (APC) for the removal of volatile methyl siloxane (VMS) has attracted significant research attention. However, the development of materials with high adsorption capacity remains a challenge. In this study, we successfully developed a high-specific-surface-area (2551 m2 g−1) APC material with a large porous texture (1.30 cm3 g−1) using coconut shell waste and NaOH as the activating agent. The performance of the APC material in the removal of hexamethyldisiloxane (L2) was evaluated using a fixed-bed dynamic adsorption setup. Notably, at 0 °C, the APC demonstrated a remarkable L2 removal ability, achieving a breakthrough adsorption capacity of 898.6 mg g−1. By increasing the inlet concentration of L2 and decreasing the temperature appropriately, the L2 adsorption capacity could be further improved. One advantage of APCs is their simple recycling process, which allows for sustained adsorption performance even after five consecutive cycles of adsorption and desorption. Therefore, the prepared APC material holds great promise as an efficient adsorbent for the removal of VMS.
Volatile methyl siloxanes (VMSs) as a trace impurity in biogas decreases its energy utilization, and thus need to be removed. In this paper, a one-step hydrothermal reduction was performed to produce three-dimensional reduced graphene oxide aerogels (rGOAs) using industrial-grade graphene oxide (IGGO) as raw material and vitamin C (VC) as a reductant to facilitate the fabrication of rGOAs. The synthesis of rGOAs was a simple, green, and energy-efficient process. The developed rGOAs were characterized using the Brunauer–Emmett–Teller method, Raman spectrometry, scanning electron microscopy, Fourier-transform infrared spectroscopy, X-ray diffraction measurements and contact angle. The results obtained showed that rGOA-1 with a VC/IGGO ratio of 1/1 (m/m) exhibited a hierarchical porous structure and super-hydrophobicity, yielding a high specific surface area (137.9 m2 g−1) and superior water contact angle (143.8°). The breakthrough adsorption capacity of rGOA-1 for hexamethyldisiloxane (L2, a VMS model) was 11 times higher than that of IGGO. Low inlet concentration and bed temperature were considered beneficial for the L2 adsorption. Interestingly, rGOA-1 was less sensitive to water, and it was readily regenerated for reuse by annealing at 80 °C. The rGOAs have been demonstrated to have great potential for the removal of siloxanes from biogas.
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