A Study on Electron Acceptor of Carbonaceous Materials for Highly Efficient Hydrogen Uptakes

Significant efforts have been directed toward the identification of carbonaceous materials that can be utilized for hydrogen uptake in order to develop on-board automotive systems with a gravimetric capacity of 5.5 wt.%, thus meeting the U.S. Department of Energy technical targets. However, the capacity of hydrogen storage is limited by the weak interaction between hydrogen molecules and the carbon surface. Cigarette butts, which are the most abundant form of primary plastic waste, remain an intractable environmental pollution problem. To transform this source of waste into a valuable adsorbent for hydrogen uptake, we prepared several forms of oxygen-rich cigarette butt-derived porous carbon (CGB-AC, with the activation temperature range of 600 and 900 °C). Our experimental investigation revealed that the specific surface area increased from 600 to 700 °C and then decreased as the temperature rose to 900 °C. In contrast, the oxygen contents gradually decreased with increasing activation temperature. CGB-AC700 had the highest H2 excess uptake () of 8.54 wt.% at 77 K and 20 bar, which was much higher than that of porous carbon reported in the previous studies. We found that the dynamic interaction between the porosity and the oxygen content determined the hydrogen storage capacity. The underlying mechanisms proposed in the present study would be useful in the design of efficient hydrogen storage because they explain the interaction between positive carbonaceous materials and negative hydrogen molecules in quadrupole orbitals.

Process Water Recirculation During Hydrothermal Carbonization as a Promising Process Step Towards the Production of Nitrogen-Doped Carbonaceous Materials

Hydrothermal Carbonization (HTC) refers to the conversion of biogenic wastes into char-like solids with promising perspectives for application, but a process water (PW) results which is difficult to dispose untreated. Thus, a biorefinery approach including one or two recirculation steps with the additional objective of improving the physico-chemical characteristics of the solid was performed in this study. During HTC, constitutive molecules such as saccharides, proteins and lignin of Brewer’s Spent Grains decompose into hundreds of organic compounds, following complex reactions. To get deeper insights a combination of proximate, ultimate and structural analysis for solid products as well as liquid chromatography for liquid products were the choice. The main reactions could be identified by key compounds of low and high molecular weight resulting from hydrolysis, dehydration, decarboxylation, deamination as well as amide formation and condensation reactions. Their intensity was influenced by the feedwater pH and reaction temperature. Via reactions of Maillard character up to around 90% of the dissolved nitrogen of the recirculated process water at 200, 220 and 240 °C result in the formation of nitrogen containing heterocycles or rather Quartnernary nitrogen incorporated into the hydrochar (HC). Thus, already one recirculation step during HTC at 240 °C promises the fabrication of high added-value materials, i.e. nitrogen doped carbonaceous materials. Graphic Abstract