C - Journal of Carbon Research

Halomethanes (CH₃X, where X = F, Cl, Br) are potent atmospheric pollutants, and their removal via adsorption on activated carbons (ACs) is a critical remediation strategy. However, the molecular-level influence of AC surface chemistry on adsorption, especially under realistic environmental conditions, is not fully understood. This work utilizes Grand Canonical Monte Carlo (GCMC) simulations to investigate the adsorption of CH₃F, CH₃Cl, and CH₃Br on realistic carbon models, comparing unfunctionalized graphitic surfaces (AC0) with surfaces functionalized with alcohol (AC1), carbonyl (AC2), and carboxyl (AC3) groups. We analyze the process for both pure components and in realistic mixtures (Quarantine and Pre-Shipment concentrations). Our findings reveal a critical inversion in adsorption preference. For pure components, CH₃Br adsorption is highest on the unfunctionalized (AC0) surface, driven by strong adsorbate–adsorbate interactions leading to condensation, characterized by a rising isosteric heat of adsorption ( kJ/mol) that matches the enthalpy of sublimation. Conversely, in realistic humid mixtures, the pristine surface suffers a capacity collapse (>90% loss). The functionalized surfaces (especially AC3) demonstrate superior performance, exhibiting a thermodynamic selectivity of $S_{C{H}_{3}Br/Air}>100$ (compared to $S\approx 15$ for AC0) and retaining approximately 60% of their dry-condition affinity. This study elucidates the distinct roles of surface chemistry and intermolecular forces, providing a molecular basis for designing carbon materials optimized for high selectivity in complex environmental gas streams.

Reducing emissions of nitrogen compounds represents a significant challenge in environmental protection, and catalytic treatment is an effective approach. Carbon-based catalysts offer a promising alternative by exploiting the redox properties of carbon materials and eliminating the need for external reducing agents. In this study, nitrogen-free and nitrogen-doped activated carbons were used for NO reduction. The catalysts were developed by incorporating transition metals (Cu and Fe), alkali metals (K), and bimetallic Cu-K formulations. The addition of K to Cu and the presence of nitrogen functionalities improved the catalytic performance and an optimum Cu/K ratio was identified. The best-performing catalyst, AC_M_BM@5Cu5K, achieved 100% NO conversion at 410 °C, producing mainly N₂ and CO₂, while N₂O was detected as an intermediate and CO was not observed. The catalyst’s stability was evaluated in a 100 h continuous test at 376 °C, during which the catalyst maintained approximately 90% NO conversion for 40 h before deactivation. The deactivation mechanism is discussed in detail.

Monte Carlo simulations of the transport of atoms in gases related to the deposition process and the contamination of amorphous carbon thin films during deposition in magnetron discharges have been performed. These films are of interest in accelerator technology due to their low secondary electron yield when their structures are dominated by sp² carbon. Two codes, which practically share the same algorithm, are introduced: TAGs 1 simulates the transport of sputtered atoms from the target to the substrate, and TAGs 2 simulates the transport of atoms from the plasma towards the target and the substrate. The similar results of TAGs 1 and the well-established SIMTRA for the same input parameters imply the algorithm’s accuracy. The codes were used to model the transport of different atoms (C, H, O, D) in a magnetron Ar discharge. The simulations reveal that the operating pressure should be higher than 1 Pa for a sample-target distance of 90 mm to secure sp² carbon formation. The contamination mechanisms of amorphous carbon coatings were then studied by merging the results obtained with both programs. Preliminary comparisons with experiments suggest that the combined results of TAGs 1 and 2 agree very well with the experiments.