Search

[Display omitted] • Novel nitrogen-doped graphene cubes (NGCs) were synthesised. • The lightweight NGCs were employed for sulfamethoxazole (SMX) degradation. • Identification of reactive oxygen species was conducted. • Comprehensive mechanistic studies on SMX degradation were performed. As a sustainable and green approach, carbocatalysis, a metal-free strategy, has shown exceptional results in advanced oxidation processes (AOPs). Nonetheless, the recovery of these catalysts has been a major shortcoming over the years. Herein, three-dimensional nitrogen-doped graphene macrostructures (3D-NGMs), in the form of macro cubes, were synthesised by a simple cross-linking and thermal annealing procedure, after which they were employed in the activation of peroxydisulfate (PS) for the degradation of sulfamethoxazole (SMX). The catalytic cubes were loaded with different amounts of nitrogen precursor to investigate the role of nitrogen configuration in the sp2 hybridised carbon network on AOPs. NGC3 cubes with optimum N-loading exhibited outstanding performance for SMX degradation owing to their optimum N/C ratio. Various reaction parameters were studied to optimise the catalytic system. Comprehensive studies on the radical generation were done and illustrated the dominance of the non-radical pathway leading to the proposal of a possible reaction mechanism for SMX. This study not only suggests the role of nitrogen doping on graphene macrostructures but also provides novel insights into macro catalysis to overcome the recovery challenges posed by nano catalysis. [ABSTRACT FROM AUTHOR]

[Display omitted] • A perforated CuFe 2 O 4 /Fe 2 O 3 composite was designed by a MOF-derived solid-state process. • The composite shows efficient PMS activation for sulfamethoxazole degradation. • Both radical and non-radical degradation contributed to SMX remediation. • Possible degradation mechanisms were proposed. • The catalyst shows excellent stability and reusability via magnetic recovery. Design of metal–organic framework (MOF) derived metal oxides is an effective approach for environmental remediation. The current study describes the fabrication of MIL-53-derived perforated CuFe 2 O 4 /Fe 2 O 3 using a facile, one-step, post-thermal solid-state approach by varying Cu/Fe ratios. Herein, the release of CO 2 and H 2 O during the thermal treatment facilitates the incorporation of Cu2+ onto the Fe 2 O 3 structure, forming a perforated hollow CuFe 2 O 4 /Fe 2 O 3 composite via an in-situ ion-exchange mechanism. The optimised catalyst CF-0.5 displays a high degradation efficiency for the removal of sulfamethoxazole (SMX) by heterogeneous activation of peroxymonsulfate (PMS), ascribing to the better textural, morphological, and elemental properties of the novel catalyst. Important reaction parameters such as pH, catalyst loading, PMS dosage, pollutant kind and concentration, and reaction temperature are further optimised to develop a cost-effective catalytic system. The magnetically recoverable catalyst outlines a high stability rate, and only a 9 % efficiency loss is observed even after the fourth cycle. Reactive oxygen species (ROS) are identified by electron paramagnetic resonance spectroscopy (EPR) and their roles are determined by performing quenching experiments. In the end, a detailed study of the mineralisation ability and reaction intermediates is performed and possible pathways for the degradation mechanism are proposed. This study not only introduces a facile approach for the fabrication of MOF-driven nanomaterials but provides insights into the removal of emerging contaminants such as SMX. [ABSTRACT FROM AUTHOR]

[Display omitted] • A novel g-C 3 N 4 /Fe 2 O 3 /rGO ternary composite was synthesised using a hydrothermal process. • The catalyst exhibits a high photocatalytic oxidation efficiency for the removal of sulfamethoxazole. • Reactive oxygen species were identified by quenching tests and electron paramagnetic resonance spectra. • Detailed mechanistic studies were performed to deduce the radical and non-radical degradation pathways. Rational design of semiconductor photocatalysts is an effective way to achieve efficient visible-light-driven environmental remediation. Herein, a series of graphitic carbon nitride (g-C 3 N 4) engineered hematite (Fe 2 O 3)/reduced graphene oxide (rGO) photocatalysts were synthesised and employed in visible-light-driven photo-Fenton-like degradation of sulfamethoxazole (SMX). The exceptional performance of the optimal photocatalyst (0.4-FerGCN-3) was achieved because of the successful structural integration of g-C 3 N 4 /Fe 2 O 3 /rGO for efficient separation and migration of photoinduced charge carriers (e−/h+). Photochemical decomposition efficiency was also optimised by analysing the important reaction parameters such as initial catalyst loading, initial H 2 O 2 dosage, pH, and reaction temperature. Detailed studies on the generation of reactive species and degradation intermediates were performed to propose a possible mechanism for SMX degradation. The findings may provide not only a strategy for nanostructure engineering of semiconductor photocatalysts but also insights into the effective remediation of emerging contaminants such as SMX. [ABSTRACT FROM AUTHOR]