Covalent modification of reduced graphene oxide with piperazine as a novel nanoadsorbent for removal of H2S gas

In the present research, piperazine grafted-reduced graphene oxide RGO-N-(piperazine) was synthesized through a three-step reaction and employed as a highly efficient nanoadsorbent for H2S gas removal. Temperature optimization within the range of 30–90 °C was set which significantly improved the adsorption capacity of the nanoadsorbent. The operational conditions including the initial concentration of H2S (60,000 ppm) with CH4 (15 vol%), H2O (10 vol%), O2 (3 vol%) and the rest by helium gas and gas hour space velocity (GHSV) 4000–6000 h−1 were examined on adsorption capacity. The results of the removal of H2S after 180 min by RGO-N-(piperazine), reduced graphene oxide (RGO), and graphene oxide (GO) were reported as 99.71, 99.18, and 99.38, respectively. Also, the output concentration of H2S after 180 min by RGO-N-(piperazine), RGO, and GO was found to be 170, 488, and 369 ppm, respectively. Both chemisorption and physisorption are suggested as mechanism in which the chemisorption is based on an acid–base reaction between H2S and amine, epoxy, hydroxyl functional groups on the surface of RGO-N-(piperazine), GO, and RGO. The piperazine augmentation of removal percentage can be attributed to the presence of amine functional groups in the case of RGO-N-(piperazine) versus RGO and GO. Finally, analyses of the equilibrium models used to describe the experimental data showed that the three-parameter isotherm equations Toth and Sips provided slightly better fits compared to the three-parameter isotherms

Building and identifying highly active oxygenated groups in carbon materials for oxygen reduction to H2O2

The one-step electrochemical synthesis of H2O2 is an on-site method that reduces dependence on the energy-intensive anthraquinone process. Oxidized carbon materials have proven to be promising catalysts due to their low cost and facile synthetic procedures. However, the nature of the active sites is still controversial, and direct experimental evidence is presently lacking. Here, we activate a carbon material with dangling edge sites and then decorate them with targeted functional groups. We show that quinone-enriched samples exhibit high selectivity and activity with a H2O2 yield ratio of up to 97.8 % at 0.75V vs. RHE. Using density functional theory calculations, we identify the activity trends of different possible quinone functional groups in the edge and basal plane of the carbon nanostructure and determine the most active motif. Our findings provide guidelines for designing carbon-based catalysts, which have simultaneous high selectivity and activity for H2O2 synthesis. The identity of catalytic sites for H2O2 generation in carbon-based materials remains controversial with limited experimental evidence to date. Here, the authors decorate various target functional groups on carbon materials and quinone-enriched samples exhibit the highest activity and selectivity