In municipal wastewater treatment plants, some dissolved methane can enter the aerobic bioreactors. This greenhouse gas originates from sewers and return flows from anaerobic sludge treatment. In well-mixed conventional activated sludge reactors, methane emissions are largely avoided because methane oxidizing bacteria consume a large fraction, even without optimizing for this purpose. In this work, the fate of dissolved methane is studied in aerobic granular sludge reactors, as they become increasingly popular. The influence of the characteristic design and operating conditions of these reactors are studied with a mathematical model with apparent conversion kinetics and stripping: the separation of feeding and aeration in time, a higher substrate transport resistance, a high retention time of granular biomass and a taller water column. Even for a best-case scenario combining an unrealistically low intragranule substrate transport resistance, a high retention time, a tall reactor, an extremely high influent methane concentration and no oxygen limitation, the methane conversion efficiency was only 12% when feeding and aeration were separated in time, which is lower than for continuous activated sludge reactors under typical conditions. A more rigorous model was used to confirm the limited conversion, considering the multi-species and multi-substrate biofilm kinetics, anoxic methane consumers and the high substrate concentration at the bottom during upward plug flow feeding. The observed limited methane conversion is mainly due to the high concentration that accumulates during unaerated feeding phases, which favours stripping more than conversion in the subsequent aeration phase. Based on these findings, strategies were proposed to mitigate methane emissions from wastewater treatment plants with sequentially operated reactors.

This work shows how more variables can be monitored with a single off-gas sampler on sequentially operated than on continuously fed and aerated reactors and applies the methods to data from a full-scale aerobic granular sludge reactor as a demonstration and to obtain insight in this technology. First, liquid-gas transfer rates were calculated. Oxygen (O₂) absorption and carbon dioxide (CO₂) emission rates showed comparable cyclic trends due to the coupling of O₂ consumption and CO₂ production. Methane (CH₄) emissions showed a stripping profile and nitrous oxide (N₂O) emissions showed two peaks each cycle, which were attributed to different production pathways. Secondly, aeration characteristics were calculated, of which the gradual improvement within cycles was explained by surfactants degradation. Thirdly, liquid phase concentrations were estimated from off-gas measurements via a novel calculation procedure. As such, an average influent CH₄ concentration of 0.7 g·m⁻³ was found. Fourthly, reaction rates could be estimated from off-gas data because no feeding or discharge occurred during reaction phases. The O₂ consumption rate increased with increasing dissolved oxygen and decreased once nitrification was complete. Fifthly, greenhouse gas emissions could be derived, indicating a 0.06% N₂O emission factor. Sixthly, off-gas gave an indication of influent characteristics. The CO₂ emitted per kg COD catabolized corresponded with the TOC/COD ratio of typical wastewater organics in cycles with balanced nitrification and denitrification. High nitrogen removal efficiencies were associated with high catabolized COD/N ratios as estimated from the O₂ absorption. Finally, mass balances could be closed using off-gas O₂ data. As such, an observed yield of 0.27 g COD/g COD was found. All these variables could be estimated with a single sampler because aeration without feeding creates a more homogeneous off-gas composition and simplifies liquid-phase mass balances. Therefore, off-gas analyzers may have a broader application potential for sequentially operated reactors than currently acknowledged.

This study deals with the effect of aeration control strategies on the nitrogen removal efficiency and nitrous oxide (N₂O) emissions in a partial nitritation–anammox reactor with granular sludge. More specifically, dissolved oxygen (DO) control, constant airflow and effluent ammonium (NH₄⁺) control strategies were compared through a simulation study. Particular attention was paid to the effect of flocs, which are deliberately or unavoidable present besides granules in this type of reactor. When applying DO control, DO setpoints had to be adjusted to the amount of flocs present in the reactor to maintain high nitrogen removal and reduce N₂O emissions, which is difficult to realize in practice because of variable floc fractions. Constant airflow rate control could maintain a good nitrogen removal efficiency independent of the floc fraction in the reactor, but failed in N₂O mitigation. Controlling aeration based on the effluent ammonium concentration results in both high nitrogen removal and relatively low N₂O emissions, also in the presence of flocs. Fluctuations in floc fractions caused significant upsets in nitrogen removal and N₂O emissions under DO control but had less effect at constant airflow and effluent ammonium control. Still, rapid and sharp drops in flocs led to a peak in N₂O emissions at constant airflow and effluent ammonium control. Overall, effluent ammonium control reached the highest average nitrogen removal and lowest N₂O emissions and consumed the lowest aeration energy under fluctuating floc concentrations.

Gas bubbles are introduced in water to absorb or strip volatile substances in a variety of unit operations, for example during (waste)water treatment. To calculate the transfer rate of substances between the liquid phase and the gas phase, different assumptions have been made in literature regarding the gas phase composition and hydraulic pressure, which both vary along the reactor height. In this study, analytical expressions were derived for the total (macroscopic) liquid-gas transfer rate, using either the complete gradients of the mole fraction and pressure (comprehensive approach) or a uniform value, for one or both of them. Simulations with the comprehensive model were performed to understand the effect of the type of volatile substance and of the reactor design and operating conditions on the total liquid-gas transfer rate. These effects were found to be highly interactive and often non-linear. Next, the simulation results of the comprehensive model were compared with those from models that assume either a uniform mole fraction or a uniform pressure in the complete reactor volume. This illustrated that for soluble substances, the mole fraction gradient strongly affects the total liquid-gas transfer rate, while the pressure gradient became only important under operating conditions that promote stripping (i.e., for a high concentration in the liquid phase and low concentration in the inlet gas). For very poorly soluble substances, the pressure became more important under conditions that promote absorption. These results on the importance of the mole fraction and pressure gradients remained equally valid when explicitly considering a typical variation of the volumetric overall transfer coefficient (K_La) along the reactor height. Finally, a simple and fast procedure was made available through a spreadsheet to select appropriate simplifying assumptions in reactor or plant-wide models. By applying the procedure to oxygen (O₂), carbon dioxide (CO₂), methane (CH₄), nitrous oxide (N₂O) and nitrogen gas (N₂) in an aerobic biological wastewater treatment reactor, it was demonstrated that some common simplifications can lead to significant errors, for which corrections were proposed.

Wastewater treatment processes with granular sludge are compact and are becoming increasingly popular. Interest has been accompanied by the development of mathematical models. This contribution simultaneously reviews available models in the scientific literature for anaerobic, aerobic and partial nitritation-anammox granular sludge reactors because they comprise common phenomena (e.g. liquid, gas and granule transport) and thus pose similar challenges. Many of the publications were found to have no clearly defined goal. The importance of a goal is stressed because it determines the appropriate model complexity and helps other potential users to find a suitable model in the vast amount of literature. Secondly, a wide variety was found in the model features. This review explains the chosen modelling assumptions based on the different reactor types and goals wherever possible, but some assumptions appeared to be habitual within fields of research, without clear reason. We therefore suggest further research to more clearly define the range of operational conditions and goals for which certain simplifying assumptions can be made, e.g. when intragranule solute transport can be lumped in apparent kinetics and when biofilm models are needed, which explicitly calculate substrate concentration gradients inside granules. Furthermore, research is needed to better mechanistically understand detachment, removal of influent particulate matter and changes in the mixing behaviour inside anaerobic systems, before these phenomena can be adequately incorporated in models. Finally, it is suggested to perform full-scale model validation studies for aerobic and anammox reactors. A spreadsheet in the supplementary information provides an overview of the features in the 167 reviewed models.