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Anaerobic treatment of a biorefinery’s process-wastewater
(2024) Khan, Muhammad Tahir; Lemmer, Andreas
The phrase “one man's trash is another man’s treasure” perfectly embodies the concept of a circular bioeconomy, emphasizing the conversion of waste into valuable resources while embracing a zero-waste approach. In line with this perspective, the primary objective of the current research was to assess the suitability of a biorefinery’s process-wastewater as a potential feedstock for biogas plants by investigating its anaerobic biodegradability and exploring its biogas and methane production potentials. For such a specific purpose, the process-wastewater from a commercial-scale biorefinery specializing in 5-hydroxymethylfurfural (5-HMF) synthesis and refining was utilized. To fulfill the main objective, three independent sub-objectives were formulated. The initial investigation centered on assessing the biochemical methane potential (BMP) of the typical constituents present in process-wastewater, such as furans (5-HMF and furfural), phenols (syringaldehyde, vanillin, and phenol), and weak acids (levulinic and glycolic acid), as well as the full 5-HMF process-wastewater. The BMP assessments for each test substance were conducted separately at different concentrations (2, 4, 6, and 8 gCOD/L) and temperatures (37°C and 53°C) via the Hohenheim batch fermentation test. The model components at 2 gCOD/L, apart from phenol at 53°C, were efficaciously degraded, in most cases to such an extent, that supplementary methane generation was detected i.e. exceeding their maximum theoretical limits. However, increasing the concentrations of the test components in the assays resulted in diminishing methane conversion at both operating temperatures. Eventually, among the tested components, the 5-HMF process-wastewater was evaluated to be one of the most refractory substrates, following phenol, vanillin, and 5-HMF, when tested at its maximum load under mesophilic and thermophilic conditions. The subsequent investigation focused on examining the anaerobic decomposition of the 5-HMF process-wastewater and its main identified constituents, including 5-HMF, furfural, and levulinic acid in continuously operated anaerobic filters (AFs). The test substances were individually injected into the biofilm reactors operating at 43°C in a controlled manner with a randomized experimental design. This study yielded some unusual outcomes i.e., the test substrates exhibited satisfactory degradation, while at other instances, they hampered the process. Introducing butyric acid between the injected components revealed no signs of compromised consortia. The 5-HMF process-wastewater in this investigation emerged as the least favorable substrate for methane conversion. The culmination of the current research involved utilizing the 5-HMF process-wastewater as a sole feedstock for the fixed-bed reactors. Hence, necessary nutrients to support the existing microbial consortia in the AFs were added to the process-wastewater. Given its toxic nature, the substrate dosage was initiated from its reduced concentration of 10 gCOD/L and was gradually increased to 20, 30, 40, and 50 gCOD/L, with corresponding organic loading rates (OLRs) of 2, 4, 6, 8, and 10 gCOD/L.d, respectively, as the trial progressed. Despite meeting the nutrient requirements, the gas yields, in particular methane, were not remarkable. However, a noteworthy finding surfaced: as the gCOD/L of the fed substrate increased, so did the concentrations of the short-chained volatile fatty acids (SCVFAs) in the reactors. This observation led to the conclusion that the low methane yields were at the behest of the accumulation of SCVFAs in the AFs, at both mesophilic and thermophilic temperatures. Ultimately, the subpar performance of the process-wastewater as a substrate is considered to stem from its exceptionally high concentration of the pollutant 5-HMF, which significantly influences its overall characteristics, causing longer lag phases, especially at higher OLRs. This, in turn, triggers the inhibitory behavior, leading to reduced methane yields. Consequently, these factors render the 5-HMF process-wastewater a precarious choice for biogas plants in terms of efficient energy recovery. While AFs are well-suited technology for treating high-strength wastewaters, for the substrate such as 5-HMF process-wastewater, it might be beneficial to increase retention times by decreasing the OLRs. Additionally, reducing the strength via dilution combined with these adjusted process parameters could further enhance its decomposition. Anaerobic digestion (AD), traditionally used for energy recovery from (bio)wastes, has potential beyond biogas production in the bioeconomy. This research showed that the highly recalcitrant 5-HMF process-wastewater can be a viable source for producing SCVFAs through AD. Furthermore, the Muttenz biorefinery could utilize the filtration byproducts to produce levulinic acid, aligning with a cascading biorefinery approach.
Innovative process chain for the resource-efficient production of biomethane-based fuels
(2024) Holl, Elena; Lemmer, Andreas
Biogas is a key component in renewable energy production and holds significant potential for achieving Germany’s climate goals. In the transport sector, where the share of renewa-ble energy was only 6.8% in 2023, greenhouse gas (GHG) emissions must be reduced from 147.9 Mt in 2022 to 84 Mt by 2030. Biomethane-based fuels such as bio-LNG and bio-CNG are promising alternatives that are compatible with existing infrastructure and vehicle technologies, already contributing to emission reductions. This study aims to optimize biomethane production through an innovative process chain for decentralized and resource-efficient provision of methane-based fuels. Biogas production was analyzed using two-stage anaerobic digestion (TSAD) to determine optimal substrate compositions and operating parameters. Biogas upgrading was conducted via biological hydrogen methanation (BHM), a power-to-gas technology that enhances process efficiency and economic viability. The results demonstrate that TSAD achieves high methane content (> 60%) even under high organic loads, while BHM performance can be further improved through pressure and temperature optimization. A life cycle assessment (LCA) confirms the efficiency gains of the new process chain compared to conventional methods. The use of renewable energy in process stages has the greatest impact on reducing GHG emissions. Decentralized bio-LNG production from agricultural residues emerges as a feasible solution for producing CO₂-negative fuels.
Investigation of phosphorus recovery from biogas digestate: low-technology approaches for enhanced solid-liquid separation
(2025) Uppuluri, Naga Sai Tejaswi; Müller, Joachim
Phosphorus (P) is a critical nutrient for agriculture, essential for plant growth and food security. However, the global dependence on finite P reserves, primarily located in northern Africa and China, presents significant challenges, including supply chain vulnerabilities and rising fertilizer costs. Additionally, excessive P runoff into water bodies contributes to environmental issues, such as eutrophication. Addressing these challenges requires sustainable P management strategies, including P recovery from alternative sources like biogas digestate. To tackle these challenges, regulatory measures and innovative recovery techniques are being explored to improve P sustainability. In Germany, regulations like the Fertilizer Ordinance and the Sewage Sludge Ordinance have introduced strict limits on P application and mandated the recovery of P from waste streams, promoting environmentally friendly nutrient management practices. These regulations aim to reduce environmental impacts while ensuring the efficient use of P resources. A primary objective of this research is to develop a cost-effective, practically feasible method for P recovery that can be easily integrated into existing biogas plants without requiring substantial infrastructure upgrades. This study investigated the recovery of P from biogas digestate using additives such as kieserite (MgSO₄∙H₂O), straw flour, and biochar to improve separation efficiency and nutrient recovery. The additives enhanced the P content in the solid phase, making it easier to recycle P back into agricultural systems. The laboratory-scale separation trials were conducted to evaluate the effectiveness of three additives categorized into reactive (kieserite) and non-reactive (straw flour and biochar) groups. The separations were carried out using a hydraulic tincture press, with a pressure of 5 MPa applied for 120 seconds. The trials tested five different treatment times: 0 h, 1 h, 2 h, 8 h, and 20 h. Kieserite was tested at 25 °C and 50 °C, while straw flour and biochar were tested only at 25 °C. The results revealed that longer treatment durations with kieserite were more effective, with 61% of P shifting into the solid phase after 20 h. In contrast, treatment duration had little impact on the effectiveness of straw flour and biochar. Kieserite treatment increased NaOH-P and HCl-P, indicating the formation of more stable, non-labile P fractions due to the interaction between (Mg²⁺) ions from kieserite and phosphate (PO₄³⁻) ions. These findings concluded that kieserite, as a reactive additive, is more effective at enhancing P recovery by converting labile P into more stable, non-labile forms. Based on the conclusions from laboratory-scale separation trials, practical scale experiments were conducted at the research biogas facility ‘Unterer Lindenhof’ at the University of Hohenheim. In these trials, straw flour and kieserite were used as additives, with treatment durations of 4 h and 22 h. The shorter duration represented same-day processing, while the longer duration simulated overnight treatment. Results showed that extending the treatment time with kieserite significantly improved P removal efficiency (PRE), reaching 67% of P shifted to the solid phase after 22 h. Straw flour, on the other hand, achieved a 52% PRE at the same duration, with most of the P remaining in labile fractions regardless of treatment time. Kieserite treatment resulted in notable changes in the distribution of P fractions, shifting from NaHCO₃-P to more stable NaOH-P and HCl-P fractions as the treatment duration increased. These experiments provide a technical proof-of-concept for the use of additives in biogas plants for digestate treatment to enhance P recovery into the solid phase, supporting more sustainable nutrient management practices. Biochar modified with kieserite and calcium chloride (CaCl₂) was evaluated as an additive for P recovery, along with the metal salts used independently. The modification aimed to load Mg²⁺ and Ca²⁺ ions onto the biochar surface, enhancing its effectiveness. Initial separation trials established that using 5 gadditive/Ldigestate with a 22 h treatment time provided optimal conditions for solid-liquid separation. The separation trials were made in the laboratory using a hydraulic tincture press. The modification significantly increased the Mg content in kieserite-modified biochar (KIS-B) and the Ca content in CaCl₂-modified biochar (Ca-B). Both modified biochars and the metal salts increased P transfer to the solid phase, with the metal salts alone demonstrated higher PRE. KIS-B and Ca-B shifted P to non-labile fractions, while kieserite and CaCl₂ alone resulted in an even higher proportion of non-labile P fractions. Although the modified biochar showed slightly lower PRE compared to metal salts, its potential benefits in agricultural applications are noteworthy. Future studies should include a comprehensive cost-benefit analysis to evaluate the long-term financial sustainability of implementing these recovery techniques at full scale. Reducing the reliance on expensive, finite phosphorus reserves through local recovery can lower input costs for farmers, making the process economically attractive. Additionally, plant pot trials will be essential in assessing the agronomic efficiency of P recovered from biogas digestate. These trials can help determine how effectively the recovered P promotes plant growth and nutrient uptake compared to conventional fertilizers. Ultimately, refining these recovery techniques and assessing their impact on both economic viability and agricultural productivity will play a key role in advancing sustainable nutrient management practices globally.

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