Resilient High-Rate Sulfidogenesis in a Hydrogen-Based Membrane Biofilm Reactor: Mechanistic Analysis of Kinetic-Limited Performance Under Variable Loading.
Copper mining industry generates water with high sulfate (SO4 2-) concentrations. The hydrogen-based membrane biofilm reactor (H2-MBfR) is a promising sulfidogenesis solution, using H2 as a clean electron donor. An H2-MBfR was operated for 209 days treating synthetic mining-influenced water under varying conditions (HRT, H2 pressure, SO4 2- loadings). The system proved highly resilient, achieving stable SO4 2- removal (> 90%) and fully recovering from a severe shock load (4500 mg S L-1). To identify the governing mechanisms, a transient pseudoanalytical biofilm model was developed. A Global Sensitivity Analysis (Sobol) showed performance is dominated by the maximum specific growth rate ( ), detachment coefficient ( ), and H2S inhibition ( ). The model was calibrated on Stages 1-3 (Days 0-169, n = 44), achieving R² = 0.962 (calibration) and R² = 0.572 (blind validation, Stage 4). Crucial findings from the model calibration ( = 0.344 d-1) and a diagnostic analysis using the Thiele Modulus (mean = 0.224) strongly indicate that the system operated in a kinetically-limited regime. Performance was governed by the delicate balance of slow growth and high detachment, not by mass transfer (H2 supply or SO4 2- diffusion). This research validates the H2-MBfR for high-rate applications and correctly shifts the bottleneck for future optimization from mass transfer to biofilm retention kinetics.
- Research Article
2
- 10.1016/j.memsci.2023.122390
- Dec 26, 2023
- Journal of Membrane Science
Effects of hydrogen pressure on stabilization with improved denitrification in a hydrogen-based membrane biofilm reactor
- Research Article
19
- 10.1016/j.ces.2018.11.032
- Nov 14, 2018
- Chemical Engineering Science
Model-based evaluation of selenate and nitrate reduction in hydrogen-based membrane biofilm reactor
- Research Article
30
- 10.1007/s11356-016-7370-1
- Aug 13, 2016
- Environmental Science and Pollution Research
Tetracycline (TC) in aqueous environment could be reductively degraded by using a hydrogen-based membrane biofilm reactor (H2-MBfR) under denitrifying conditions as it provides an appropriate environment for the antibiotic-degrading bacteria in biofilm communities. This study evaluates the performance of H2-MBfR for simultaneous removal of nitrate and TC, formation of degradation products of TC, and community analysis of the biofilm grown on the gas-permeable hollow fiber membranes. Hence, a H2-MBfR receiving approximately 20mg N/l nitrate and 0.5mg/l TC was operated under different H2 pressures, hydraulic retention times (HRTs), and influent TC concentrations in order to provide various nitrate and TC loadings. The results showed that H2-MBfR accomplished successfully the degradation of TC, and it reached TC removal of 80-95% at 10h of HRT and 6psi (0.41atm) of H2 gas pressure. TC degradation took placed at increased HRT and H2 pressures while nitrate was the preferred electron acceptor for most of the electrons generated from H2 oxidation used for denitrification. The transformation products of TC were found at part per billion levels through all the experiments, and the concentrations decreased with the increasing HRT regardless of H2 pressure. Analyses from clone library showed that the microbial diversity at the optimal conditions was higher than that at the other periods. The dominant species were revealed to be Betaproteobacteria, Acidovorax caeni, and Alicycliphilus denitrificans.
- Research Article
65
- 10.1016/j.jhazmat.2016.08.014
- Aug 5, 2016
- Journal of Hazardous Materials
Chlortetracycline removal by using hydrogen based membrane biofilm reactor
- Research Article
33
- 10.1016/j.watres.2014.03.053
- Mar 28, 2014
- Water Research
Bio-reduction of tetrachloroethen using a H2-based membrane biofilm reactor and community fingerprinting
- Research Article
154
- 10.1021/es051251g
- Feb 1, 2006
- Environmental Science & Technology
A H2-based, denitrifying and sulfate-reducing membrane-biofilm reactor (MBfR) was shown to be effective for removing selenate (Se(VI)) from water or wastewater by reducing it to insoluble Se(0). When Se(VI) was first added to the MBfR, Se(VI) reduction--first to selenite (Se(IV)) and then mostly to Se(0)--took place immediately and then increased over three weeks, suggesting enrichment for dissimilatory selenium-reducing bacteria. Increasing the H2 pressure improved the Se(VI) reduction rate and total-Se removal, and lowering the influent Se(VI) concentration from 1000 to 260 microg Se/L increased the average Se removal to 94%, which corresponded to an effluent Se concentration of less than 12 microg Se/L, a value well below the standard of 50 microg Se/L. The fact that the effluent suspended solids contained reduced Se suggests that Se(0) was retained in the biofilm, which detached to form the effluent suspended solids. A series of short-term experiments elaborated on how decreased influent selenate loading and increased H2 pressure could systematically improve the reduction of Se(VI) and removal of total Se. Short-term experiments also demonstrated that selenate reduction improved with lower influent nitrate concentration, suggesting that H2 was more available for selenate reduction when the H2 demand for denitrification was smaller. Complete sulfate reduction, which occurred in parallel to nitrate reduction, dominated the electron-equivalent flux. Like selenate reduction, but unlike nitrate reduction, sulfate reduction was sensitive to H2 pressure and appeared to be inhibited by selenate. Finally, selenate reduction was relatively insensitive to pH in the range of 7.0 to 9.0. This research shows that the MBfR can be effective for removing Se(VI) in water or wastewater to below the 50 microg Se/L standard.
- Research Article
38
- 10.1016/j.cej.2015.04.061
- Apr 18, 2015
- Chemical Engineering Journal
Bioreduction of nitrate in a hydrogen-based membrane biofilm reactor using CO2 for pH control and as carbon source
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22
- 10.1016/j.bej.2012.09.006
- Sep 12, 2012
- Biochemical Engineering Journal
Effect of the kinetics of ammonium and nitrite oxidation on nitritation success or failure for different biofilm reactor geometries
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9
- 10.1016/j.elecom.2020.106823
- Aug 26, 2020
- Electrochemistry Communications
Defect-free metallization of through-glass vias with engineered geometry in additive-free electrolyte
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21
- 10.2166/wst.2005.0189
- Oct 1, 2005
- Water Science and Technology
The hydrogen-based membrane biofilm reactor (MBfR) is effective for reducing nitrate-N to N2 gas, but most wastewaters contain ammonium-N. Here, we document that an aerobic/anoxic MBfR system achieves nearly total N removal (<2 mgN/L) when the influent N is ammonium. The aerobic/anoxic MBfR couples two MBfR modules. The aerobic MBfR is supplied O2 and brings about nitrification of ammonium to nitrate or nitrite. The anoxic MBfR is supplied H2 and brings about denitrification to N2 gas. Total N removal is most strongly influenced by the O2 pressure in the aerobic module: too low O2 caused poor nitrification, while too high O2 inhibited denitrification in the anoxic module. Hydrogen pressure does not strongly affect total-N removal, and the best total-N removal occurs when the H2 and O2 pressures are similar.
- Research Article
33
- 10.1080/03650340.2019.1657845
- Aug 25, 2019
- Archives of Agronomy and Soil Science
Crop model parameters usually vary with diverse field management and environment conditions, which hinder the model calibration. Sensitivity analysis (SA) and uncertainty analysis (UA) for model parameters and outputs are helpful for calibrating crop model under diverse conditions. A global SA and UA were used to determine the maize parameters sensitivity and outputs uncertainty of the AquaCrop model under different irrigation and fertilizer management conditions, i.e. none, slight, and moderate stress pertaining to water and fertility. The results indicated that the sensitive parameters to maximum above ground biomass (AGB) and yield differed from those to canopy cover development and AGB production (time-response outputs of the AquaCrop). The sensitive parameters should be preferentially calibrated given their strong effects on all type of model outputs, besides, the sensitive parameters to the model time-response outputs were somewhat different from those to the model non-time-response outputs. The interaction effects among parameters on the model outputs should receive more attention in the model calibration. The SA and UA results between diverse management were clearly different, and these differences between different fertility stress levels were larger. Fertility stress is a more influential factor on parameters sensitivity and outputs uncertainty than water stress in the AquaCrop model.
- Research Article
12
- 10.3390/w12113196
- Nov 15, 2020
- Water
The back-diffusion of inactive gases severely inhibits the hydrogen (H2) delivery rate of the close-end operated hydrogen-based membrane biofilm reactor (H2-based MBfR). Nevertheless, less is known about the response of microbial communities in H2-based MBfR to the impact of the gases’ back-diffusion. In this research, the denitrification performance and microbial dynamics were studied in a H2-based MBfR operated at close-end mode with a fixed H2 pressure of 0.04 MPa and fed with nitrate (NO3−) containing influent. Results of single-factor and microsensor measurement experiments indicate that the H2 availability was the decisive factor that limits NO3− removal at the influent NO3− concentration of 30 mg N/L. High-throughput sequencing results revealed that (1) the increase of NO3− loading from 10 to 20–30 mg N/L resulted in the shift of dominant functional bacteria from Dechloromonas to Hydrogenophaga in the biofilm; (2) excessive NO3− loading led to the declined relative abundance of Hydrogenophaga and basic metabolic pathways as well as counts of most denitrifying enzyme genes; and (3) in most cases, the decreased quantity of N metabolism-related functional bacteria and genes with increasing distance from the H2 supply end corroborates that the microbial community structure in H2-based MBfR was significantly impacted by the gases’ back-diffusion.
- Research Article
15
- 10.1016/j.scitotenv.2021.150504
- Sep 23, 2021
- Science of The Total Environment
Global sensitivity and uncertainty analysis of a microalgae model for wastewater treatment
- Research Article
21
- 10.1016/j.jhydrol.2023.129604
- Apr 29, 2023
- Journal of Hydrology
Standard hydrologic model evaluation and calibration approaches focus on the accurate simulation of streamflow, disregarding internal process simulations. Stable isotope tracers can provide additional information on water sources, and process flux and storage, which can be used to inform model calibration. This study assesses the added value of isotope data in comparison to current best-practice flow-only calibration methods and evaluates the merits and limitations of isotope simulation performance metrics for the purposes of hydrological model calibration. Following several years of regular isotope sampling and measurement, an isotope-enabled process-based hydrologic model was tested on a large watershed in western Canada (Athabasca River), which allowed model calibration using global sensitivity analyses, Monte Carlo simulations, and multi-objective optimizations. Isotope tracer data were found to improve both process and streamflow component identifiability and produced some minor improvement in individual parameter value identifiability. Calibrating to optimize both flow and isotope simulation performance produced better flow simulation ensembles, with improved observation capture and validation performance, relative to calibrating to optimize flow simulations alone. Using an isotope simulation performance metric which includes timing error as a secondary optimization objective led to more robust streamflow modeling, even in mesoscale watersheds with limited isotope observation datasets.
- Research Article
193
- 10.1016/s0010-4655(01)00159-x
- May 1, 2001
- Computer Physics Communications
Sensitivity analysis in model calibration: GSA-GLUE approach