Forschungsdaten – Titel und Zusammenfassungen von Publikationen, extrahierte Daten und Katalogeinträge – erscheinen in ihrer Originalsprache Englisch.

KI-Zusammenfassung

78 % Konfidenz

This study operated a sequential two-reactor bioelectrochemical system (reductive cathode at −450 mV SHE, oxidative anode at +1.4 V SHE) for PCE dechlorination under two feeding regimes: mineral medium and synthetic groundwater containing SO₄²⁻ (680 mg/L) and NO₃⁻ (20 mg/L). Switching to synthetic groundwater caused temporary PCE removal efficiency to drop from 99±1% to 85±2%, accompanied by a 45-fold decrease in D. mccartyi 16S rRNA abundance. The system compensated by increasing current from −19 mA to −65 mA, driven by competing SO₄²⁻ and NO₃⁻ reduction (45% and 4% coulombic efficiency respectively), not by RD competition but by lower ionic strength and missing trace nutrients in the synthetic groundwater.

Zentrale Erkenntnisse

  • Mechanismus Sulfate reduction consumed 45±9% of cathode current at −450 mV SHE, yet did not compete with PCE dechlorination for reducing power; instead, current increased 3.6-fold to supply both reactions, indicating electron availability was not the limiting factor.

    Was heißt das. Operators should not assume that SO₄²⁻ and NO₃⁻ in groundwater will inhibit RD via electron competition; instead, monitor biomass viability (D. mccartyi abundance) and ionic strength as the real limiting factors.

  • Leistung D. mccartyi 16S rRNA gene copies dropped from 1.30×10⁸ to 2.92×10⁶ copies/L (45-fold decrease) when synthetic groundwater replaced mineral medium, despite complete PCE removal being restored after 2 HRT, indicating biomass recovery without proportional gene recovery.

    Was heißt das. Gene copy abundance alone is not a reliable real-time indicator of RD capacity recovery; measure PCE removal rate and product distribution to confirm functional restoration.

  • Zielkonflikt RD coulombic efficiency collapsed from 8±2% (mineral medium) to 1±1% (synthetic groundwater) at the same cathode potential (−450 mV SHE), while global current recovery improved from 10±2% to 61±16%, revealing that unrecovered current remained substantial (17 mA → 25 mA absolute) and unrelated to identified reduction pathways.

    Was heißt das. Membrane-less, internal counter-electrode designs suffer from persistent electron loops (H₂ cycling, side reactions) that scale with current; quantify unaccounted current to identify hidden parasitic pathways.

  • Mechanismus Oxidative reactor developed reductive dechlorination capacity (86±3% TCE removal, 116±32 µeq/Ld RD rate) after 10 HRT exposure to incomplete RD products from the cathode, driven by D. mccartyi colonization of the internal graphite counter-electrode at −0.7±0.1 V SHE.

    Was heißt das. Anode compartments with cathodic internal electrodes can become unintended RD zones; isolate counter-electrodes or operate at potentials >+0.5 V SHE to suppress anaerobic biofilm growth.

  • Schwellenwert Nitrate reduction (20 mg/L NO₃⁻ inlet) consumed only 4±1% of cathode current despite complete removal, whereas sulfate (680 mg/L SO₄²⁻) consumed 45±9%, indicating NO₃⁻ reduction kinetics are much faster or that NO₃⁻ is not the rate-limiting electron sink at −450 mV SHE.

    Was heißt das. At −450 mV SHE, NO₃⁻ reduction is kinetically favorable but not a major current sink; SO₄²⁻ becomes the dominant competing electron acceptor in realistic groundwater.

Ansatzpunkte6

Konkrete Lücken in dieser Publikation, jeweils mit einem Experiment, das sie schließen würde.

  • Hoch No measurement of N₂O or NO₂⁻ accumulation during nitrate reduction at −450 mV SHE; the paper assumes complete reduction to N₂ but provides no gas chromatography or ion chromatography data for intermediate N species.

    Nitrate reduction is reported as 'complete' (Figure 6b shows inlet 20 mg/L → outlet ~0 mg/L) but the reduction product is never identified. At −450 mV SHE, incomplete reduction to N₂O or NO₂⁻ is possible and would affect coulombic efficiency calculation and environmental impact.

    Versuch. Measure N₂O, NO, and NO₂⁻ in reductive reactor headspace and effluent using GC-ECD and ion chromatography across −350 to −550 mV SHE cathode potential range; quantify N balance.

  • Hoch No systematic variation of cathode potential to identify the operating window where RD is favored over SO₄²⁻ reduction; only −450 mV SHE is tested with synthetic groundwater.

    The paper states prior work tested −550 mV SHE (reference 24) but does not compare RD vs SO₄²⁻ reduction selectivity across a potential range. At −450 mV SHE, SO₄²⁻ reduction dominates (45% CE); more negative potentials might suppress it or enhance RD.

    Versuch. Operate reductive reactor at −350, −400, −450, −500, −550 mV SHE with synthetic groundwater; measure RD rate, SO₄²⁻ removal rate, and D. mccartyi abundance as functions of potential.

  • Mittel No investigation of ionic strength or trace nutrient supplementation to restore D. mccartyi abundance without changing the groundwater composition; the paper identifies low ionic strength (0.83 mS/cm) and missing nutrients as the cause but does not test remediation.

    The authors conclude 'the decrease of the RD rate was probably related to the different composition of the feeding solution, both in terms of nutrients and ionic strength' but do not experimentally validate this by adding back NaCl or trace metals to synthetic groundwater.

    Versuch. Prepare three synthetic groundwater variants: (1) baseline (0.83 mS/cm), (2) + NaCl to 2.68 mS/cm, (3) + trace metals (Fe, Ni, Co, Mo); measure PCE removal rate, D. mccartyi 16S rRNA, and RD coulombic efficiency.

  • Mittel No characterization of the unrecovered current (25 mA or 39% of total during synthetic groundwater period); the paper acknowledges it but does not identify the electron sink.

    Text states 'the unrecovered current, i.e., the current that was not justified by the identified reduction reactions, reached a similar value' and attributes it to 'electron loops of species such as hydrogen' but provides no direct measurement of H₂ production or oxidation rates.

    Versuch. Measure H₂ concentration in reductive reactor headspace and effluent using GC-TCD; calculate H₂ production rate and compare to unrecovered current; test with and without internal counter-electrode.

  • Mittel No measurement of catholyte pH or buffering capacity during synthetic groundwater operation; pH can affect both RD kinetics and SO₄²⁻ reduction product speciation (H₂S vs HS⁻).

    The paper does not report pH in either feeding solution or reactor effluent. Synthetic groundwater may have lower buffering capacity than mineral medium, affecting microbial metabolism and product distribution.

    Versuch. Monitor catholyte pH continuously during synthetic groundwater operation; measure H₂S and HS⁻ speciation in effluent; test pH buffering with added bicarbonate.

  • Niedrig Oxidative reactor developed unintended RD capacity (TCE removal, cisDCE accumulation) but no systematic study of how to suppress it or exploit it; the paper treats it as an artifact.

    The authors note 'the presence of D. mccartyi in the oxidative reactor was likely due to the presence of the internal graphite counter electrode' and show 86±3% TCE removal, but do not test whether this is beneficial (removes incomplete RD products) or detrimental (wastes oxidative capacity).

    Versuch. Compare oxidative reactor performance with and without internal counter-electrode; measure VC and Eth removal efficiency as a function of counter-electrode potential (−0.5 to +0.2 V SHE).

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Was gemacht wurde

Systemtyp
MEC

Was funktioniert hat

Noch keine Ergebniskennzahlen extrahiert.

Zusammenfassung

Chlorinated aliphatic hydrocarbons (CAHs) are common groundwater contaminants due to their improper use in several industrial activities. Specialized microorganisms are able to perform the reductive dechlorination (RD) of high-chlorinated CAHs such as perchloroethylene (PCE), while the low-chlorinated ethenes such as vinyl chloride (VC) are more susceptible to oxidative mechanisms performed by aerobic dechlorinating microorganisms. Bioelectrochemical systems can be used as an effective strategy for the stimulation of both anaerobic and aerobic microbial dechlorination, i.e., a biocathode can be used as an electron donor to perform the RD, while a bioanode can provide the oxygen necessary for the aerobic dechlorination reaction. In this study, a sequential bioelectrochemical process constituted by two membrane-less microbial electrolysis cells connected in series has been, for the first time, operated with synthetic groundwater, also containing sulphate and nitrate, to simulate more realistic process conditions due to the possible establishment of competitive processes for the reducing power, with respect to previous research made with a PCE-contaminated mineral medium (with neither sulphate nor nitrate). The shift from mineral medium to synthetic groundwater showed the establishment of sulphate and nitrate reduction and caused the temporary decrease of the PCE removal efficiency from 100% to 85%. The analysis of the RD biomarkers (i.e., Dehalococcoides mccartyi 16S rRNA and tceA, bvcA, vcrA genes) confirmed the decrement of reductive dechlorination performances after the introduction of the synthetic groundwater, also characterized by a lower ionic strength and nutrients content. On the other hand, the system self-adapted the flowing current to the increased demand for the sulphate and nitrate reduction, so that reducing power was not in defect for the RD, although RD coulombic efficiency was less.

Schlagwörter

Reductive dechlorinationDehalococcoidesNitrateEnvironmental chemistryVinyl chlorideMicroorganism

Kennungen

Zeitschrift
Processes
Jahr
2021
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