Research progress and prospect of low-carbon biological technology for nitrate removal in wastewater treatment
Ru Zheng, Kuo Zhang, Lingrui Kong, Sitong Liu
AI summary
72% confidenceThis review synthesizes low-carbon nitrogen removal technologies for wastewater treatment, emphasizing autotrophic and photoelectrotrophic pathways as alternatives to heterotrophic denitrification. It covers sulfur autotrophic denitrification (SAD), hydrogen autotrophic denitrification (HAD), nitrate/nitrite-dependent anaerobic methane oxidation (n-DAMO), and photoelectrotrophic denitrification (PEDeN). The paper highlights operating trade-offs: SAD reduces N2O emissions by ~96% versus heterotrophic denitrification but produces 2.51–4.07 g SO₄²⁻–S per g NO₃⁻–N; HAD achieves 6× higher denitrification rates than S⁰-driven SAD but faces H₂ solubility limits and cost barriers (~3 USD/kg); n-DAMO enables simultaneous CH₄ and N removal at short HRTs (2.16 h) but requires specialized consortia. The review identifies photoelectrotrophic systems as emerging solar-driven alternatives but provides limited quantitative operating windows for cathode potential, current density, or pH effects on product selectivity.
Key insights
Trade-off SAD coupled with anammox reduces sulfur consumption from 2.5 g to 0.43–0.55 g per 1 g nitrogen treated by consuming nitrite intermediates, lowering sulfate production and operational cost.
So what. Operators should couple SAD with anammox in series or single-reactor configurations to minimize sulfate accumulation and reduce electron donor demand, especially when treating low C/N wastewater.
Threshold HAD denitrification rate is ~6× higher than S⁰-driven SAD, but H₂ bioavailability is limited by aqueous solubility of 7.4×10⁻⁴ mol/L at 30 °C, requiring gas-permeable membranes to approach heterotrophic denitrification rates.
So what. Designers must integrate hollow-fiber or porous membranes into HAD reactors to maintain H₂ delivery; without them, nitrogen removal rates will remain below heterotrophic benchmarks despite higher intrinsic kinetics.
Performance PN-n-DAMO-anammox achieves very short HRT of 2.16 h with dissolved CH₄ removal at 10 °C in granular sludge, indicating cold-temperature stability and methane utilization efficiency not reported for other autotrophic pathways.
So what. Operators treating cold wastewater or biogas-containing effluent should prioritize PN-n-DAMO-anammox in granular reactors to exploit dissolved methane and minimize residence time.
Performance SAD process reduces N2O emissions by ~96% compared to heterotrophic denitrification, and CO₂ is not produced as a direct result; instead, CO₂ is fixed by SOB for biomass synthesis, enabling potential negative carbon emissions.
So what. Facilities targeting greenhouse gas reduction should adopt SAD as a primary nitrogen removal stage, especially when coupling with anammox to further suppress nitrite accumulation and N2O formation.
Threshold Sulfate production in SAD is a critical secondary pollution issue: S²⁻-driven SAD produces 4.07 g SO₄²⁻–S/g NO₃⁻–N and S⁰-driven SAD produces 2.51 g SO₄²⁻–S/g NO₃⁻–N; concentrations >400 mg SO₄²⁻–S/L stress aquatic ecosystems and can be reduced to H₂S under anaerobic conditions.
So what. Operators must monitor and limit sulfate accumulation by coupling SAD with anammox or sulfammox, or by post-treatment sulfate removal, to prevent ecosystem damage and odor/corrosion issues.
Opportunity areas6
Specific gaps in this paper, with an experiment that would close each.
High No quantitative operating windows provided for cathode potential, anode potential, or current density in photoelectrotrophic denitrification (PEDeN) systems; paper mentions PEDeN as 'emerging' but provides no electrochemical parameters, pH ranges, or HRT values.
Section 1 and abstract highlight PEDeN as a key emerging technology, but the body text (truncated at 32,000 chars) does not contain detailed electrochemical operating conditions, suggesting this section was cut off or underdeveloped.
Try. Vary cathode potential (-0.4 to -1.0 V vs. Ag/AgCl), anode potential (0 to +0.8 V), current density (0.5–5 A/m²), pH (6–8), and HRT (4–24 h) in a photoelectrotrophic denitrification reactor; measure NO₃⁻ removal, N₂O selectivity, and electron recovery.
High No systematic comparison of N2O accumulation risk across SAD, HAD, and n-DAMO under varying C/N ratios, dissolved oxygen, or catholyte pH; paper states SAD reduces N2O by 96% but does not specify operating conditions (HRT, temperature, influent NO₃⁻ concentration) under which this is achieved.
Section 2.1 claims N2O reduction but does not provide the operating window (e.g., HRT, C/N, DO, pH) that ensures this performance; Section 3 and 4 do not quantify N2O or nitrite accumulation risk.
Try. Test SAD, HAD, and n-DAMO reactors at C/N ratios of 2–10, HRTs of 4–48 h, influent NO₃⁻–N of 50–500 mg/L, and pH 6.5–8.5; measure N2O, NO₂⁻, and N2 production rates to define safe operating windows.
Medium Nitrite accumulation risk in PN-n-DAMO-anammox is mentioned qualitatively ('does not have excessive nitrate accumulation') but no quantitative threshold or control strategy is provided; no data on NO₂⁻ concentration limits or feedback control.
Section 4.1 states nitritation-n-DAMO 'does not have excessive nitrate accumulation and N2O emission' but provides no numbers, setpoints, or control logic for maintaining stable nitrite levels.
Try. Operate PN-n-DAMO-anammox at varying aeration rates (0.5–2 kg O₂/kg N) and measure steady-state NO₂⁻ concentration; define the maximum tolerable NO₂⁻ level before n-DAMO or anammox inhibition occurs.
Medium No data on the effect of temperature on HAD or n-DAMO kinetics and H₂ or CH₄ solubility; paper mentions 10 °C stability for n-DAMO but does not compare performance across 5–35 °C range or provide activation energy estimates.
Section 4.1 reports 10 °C performance for n-DAMO but does not systematically vary temperature; Section 3 does not address temperature effects on H₂ solubility or HAD kinetics.
Try. Operate HAD and n-DAMO reactors at 5, 10, 15, 20, 25, and 30 °C; measure denitrification rate, H₂/CH₄ solubility, and microbial community composition to define optimal temperature windows.
Medium Sulfammox process is mentioned as a method to reduce sulfate production in SAD but is described as 'limited and remains at the proof-of-concept stage'; no pilot or full-scale data provided, and no comparison of sulfammox performance under varying S/N ratios or HRTs.
Section 2.3 states 'sulfammox is limited and remains at the proof-of-concept stage' but provides no quantitative performance data, operating windows, or engineering design criteria.
Try. Operate a SAD-sulfammox coupled reactor at S/N ratios of 0.5–2.0 and HRTs of 8–48 h; measure sulfate production, ammonia oxidation rate, and nitrite accumulation to establish design guidelines.
Medium No comparison of electron recovery or coulombic efficiency in MEC-based HAD systems (MEC-MBfR, MEC-PRB) versus standalone HAD or heterotrophic denitrification; paper reports total nitrogen removal but not energy efficiency or electron balance.
Table 2 reports nitrogen removal efficiency (>90%, 97.8%, 80.6%, 85%) but does not provide cathode potential, current density, applied voltage, or coulombic efficiency, making it impossible to assess energy cost per kg N removed.
Try. Operate MEC-MBfR at applied voltages of 0.5–2.0 V and measure cathode potential, current density, H₂ production rate, and nitrogen removal rate; calculate coulombic efficiency and energy cost per kg NO₃⁻–N removed.
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Abstract
Abstract Wastewater treatment plants are the major energy consumers and significant sources of greenhouse gas emissions, among which biological nitrogen removal of wastewater is an important contributor to carbon emissions. However, traditional heterotrophic denitrification still has the problems of excessive residual sludge and the requirement of external carbon sources. Consequently, the development of innovative low-carbon nitrate removal technologies is necessary. This review outlines the key roles of sulfur autotrophic denitrification and hydrogen autotrophic denitrification in low-carbon wastewater treatment. The discovered nitrate/nitrite dependent anaerobic methane oxidation enables sustainable methane emission reduction and nitrogen removal by utilizing available methane in situ . Photosynthetic microorganisms exhibited a promising potential to achieve carbon-negative nitrate removal. Specifically, the algal-bacterial symbiosis system and photogranules offer effective and prospective low-carbon options for nitrogen removal. Then, the emerging nitrate removal technology of photoelectrotrophic denitrification and the underlying photoelectron transfer mechanisms are discussed. Finally, we summarize and prospect these technologies, highlighting that solar-driven biological nitrogen removal technology is a promising area for future sustainable wastewater treatment. This review has important guiding significance for the design of low-carbon wastewater treatment systems.
Keywords
Identifiers
- Journal
- Frontiers of Environmental Science & Engineering
- Year
- 2024
Reported parameters
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