Alkaline peroxide generation using a novel perforated bipole trickle-bed electrochemical reactor

A novel perforated bipole trickle-bed electrochemical reactor is investigated for the electro-synthesis of alkaline peroxide. The process uses a relatively simple cell configuration in which a single electrolyte flows with oxygen gas in a flow-by graphite felt cathode, sandwiched between a micro-porous diaphragm and a perforated bipolar electrode plate. The graphite felt cathodes are 120 mm high by 25 mm wide and have a thickness of 3.2 mm. The reactor is operated at current densities in the range 1–5 kA m⁻², ca. 800 kPa (abs) pressure and temperature (In/Out) 20–45 °C with one and two-cells. The reactor shows good performance (current efficiency ∼78% at 2 kA m⁻² and a specific energy of 5 kWh per kg of peroxide generated) with peroxide concentrations from 0.02 to 0.15 M in 1 M NaOH.     

Scale-up of the perforated bipole trickle-bed electrochemical reactor for the generation of alkaline peroxide

This paper reports work on the scale-up of a perforated bipole trickle-bed electrochemical reactor for the electro-synthesis of alkaline peroxide. The reactor uses a relatively simple cell configuration in which a single electrolyte flows with oxygen gas in a flow-by graphite felt cathode, sandwiched between a microporous polyolefin diaphragm and a nickel mesh/perforated Grafoil anode/bipole. Both one and two-cell reactors are scaled-up from cathode dimensions 120 mm high by 25 mm wide and 3.2 mm thick (reactor-A) to 630 mm high by 40 mm wide and 3.2 mm thick (reactor-B). The scale-up is achieved by the use of constrictions that prevent segregation of the 2-phase flow in the larger cell, combined with switching from a polypropylene to a polyethylene diaphragm with improved transport properties and raising the electrolyte feed concentration from 1 to 2 M NaOH.For the one-cell reactor-B with a polypropylene diaphragm, operating on a feed of 1 M NaOH and oxygen at 900 kPa(abs)/20 °C, the peroxide current efficiency at a superficial current density of 5 kA m⁻² increases from 27% (un-constricted cathode) to 57% with a constricted cathode. The corresponding current efficiencies at 3–5 kAm⁻² for reactor-A and the constricted reactor-B are respectively 69–64% and 66–57%. Under similar conditions at 3–5 kA m⁻² the one-cell constricted reactor-B with a polyethylene diaphragm gives current efficiencies of 88–64%, and changing to an electrolyte of 2 M NaOH raises this range to 90–80%. At 3–5 kA m⁻² the equivalent two-cell (bipolar) constricted reactor-B shows current efficiencies of 82–74% and at 5 kA m⁻² obtains 0.6 M peroxide in 2 M NaOH with specific energy 6.5 kWh per kg H₂O₂.     

Multiple steady-states for the oxidation of aqueous ethanol with oxygen on a carbon supported platinum catalyst

The selective oxidation of aqueous ethanol by dioxygen over a platinum on carbon catalyst was investigated in a three-phase continuously stirred tank reactor at a total pressure of 600 kPa, a temperature of 323 K, a pH of 8.4, and a catalyst concentration of 2.3 kg m^–3. Multiple steady-states were obtained by systematic changes in the start-up procedure and variation of the feed concentration of ethanol and partial oxygen pressure in the reactor. The ethanol feed concentration was varied from 100 to 2500 mol m^–3 and the partial oxygen pressure from 8 to 120 kPa. On the time scale of the experiments, i.e. 21 ks, two steady-states of the net disappearance rate of ethanol are observed in the ethanol feed concentration range from 500 to 2500 mol m^–3 at a partial oxygen pressure of 58 kPa and in the range of partial pressure of oxygen from 8 to 120 kPa at an ethanol feed concentration of 500 mol m^–3. Three steady-states are observed in the feed ethanol concentration range from 200 to 400 mol m^–3 and a partial oxygen pressure of 58 kPa.     

High Performance Activated Carbon/Carbon Cloth Cathodes for Microbial Fuel Cells

Replacing precious metal catalysts by inexpensive activated carbon (AC) is a breakthrough in microbial fuel cell (MFC) cathode fabrication. In this study, AC powders made from bamboo, peat, coal, coconut, and hardwood sources are evaluated in terms of their electrochemical performance with carbon cloth as the base material. These ACs are characterized in terms of their conductivity, surface chemistry, surface area, and pore size distribution. The bamboo‐based AC demonstrates the highest potential for use as a catalyst for carbon cloth based cathode, reaching 10.6 A m⁻² at 0V vs. Ag/AgCl and a loading of 25 mg cm⁻². The maximum power density reached 3.3 W m⁻² in CEA–MFCs. The high performance of the bamboo‐based AC cathode was possible due to the good conductivity and suitable surface chemistry of the bamboo AC and the high surface area of the base material. The hydrostatic pressure tolerance of the AC carbon cloth cathode is greater than 1.8 m, allowing for a more versatile cathode, suitable for use in many different reactor configurations.     

Sustained nitrite accumulation in a membrane‐assisted bioreactor (MBR) for the treatment of ammonium‐rich wastewater

A membrane‐assisted bioreactor (MBR) for sustained nitrite accumulation is presented, treating a synthetic wastewater with total ammonium nitrogen (TAN) concentrations of 1 kg N m^?3 at a hydraulic retention time down to 1 day. Complete biomass retention was obtained by microfiltration with submerged hollow fibre membranes. A membrane flux up to 189.5 dm³ day^?1 m^?2 could be maintained at a suction pressure below 100 kPa. Nitrification was effectively blocked at the nitrite stage (nitritation), and nitrate concentration was less than 29 g N m^?3. The rate of aeration was reduced to obtain a mixture of ammonium and nitrite, and after adjusting this rate the TAN/NO₂‐N ratio in the reactor effluent was kept around unity, making it suitable for further treatment by anaerobic oxidation of ammonium with nitrite. After increasing again the rate of aeration, complete nitrification to nitrate recovered after 11 days. It is suggested that nitrite accumulation resulted from a combination of factors. First, the dissolved oxygen (DO) concentration in the reactor was always limited with concentrations below 0.1 g DO m^?3, thereby limiting nitrification and preventing significant nitrate formation. The latter is attributed to the fact that ammonium‐oxidising bacteria cope better with low DO concentrations than nitrite oxidisers. Second, the MBR was operated at a high ammonia concentration of 7–54 g N m^?3, resulting in ammonia inhibition of the nitrite‐oxidising microorganisms. Third, a temperature of 35 °C was reported to yield a higher maximum growth rate for ammonium‐oxidising bacteria than for nitrite‐oxidising bacteria. Nitrite oxidisers were always present in the MBR but were out‐competed under the indicated process conditions, which is reflected in low concentrations of nitrate. Oxygen limitation was shown to be the most important factor to sustain nitrite accumulation. Nevertheless, nitritation was possible at ambient temperature (22–24 °C), lower ammonia concentration (<7 g N m^?3) and when using raw nitrogenous wastewater containing some biodegradable carbon. Overall, application of the MBR for nitritation was shown to be a reliable technology. © 2003 Society of Chemical Industry     

Development of a continuous reactor for the electro-reduction of carbon dioxide to formate – Part 2: Scale-up

This paper reports experimental and modeling work for the laboratory scale-up of continuous “trickle-bed” reactors for the electro-reduction of CO₂ to potassium formate. Two reactors (A and B) were employed, with particulate tin 3D cathodes of superficial areas, respectively, 45 × 10⁻⁴ (2–14 A) and 320 × 10⁻⁴ m² (20–100 A). Experiments in Reactor A using granulated tin cathodes (99.9 wt% Sn) and a feed gas of 100% CO₂ showed slightly better performance than that of the tinned-copper mesh cathodes of our previous communications, while giving substantially improved temporal stability (200 vs. 20 min). The seven-fold scaled-up Reactor B used a feed gas of 100% CO₂ with the aqueous catholyte and anolyte, respectively [0.5 M KHCO₃ + 2 M KCl] and 2 M KOH, at inlet pressure from 350 to 600 kPa(abs) and outlet temperature 295 to 325 K. For a superficial current density of 0.6–3.1 kA m⁻² Reactor B achieved corresponding formate current efficiencies of 91–63%, with the same range of reactor voltage as that in Reactor A (2.7–4.3 V), which reflects the success of the scale-up in this work. Up to 1 M formate was obtained in the catholyte product from a single pass in Reactor B, but when the catholyte feed was spiked with 2–3 M potassium formate there was a large drop in current efficiency due to formate cross-over through the Nafion 117 membrane. An extended reactor (cathode) model that used four fitted kinetic parameters and assumed zero formate cross-over was able to mirror the reactor performance with reasonable fidelity over a wide range of conditions (maximum error in formate CE = ±20%), including formate product concentrations up to 1 M.     

Enhancing completely autotrophic nitrogen removal over nitrite by trace NO2 addition to an AUSB reactor

BACKGROUND: Completely autotrophic nitrogen removal over nitrite (CANON) could decrease energy consumption and CO₂ release compared with conventional nitration–denitrification. Trace NO₂ addition could enhance the activities of aerobic and anaerobic ammonium oxidation. RESULTS: An aerated upflow sludge bed (AUSB) reactor inoculated simultaneously with aerobic and anaerobic ammonium oxidizing sludge was operated to cultivate granular sludge capable of carrying out CANON. The results showed that the efficiency and rate of total nitrogen (TN) removal reached 61% and 0.114 kgN, respectively (m^?3 day^?1) for DO = 0.5–0.6 mg L^?1. Batch tests indicated that trace NO₂ addition could increase the CANON activity of sludge. The TN removal rate and efficiency of the reactor was increased to 0.234 kgN m^?3 day^?1 and 63%, respectively, when the reactor was aerated with air containing 2.7–3.3 mmol m^?3 NO₂ and DO was at 0.5–0.8 mg L^?1. CONCLUSIONS: Trace NO₂ addition provides an alternative to increase the capacity of a CANON system at low DO concentration. Copyright © 2009 Society of Chemical Industry     

Development of a continuous reactor for the electro-reduction of carbon dioxide to formate – Part 1: Process variables

This paper reports an experimental investigation into the effects of five process variables on the performance of a bench-scale continuous electrochemical reactor used in the reduction of CO₂ to potassium formate, and interprets the data in terms of reactor engineering for a (speculative) industrial process for electro-reduction of CO₂. The process variables: temperature, catholyte species, catholyte conductivity, cathode specific surface area and cathode thickness were studied, along with CO₂ pressure and current density, in a set of factorial and parametric experiments aimed to unravel their main effects and interactions. These variables showed complex interdependent effects on the reactor performance, as measured by the current efficiency and specific energy for generation of formate (HCO₂⁻). The “best” result has a formate current efficiency of 86% at a superficial current density of 1.3 kA m⁻², with a product solution of 0.08 m KHCO₂ and specific electrochemical energy of 260 kWh per kmole formate. The combined results indicate good prospects for process optimization that could lead to development of an industrial scale reactor.     

The Electro-Reduction of Carbon Dioxide in a Continuous Reactor

This paper reports an investigation into the electro-reduction of CO₂ in a laboratory bench-scale continuous reactor with co-current flow of reactant gas and catholyte liquid through a flow-by 3D cathode of 30^# mesh tinned-copper. Factorial and parametric experiments were carried out in this apparatus with the variables: current (1–8 A), gas phase CO₂ concentration (16–100 vol%) and operating time (10–180 min), using a cathode feed of [CO₂ + N₂] gas and 0.45 m KHCO₃(aq) with an anolyte feed of 1 m KOH(aq), in operation near ambient conditions (ca. 115 kPa(abs), 300 K). The primary and secondary reactions here were respectively the reduction of CO₂ to formate (HCOO⁻) and of water to hydrogen, while up to ca. 5% of the current went to production of CO, CH₄ and C₂H₄. The current efficiency for formate depended on the current density and CO₂ pressure, coupled with the hydrogen over-potential plus mass transfer capacity of the cathode, and decreased with operating time, as tin was lost from the cathode surface. For superficial current densities ranging from 0.22 to 1.78 kA m⁻², the measured values of the performance indicators are: current efficiency for HCOO⁻ = 86–13%, reactor voltage = 3–6 Volt, specific energy for HCOO⁻ = 300–1300 kWh kmol⁻¹, space-time yield of HCOO⁻ = 2 × 10⁻⁴–6 × 10⁻⁴ kmol m⁻³ s⁻¹, conversion of CO₂ = 20–80% and yield of organic products from CO₂ = 6–17%.     

Preparation,characterization, and performance evaluation of LTA zeolite–ceramic composite membrane by separation of BSA from aqueous solution

Using low-cost clay supports as substrates, ceramic–LTA zeolite composite membranes (Z1–Z4) were fabricated with hydrothermal crystallization. The composite membranes were achieved with variations in the sequential zeolite depositional steps. For Z1–Z4 membranes, various characterization techniques such as thermogravimetric (TG), particle size distribution (PSD), X-ray diffraction (XRD), and field emission scanning electron microscopic (FE-SEM) analysis were applied. For the Z1–Z4 membranes, the pure water permeability, porosity, and average pore size varied from 1.22 × 10^?7 to 1.19 × 10^?8 m³/m²s kPa, 30–23%, and 215–76 nm, respectively. For the Z4 membrane, ultrafiltration experiments were conducted at a pH of 2.5 and transmembrane pressure differential of 207 kPa using aqueous bovine serum albumin (BSA) solutions. The optimal flux and rejection correspond to 4.54 × 10^?7 m³/m²s and 80%, respectively.     

Removal of cadmium and production of cadmium powder using a continuous undivided electrochemical reactor with a rotating cylinder electrode

The behaviour of a continuous undivided electrochemical reactor with a rotating cylinder electrode under potentiostatic control is examined for the abatement of cadmium from synthetic sodium sulfate solutions with Cd(II) concentrations lower than 500 mg dm^?3 at a reactor inlet pH ? 7. The process was designed to convert the metal ions in solution to metal powder, which settles to the conical of the reactor and may be removed at intervals as a sludge by opening a drop valve. The effect of applied potential, inlet cadmium concentration, rotation speed and hydrogen evolution as side cathodic reaction on the ‘figures of merit’ of the reactor are analysed. The best results were obtained for cathode potentials in the range from ?0.9 V to ?1.0 V against the saturated calomel electrode. Therefore, when the rotation speed was 1000 rpm the space time yield and the normalized space velocity were 0.64 ×10^?2 mol m^?3 s^?1 and 0.89 h^?1 respectively, while the fractional conversion per pass was 35% with a current efficiency higher than 74%. The surface morphology of the deposits as a function of the process variables is also reported. © 2002 Society of Chemical Industry     

Vapour permeation applied for the separation of water from organic compounds and gases using asymmetric polyetherimide/polyvinylpyrrolidone capillary tubes

Asymmetric integrally skinned capillary tubes were produced from the polymers PEI (polyetherimide) and PVP (polyvinylpyrrolidone) for vapour permeation modules which were applied for the separation of water from organic compounds and gases. Water treatment and recovery of desirable organic compounds was achieved. The capillary tubes had intrinsic permeability coefficients of 7.5 × 10^?7 mol/m²·s·Pa for water and 1.6 × 10^?9 mol/m²·s·Pa for 1-propanol for a 1:1 mass ratio vapour feed mixture under pyrolysis conditions. The vapour was fed at the interior of the capillary tubes with total pressure of 30 kPa; the permeate total pressure was 14 kPa, and the temperature was 86°C. Modules, with surface areas up to 1.0 m², were constructed and tested with feed flow rates as high as 4 kg/h with a process development unit. Tests were performed with the vapours from wood chips and contaminated soils subjected to vacuum pyrolysis.     

Wet oxidation pre‐treatment of woody yard waste: parameter optimization and enzymatic digestibility for ethanol production

Woody yard waste with high lignin content (22% of dry matter (DM)) was subjected to wet oxidation pre‐treatment for subsequent enzymatic conversion and fermentation. The effects of temperature (185–200 °C), oxygen pressure (3–12 bar) and addition of sodium carbonate (0–3.3 g per 100 g DM biomass) on enzymatic cellulose and hemicellulose (xylan) convertibility were studied. The enzymatic cellulose conversion was highest after wet oxidation for 15 min at 185 °C with addition of 12 bars of oxygen and 3.3 g Na₂CO₃ per 100 g waste. At 25 FPU (filter paper unit) cellulase g^?1 DM added, 58–67% and 80–83% of the cellulose and hemicellulose contained in the waste were converted into monomeric sugars. The cellulose conversion efficiency during a simultaneous saccharification and fermentation (SSF) assay at 10% DM was 79% for the highest enzyme loading (25 FPU g^?1 DM) while 69% conversion efficiency was still reached at 15 FPU g^?1 DM. Total carbohydrate recoveries were high (91–100% for cellulose and 72–100% for hemicellulose) and up to 49% of the original lignin and 79% of the hemicellulose could be solubilized during wet oxidation treatment and converted into carboxylic acids mainly (total carboxylic acids = 3.1–7.4% on DM basis). Copyright © 2004 Society of Chemical Industry     

Oxygen and water vapor gas barrier poly(ethylene naphthalate) films by deposition of SiOx plasma polymers from mixture of tetramethoxysilane and oxygen

SiO_x films were deposited from a mixture of tetramethoxysilane (TMOS) and oxygen on poly(ethylene 2,6‐naphthalate) film using ion‐assisted plasma polymerization technique (Method II) and conventional plasma polymerization technique (Method I), and were compared in chemical composition and gas barrier properties. Methods I and II were different in electrical circuit between electrodes (anode and cathode) and electric power supply. In Method I, the anode electrode was grounded, and the cathode electrode was coupled to the discharge power supply. In Method II, the anode electrode was connected with the discharge power supply, and the cathode electrode was grounded. There was not large difference in SiO_x deposition rate between the plasma polymerizations by Methods I and II. Plasma polymers deposited from TMOS/O₂ mixtures by Method II possessed smaller C/Si and O/Si atomic ratios than those deposited by Method I and showed advantage in gas barrier properties. The oxygen and water vapor permeation rates were 0.08–0.13 cm³ m^?2 day^?1 atm^?1 at 30°C at 90% RH and 0.244–0.276 g m^?2 day^?1 at 40°C at 90% RH, respectively. From these results, it can be concluded that the ion‐assisted plasma polymerization is a useful technique for deposition of gas barrier SiO_x thin films. © 2007 Wiley Periodicals, Inc. J Appl Polym Sci 104: 915–925, 2007     

New electrodes for oxygen evolution in acidic solution

Conventional electrowinning of metals such as zine and copper from 1–1.5 kmol m^–3 H₂SO₄ electrolytes involves anodic oxygen evolution at Pb alloy/PbO₂ anodes operating at 200–800 A m^–2. The oxygen overpotential, estimated to be about 0.6 V, constitutes a significant proportion of the cell voltage (typically 2.5 V for Cu and 3.3 V for Zn). The objective of this work was to lower the anode overpotential and so decrease the process specific energy requirements, by devising new anode materials based on: (1) PTFE-bonded PbO₂ catalysts, supported on Pb–Ag alloys; (2) modification of the pore structure of porous electrodes to maximize the utilization of the available surface without the use of PTFE bonding. Both methods are shown to produce significant benefits in lowering oxygen overpotentials, though the latter technique has been tested only in alkaline electrolytes, as yet. However, with the former approach, substrate oxidation through the porous catalyst layer has been found to cause catalyst shedding after>60 h at 1 kA m^–2, though careful pre-oxidation of the anode substrate appears to extend the anode life.Paper presented at the 2nd International Symposium on Electrolytic Bubbles organized jointly by the Electrochemical Technology Group of the Society of Chemical Industry and the Electrochemistry Group of the Royal Society of Chemistry and held at Imperial College, London, 31st May and 1st June 1988.     

Effect of temperature on the performance of microbial fuel cells

Single and double chamber microbial fuel cells (MFCs) were tested in batch mode at different temperatures ranging from 4 to 35 °C; results were analysed in terms of efficiency in soluble organic matter removal and capability of energy generation. Brewery wastewater diluted in domestic wastewater (initial soluble chemical oxygen demand of 1200 and 492 mg L⁻¹ of volatile suspended solids) was the source of carbon and inoculum for the experiments. Control reactors (sealed container with support for biofilm formation) as well as baseline reactors (sealed container with no support) were run in parallel to the MFCs at each temperature to assess the differences between water treatment including electrochemical processes and conventional anaerobic digestion (in the presence of a biofilm, or by planktonic cells). MFCs showed improvements regarding rate and extent of COD removal in comparison to control and baseline reactors at low temperatures (4, 8 and 15 °C), whilst differences became negligible at higher temperatures (20, 25, 30 and 35 °C). Temperature was a crucial factor in the yield of MFCs both, for COD removal and electricity production, with results that ranged from 58% final COD removal and maximum power of 15.1 mW m⁻³ reactor (8.1 mW m⁻² cathode) during polarization at 4 °C, to 94% final COD removal and maximum power of 174.0 mW m⁻³ reactor (92.8 mW m⁻² cathode) at 35 °C for single chamber MFCs with carbon cloth-based cathodes. Bioelectrochemical processes in these MFCs were found to have a temperature coefficient, Q10 of 1.6.A membrane-based cathode configuration was tested and gave promising results at 4 °C, where a maximum power output of 294.6 mW m⁻³ reactor (98.1 mW m⁻² cathode) was obtained during polarization and a maximum Coulombic efficiency (Y_Q) of 25% was achieved. This exceeded the performance at 35 °C with cloth-based cathodes (174.0 mW m⁻³; Y_Q 1.76%).     

Hydrogen peroxide production in trickle-bed electrochemical reactors

A trickle bed electrochemical reactor has been developed for the production of dilute alkaline peroxide solutions by reduction of oxygen. Oxygen gas and sodium hydroxide flow concurrently downward through a cell which consists of a thin packed cathode bed of graphite particles separated from the anode plate by a porous diphragm. Current flows perpendicular to the flow of electrolyte. The effects of current density, oxygen pressure and flow rate, electrolyte concentration and flow rate, graphite particle size, bed thickness and length were investigated. In 2 M NaOH peroxide solutions of 0.8 M have been produced at 60% efficiency with current densities of 1200 A m^–2 and cell voltages of 1.8 V. A bipolar cell stack consisting of five cells has been tested.     

BDD anodic oxidation as tertiary wastewater treatment for the removal of emerging micro‐pollutants,pathogens and organic matter

This work reports for the first time the removal of 17α‐ethynylestradiol (EE2), a synthetic estrogen hormone, from secondary treated effluents by electrochemical oxidation. Experiments were conducted in a single compartment reactor comprising a boron‐doped diamond (BDD) anode and a zirconium cathode. EE2, in the range 100–800 µg L^?1, was spiked in the post‐chlorination effluent of a municipal treatment plant and oxidized at 0.9–2.6 mA cm^?2 current density. Complete degradation of 100 µg L^?1 EE2 was achieved in 7 min at 2.1 mA cm^?2 and inherent conditions, while the addition of 0.1 mol L^?1 NaCl achieved removal in just a few seconds. The process was then tested in the pre‐chlorination effluent at 2.1 mA cm^?2 and inherent conditions; complete E. coli killing and EE2 removal occurred in just 1.5 and 3.5 min, respectively, while overall estrogenicity (assessed by the YES assay) and residual organic matter (in terms of chemical oxygen demand (COD)) decreased by 50% and 85% after 30 min, respectively. These results clearly show the potential of BBD electrochemical oxidation to serve as an efficient tertiary wastewater treatment. Copyright © 2011 Society of Chemical Industry     

Removal of Arsenic from Wastewaters by Airlift Electrocoagulation. Part 1: Batch Reactor Experiments

Abstract

Arsenic removal from wastewater is a key problem for copper smelters. This work shows results of electrocoagulation in aqueous solutions containing arsenic in a newly designed and constructed 1 L batch airlift reactor. Iron electrodes were used in the cell. The airlift electrocoagulation reactor allowed simultaneously a) anodic Fe²⁺ production, b) Fe²⁺ to Fe³⁺ oxidation by air or oxygen, and c) precipitate/coagulate formation due to the turbulent conditions in the cell. A series of electrocoagulation experiments were carried out in the batch airlift reactor. The variables were: initial As(V) concentration, use of either a pure oxygen or an air flow, and electric current density. The results showed that the airlift electrocoagulation process could reduce an initial As concentration from 1000 mg L^?1 to 40 mg L^?1–corresponding to a reduction of 96%. At higher initial concentrations (e.g. 5000 mg L^?1 As) the oxidation of Fe²⁺ to Fe³⁺ seems to be rate determining. Oxidation with compressed oxygen was clearly more efficient than air at high initial As concentration. Arsenate removal from a solution with initially 100 mg L^?1 was efficient with both air and oxygen addition–more than 98% of As precipitated. When the electrocoagulation process was working efficiently, the arsenic removal rate in the cell was found to be around 0.08–0.1 mg As/C. The Fe‐to‐As (mol/mol) ratio, when electrocoagulation was working properly, was in the range of 4–6.