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Volume 10, Number 2 (January 2023):4119-4127, doi:10.15243/jdmlm.2023.102.4119 ISSN: 2339-076X (p); 2502-2458 (e), www.jdmlm.ub.ac.id

Open Access 4119 Research Article

Ecological assessment of different electrokinetic remediation strategies:

a pilot scale study

Yudith Vega Paramitadevi1*, Beata Ratnawati1, Agus Jatnika Effendy2, Syarif Hidayat2, Mochamad Arief Budihardjo3, Bimastyaji Surya Ramadan3, Dimas Ardi Prasetya1, Ivone Wulandari Budiharto1

1 The Vocational Studies of IPB University, Kumbang 14th Street, Bogor, Indonesia

2 Bandung Institute of Technology, Ganesha 10th Street, Bandung, Indonesia

3 Diponegoro University, Prof. Sudharto Street (Shared College Building), Semarang, Indonesia

*corresponding author: yudith.vega@apps.ipb.ac.id

Abstract Article history:

Received 2 September 2022 Accepted 22 October 2022 Published 1 January 2023

The electrokinetic remediation method can function as a primary or secondary technology and can be applied in conjunction with other physical and biological methods, such as soil washing, phytoremediation, and bioremediation. Environmental impacts arising from the electrokinetic remediation process can be determined using life cycle assessment analysis (LCA) or other tools. This study compared the conventional electrokinetic remediation strategy with two hybrid strategies: electrokinetic- phytoremediation (EKR-Phyto) and electrokinetic-bioremediation (EKR- Bio). The environmental performance of the three strategies is then tested through LCA analysis. The database used was The Ecoinvent, and the freeware software used during the inventory stage was OpenLCA. The impact assessment stage was used in the Recipe I (2016) midpoints, Available Water Remaining (AWARE) midpoint, Intergovernmental Panel Climate Change (IPCC) midpoint (2003), UNEP Society of Environmental Toxicology (USEtox) midpoint, and cumulative energy demand midpoint.

The significance of the analysis results was not obtained for the GWP parameter but for the freshwater eutrophication parameter. Among the three strategies, the EKR-Phyto strategy showed the highest significance in eutrophication but the lowest significance in land change. Substitution of chemical fertilizers into natural fertilizers in the EKR-Phyto strategy can be an opportunity for environmental sustainability. The highest impact for ecological analysis of the three strategies was EKR-Phyto in terms of GWP, the sum of primary energy, Acidification Potential (AP), and Photochemical Ozone Creation Potential (POCP).

Keywords:

b&v analysis

ecological assessment electrokinetic remediation life cycle assessment open LCA

To cite this article: Paramitadevi, Y.V., Ratnawati, B., Effendy, A.J., Hidayat, S., Budihardjo, M.A., Ramadan, B.S., Prasetya, D.A. and Budiharto, I.W. 2023. Ecological assessment of different electrokinetic remediation strategies: a pilot scale study.

Journal of Degraded and Mining Lands Management 10(2):4119-4127, doi:10.15243/jdmlm.2023.102.4119.

Introduction

Heavy metals originating from industrial waste can accumulate in the soil or sediments to impact environmental pollution and decrease human health (Dobrescu et al., 2022). Lead is a heavy metal that is

persistent and difficult to remove (Zhang et al., 2013), able to seep into the aquifer and contaminate the groundwater media (Ferruci et al., 2017). Efforts to remove lead can be made through remediation, including solidification - stabilization, phytoremediation, and leaching (Hou and O'Connor,

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Open Access 4120 2020). Some removal technologies have technical

weaknesses, such as long removal times. They are not suitable to be applied to soils with low permeability, resulting in which economic and social sustainability is not achieved (Vocciante et al., 2016).

A reliable remediation technique that can be applied together with other technologies is electrokinetic remediation. Electrokinetic remediation (EKR) has been applied worldwide, involving the laboratory scale to full scale through electromigration, electroosmosis, and electrophoresis processes (Mao et al., 2019). Although the EKR technique can remove the lead metal in the soil, the process can impact the environment (Kim et al., 2014). The use of electricity, clean water, electrolytes and electrodes, and supporting materials for operational processes causes emissions and water pollution, affecting the ecological conditions around the remediation area. Thus, it is crucial to evaluate the environmental footprint.

The initial environmental footprint evaluation was in green and sustainable remediation developed by the US EPA and European Union countries, including assessing environmental, social, and economic aspects based on a qualitative approach (Yasutaka et al., 2016). Qualitative tools then developed into semi- qualitative in the form of life cycle assessment (LCA) or other forms such as hybrid-LCA, Input-Output (I- O) LCA analysis by Hou and O'Connor (2020), and footprint tools developed by other countries (The green remediation assessment tool for Japan/GRAT-J, Quantitative Assessment of Life Cycle Sustainability/

QUALICS and others). LCA tools can be applied to various remediation technologies, areas, and processes (Vicentin et al., 2019). The application of LCA has been applied to various scales of remediation reactors, specifically for the pilot scale; the analysis carried out is mainly in the form of indicators of climate change (Favara et al., 2011; Piccinno et al., 2016; Braun et al., 2020); evaluation of remediation, especially EKR, of ecological impacts using LCA is still rarely done (Amponsah et al., 2018; Vicentin et al., 2019).

EKR techniques can be combined with phytoremediation techniques (EK-Phyto) and bioremediation techniques (EK-Bio) (Gill et al., 2016;

Wanitsawatwichai and Sampanpanish, 2021).

Vocciante et al. (2021) have conducted full-scale LCA studies for landfill excavation, disposal, soil washing, EKR, and phytoremediation; however, the LCA analysis for the combination of remediation techniques is still very little done.

The purposes of this study were: (1) to compare the results of life cycle inventory analysis (LCIA) between three combinations of strategies and (2) to evaluate the ecological impact of the reactor combination with the lowest LCA yield using b&v analysis. The b&v analysis is a single assessment evaluation system based on ecological priorities that take into account total emissions (specific contributions), political targets (distance-to-target),

and potential damage (ecological hazards) (Teuteberg et al., 2019). The designed scenarios were compared through LCA analysis, and then the alternatives were taken through b&v analysis.

Materials and Methods LCA goal and scope

The target for lead removal is deliberately clay exposed to PbNO3 and HNO3 based on research by (Villen-Guzman et al., 2018) until the pollutant concentration reaches 800 mg kg-1. The setting of the reactor and its equipment referred to the research of Risco et al. (2016); the equipment consisted of an EKR reactor, a power supply, and an electrolyte storage tank. The soil volume was 175 x 103 cm3, the length x width x height was 70 x 50 x 50 cm3. Electrodes made of graphite with dimensions of 1 x 1 x 10 cm3 were placed in an electrolyte tank in which an electrode protector was provided, made of nylon fabric. Data loggers were installed to monitor temperature, pH, electricity consumption, electric current (average in the range of 0.3-0.5 A), and humidity.

The material flow came from 185.5 kg of soil that could be processed for two weeks. The results of the pilot-scale analysis showed that the concentration decreased to 419.35-45.4 mg kg-1. Thus, the functional unit used is the recovery of 1 kg of heavy metal contaminated soil (results of normalization of data from 185.5 kg) to set aside the initial concentration of 800 mg kg-1 to 419.35-45.4 mg kg-1. The process was limited only to the core EK process of each technology; for example, conventional EK only discusses the input flow and output material flow. The system constraint (Figures 1, 2 and 3) consisted of three different strategies discussed in the life cycle inventory section.

Life Cycle Inventory (LCI) System analysis

The LCA assessment was carried out under three different scenarios: conventional EKR; EK-Phyto, a combination of EKR with phytoremediation; EKR- Bio, a combination of EKR with bioremediation (Figures 1, 2 and 3). Efforts to prepare plants and bacteria were carried out so that the EKR-Phyto and EKR-Bio processes ran smoothly. Rhizobium spp. was cultured for 14 days and acclimatized for 14 days, placed under aerobic conditions; Cordyline fruticosa (local name, Hanjuang plant) was adapted for 14 days to check plant height, root condition, and leaf blade.

The reference for the conventional EKR process is based on the research of (Villen-Guzman et al., 2018), the reference for the EKR-Phyto and EKR-Bio processes using the principle of polarity reversal (Wang et al., 2021). Polarity reversal reduces shock loading during the remediation process so plants/microbes can survive.

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Open Access 4121 Figure 1. LCA of the EKR procedure.

Figure 2. LCA of the EKR-Phyto procedure.

Figure 3. LCA of the EKR-Bio procedure.

Data collection

All data used in this study were derived from pilot- scale data from EKR, EK-Phyto, and EK-Bio, specifically the input and output product data for energy and products using the Ecoinvent table. The analysis of the uncertainty that arises was taken from Fernández-Marchante et al. (2022).

Impact assessment

The impact evaluation method refers to the research of Fernandez-Marchante et al. (2022), namely the midpoint of ReCiPe v I 2016. In order to find more specific results, IPCC (2003), AWARE, USEtox, and Cumulative Energy Demand methods were added.

These additional methods represent the impacts of climate change, water consumption, toxicology on humans, and energy use. Midpoints analyzed were:

particulate matter formation, freshwater eutrophication, marine eutrophication, ionizing radiation, terrestrial ecotoxicity, agricultural land occupation, climate change, water depletion, natural land transformation, terrestrial acidification, photochemical oxidant formation, marine ecotoxicity, fossil depletion, human toxicity, metal depletion, freshwater ecotoxicity, urban land occupation, non- renewable and ozone depletion. Inventory and impact calculations were carried out using Ms. Excel and Open LCA software version 1.10.3.

Conventional EKR Process Electricity,

Water, EDTA Spiked soil 800 mg Pb kg-1 soil Nylon,

PVC, Electrodes

Emission to air, Contaminated water

Spiked soil

??? mg Pb kg-1 soil

Solid waste

EKR-Phyto Process Electricity,

Water, EDTA Spiked soil 800 mg Pb kg-1 soil Nylon, PVC, Electrodes, C. fructiosa plants

Emission to air, Contaminated water

Spiked soil

??? mg Pb kg-1 soil

Solid waste

EKR-Bio process Electricity,

Water, EDTA Spiked soil 800 mg Pb kg-1 soil Nylon, PVC, Electrodes, Rhizobium sp.

Emission to air, Contaminated water

Spiked soil

??? mg Pb kg-1 soil

Solid waste

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Open Access 4122 b&v analysis

The b&v analysis was previously used for product declarations that were environmentally friendly in terms of ecology. This analysis can also function to review environmentally friendly process units, strengthen the interpretation of the LCA analysis, and can be presented in the LCA interpretation stage (Figure 4). The b&v model is easier to understand by non-specialists with a more straightforward validity test (Teuteberg et al., 2019). The b&v analysis and its procedures were taken from Teuteberg et al. (2019);

the main parameters include climate change (GWP), acidification (AP), eutrophication (EP), abiotic depletion, ozone depletion (OD), photochemical

oxidant creation (POCP), total primary energy, and freshwater. The stages in this quantitative b&v analysis are determining the scoring parameters, factor analysis with scoring, and finally, the scoring results will be plotted using a radar diagram. The scoring classification is divided into five: deficient, low, medium, high, and very high impact. The determinants of the b&v analysis are potential for ecological changes, the distance to the target, and the contribution of the specific parameters. The greater the following factors, such as; the number of endpoints affected, forecast of affected people, minor reversal of impact, the magnitude of impact (regional or global), the greater the potential for ecological change (Teuteberg et al., 2019).

Figure 4. b&v single score analysis as part of LCA interpretation stage, adapted from Teuteberg et al. (2019).

The three endpoints that are taken into account include the impact on human health, the impact on the ecosystem, and the reduction of natural resources.

Furthermore, the criteria for the distance to the target will be higher if there is no procedure for reducing or removing pollutants in the remediation area. If there is a significant contribution of parameters in the remediation area, then the parameter has the highest score compared to others. The ecological priority obtained is then presented as a relative number as follows,

F = ∑ f( )+ f( )+. . . + f( ) (1) where:

F = Total of ecological priority, % f(GWP) = Global warming potential, % f(ODP) = Ozone depleted potential, % f(Freshwater) = freshwater potential, % Results

Comparison of material flow data between strategies Table 1 is the input between strategies; all scenarios show the same input for some basic parameters such as electrodes, EDTA, and nylon cloth. The exact magnitude indicates no significant change in the use of natural resources. On the other hand, the difference between the EK-Phyto process and the others is NPK

fertilizer and cordyline plants, thereby generating biomass in the output. Finally, the EK-Bio process requires yeast and molasses so that Rhizobium spp. can reach its optimal phase.

Impact analysis

Comparison between strategies

The consumption of electrical energy in the EKR process does not significantly contribute to GWP and ozone depletion (Table 2). Contributions were found to eutrophication in the use of EDTA as an electrolyte, disposal of electrodes in landfills, and disposal of liquid waste from the EKR process to the environment.

The EKR process is also influenced by the electrodes' location and the electrolyte solution that can accelerate electromigration. If electricity consumption is considered the same, then the primary environmental impact source comes from the materials used (Vocciante et al., 2017). Optimizing the EKR process by reducing the number of electrodes can reduce the environmental impact contribution to eutrophication.

The EKR-Phyto combination has the most significant role in the natural land transformation and freshwater eutrophication (Table 2). The use of fertilizers containing nutrient elements, primarily N and P, affects the impact of freshwater eutrophication. Direct disposal of biomass to landfills also impacts natural land transformation. The effectiveness of the EKR- Phytoremediation combination is excellent from a b&v categories Identification:

- Ecological hazard - Distance-to-target - Specific contribution

Ecological

priority b&v single score Interpretation Stage of LCA

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Open Access 4123 technical point of view, as evidenced by the efficiency

of heavy metal lead removal in a 14-day pilot-scale experiment of 91.41%. However, the environmental impact contributed by the combined EKR and phytoremediation activities is also significant. The EKR-Bioprocess has the lowest impact on freshwater eutrophication and agricultural and urban land occupation. The addition of molasses and yeast as

energy sources for Rhizobium spp. contributed to agricultural and urban land occupation. Furthermore, industries that produce molasses and yeast ingredients can increase the scope of agricultural and industrial land, otherwise known as agroindustry. Similar to the application of EKR-Phyto, the combination of EKR- Bio produces an environmental impact of almost the same magnitude.

Table 1. Input-output data based on pilot-scale measurements for 14 days.

Input Composition Normalized

per activity of EKR

Normalized per activity of EKR-Phyto

Normalized per activity of EKR-Bio

Unit

Spiked soil Initial Pb

concentration

800 800 800 mg kg-1 soil

Electricity Power supply 1708 1813 1855 KWh kg-1

Water Industrial 279.16 280 260.35 kg kg-1

Irrigation - 151.5 - kg kg-1

Electrodes Graphite 0.3 0.3 0.3 kg kg-1

Fertilizer NPK - 0.5 - kg kg-1

EDTA Dosage 2.92 x 10-5 2.92 x 10-5 2.92 x 10-5 kg kg-1

PVC 3/4 inch 0.16 0.16 0.16 kg kg-1

Cordyline fruticosa Plants - 0.93 - kg kg-1

Yeast - - 0.01 kg kg-1

Molasses - - 0.5 kg kg-1

Cloth Fiber woven, 0.17

mm

0.125 0.125 0.125 kg kg-1

Output

Spiked soil Final Pb

concentration 419.35 45.4 380.15 mg kg-1 soil

Contaminated water 274.11 304.00 208.2 kg kg-1

Solid waste 0.285 0.285 0.285 kg kg-1

Biomass - 1.1 - kg kg-1

Process water loss in

soil 5.05 0 0 kg kg-1

When compared between the three strategies, the toxicity of pollutants originating from seawater sources on land and clean water has values close to each other (Table 2). The lowest impact is human toxicity; this is reasonable because the remediation effort is a restoration of the ecological condition, including improving human health in the vicinity. The climate change value for EKR is lower than EK-Bio and EK-Phyto because the amount of input energy is directly used for the electromigration process only, while EK-Bio and EK-Phyto require more energy to complete the metal solubilization process. EK-Bio and EK-Phyto will continue until the electrophoresis process.

Based on the 18 midpoints in Table 2, EK-Bio strategy has the same percentage as EK-Phyto; the EKR strategy has the lowest 55% midpoint value.

When other methods, such as IPCC and Cumulative Energy Demand were used, the same thing was confirmed (Figure 5). Midpoint Recipe I 2016 (Huijbregts et al., 2017) has a positive value for freshwater eutrophication and the possibility of natural

land transformation. Efforts that can be made to reduce eutrophication, especially in the process with the highest midpoint value, are EK-Phyto, and mitigate biomass management. Climate change in GWP has negative values, like human toxicity, water use, and fossil fuels. It happens because the consumption of natural resources is relatively minor compared to full- scale conditions. Despite all the criteria, both the EK- Bio strategy and the EK-Phyto strategy significantly impact ecosystem endpoints, leading to a decline in human health.

Contribution between components

According to the input-output in the electrokinetic process of remediation, the components that contributed to the ecological assessment of the different strategies (Table 3) were the use of nylon as an electrode cap mounted in the well, NPK fertilizer, EDTA, and water for industrial use. The use of nylon is responsible for the impact of freshwater eutrophication on the overall strategy. The nylon material is imported from China and the United States.

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Open Access 4124 Table 2. Impact of midpoints for all scenarios based on ReCiPe method.

Impact Impact result

of EKR

Impact result of EKR + Phyto

Impact result of EKR + Bio

Unit

Particulate matter formation -46.92* -13.83 -28.54 kg PM10-eq

Freshwater eutrophication 0 0 0* kg P-eq

Marine eutrophication -0.48* -0.14 -0.28 kg N-eq

Ionizing radiation -2424.23* -714.45 -1420.58 kg U235-eq

Terrestrial ecotoxicity -5.34* -1.57 -3.13 kg 1.4-DCB-eq

Agricultural land occupation -1.3 -0.39 -1.77* m2a

Climate change -918.61* -268.73 -556.70 kg CO2-eq

Water depletion 0 0 0 m3 water-eq

Natural land transformation 0 0* 0 m2

Terrestrial acidification -200.63* -59.13 -121.56 kg SO2-eq

Photochemical oxidant formation -38.19* -11.24 -23.41 kg NMVOC-eq

Marine ecotoxicity -29.87* -8.8 -18.22 kg 1.4-DCB-eq

Fossil depletion 0 0 0 kg oil-eq

Human toxicity 0 -6836.92* 0 kg 1.4-DCB-eq

Metal depletion 0* 0 0 kg Fe-eq

Freshwater ecotoxicity 0* 0 0 kg 1.4-DCB-eq

Urban land occupation -0.45 -0.13 -0.61* m2

Ozone depletion 0 0* 0 kg CFC-11-eq

*Note: The lowest midpoint value in each strategy.

Figure 5. Midpoint analysis for IPCC (2003) and cumulative energy demand methods.

-1000 -800 -600 -400 -200 0

EKR EKR-Phyto EKR-Bio

GWP 20a, IPCC (2003) kgCO2-eq

0 5 10 15 20 25 30 35 40

EKR EKR-Phyto EKR-Bio

MJ

Non renewable, fossil by Cumulative Energy Demand

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Open Access 4125 Materials such as nylon and PVC cannot be recovered

if they become solid waste. The focus on these two materials is also conveyed in the research of Vocciante et al. (2021); both PVC and geotextile can only be replaced during or after the EKR process takes place.

Consumption of clean water also affects the EKR and EK-Bio strategies. This condition can be an opportunity for improvement in recirculating water in the well or additional processing of contaminated water after the reactor outlet. Organic fertilizers can also replace chemical fertilizers from the EK-Phyto process to reduce the entry of nutrients into water bodies. In the EK-Bio strategy, yeast can be reduced if the number of bacteria in the process is sufficient and the use of EDTA or other solutions can be optimized.

Table 3. Three components of main midpoints source.

Process Percentage

(%) Components EKR 88.6 Import nylon textile

11.0 EDTA

1.4 Water for industrial use EKR- 80.1 Import nylon textile Bio 5.0 Water for industrial use

4.9 Yeast EKR- 69.1 NPK fertilizer Phyto 30.9 Import nylon textile

0.1 EDTA

Ecological assessment analysis

Figure 6 is the result of visualizing radar diagrams resulting from b&v analysis for the three strategies, the most influential midpoint components are GWP, EP, POCP, and the sum of primary energy. The four midpoints lead to natural environment endpoints or contributions to ecological conditions. GWP is formed due to its association with electrical energy consumption during the EKR process; POCP is formed from the possibility of forming photochemical oxidants emitted by polluting gases during the process.

EP is formed due to the factors mentioned in the previous discussion. If the LCA analysis shows that the EK-Phyto and EK-Bio strategies have the same high environmental impact, then the b&v analysis shows that the EK-Phyto strategy has the highest environmental impact on ecology compared to the other two strategies. It also strengthens the information that EKR is the lowest environmental impact, although technically, the efficiency of EK-Phyto removal is the highest compared to the other two strategies. Although the pilot scale is the scale closest to field conditions, according to Mao et al. (2019), underestimating the LCA analysis of 78-84% can occur, so research based on actual size is recommended. Economic feasibility analysis and stakeholder acceptance analysis for each EKR strategy in the future need to be added so that the sustainability framework is achieved.

Figure 6. Midpoint analysis result of b&v.

Conclusion

Based on the results of the LCA analysis, there are two midpoints of the 18 midpoints of Recipe I (2016) and one midpoint from Cumulative Energy Demand that may impact the environment in the form of freshwater eutrophication, natural land changes and non-

renewable fossil. The midpoints of other methods are broadly similar to the actual scale, although it can be underestimated if the research is not based on the actual scale. Pilot-scale LCA studies on EKR can be applied even though they need to be combined with other analytical models to strengthen a system's decision-making. It is also necessary to add a review 0

2 4 6 8 10 12 14GWP

ODP

EP

AP POCP

ADPE Sum of Primary Energy

Freshwater

EKR EKR-Phyto EKR-Bio

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Open Access 4126 of stakeholders' economic and socio-cultural aspects in

the future so that the sustainability aspect can be achieved.

Acknowledgements

This research was funded by the 2021 World Class University-Indonesian Collaborative Research Program budget scheme with contract number 1383/IT3.L1/PN/2021.

We would like to thank The Institution of Research and Community Services of ITB, UNDIP, and IPB for providing the opportunity for foremost researchers. A part of this article was presented at the 2nd International Conference on Environment, Socio-Economic, and Health Impacts of Degraded and Mining Lands, 30-31th August 2022, Universitas Brawijaya, Malang, Indonesia.

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