Elsevier

Journal of Cleaner Production

Volume 218, 1 May 2019, Pages 130-140
Journal of Cleaner Production

Maximization of extraction of Cadmium and Zinc during recycling of spent battery mix: An application of combined genetic programming and simulated annealing approach

https://doi.org/10.1016/j.jclepro.2018.11.226Get rights and content

Highlights

  • Problem of maximum extraction of Cadmium and Zinc from spent battery mix is undertaken.

  • Combined genetic programming and simulated annealing approach is proposed.

  • Genetic programming models fits the cadmium and zinc output very well.

  • Simulated annealing optimizes the Genetic programming model to obtain the optimum inputs.

Abstract

There are a number of government directives and regulations as well as many public schemes on the recycling of batteries, in spite of this; the quantity of batteries that are actually recycled is still very low. Current production capacity cannot meet projected demand of Lithium-ion batteries. To counter this, the reclamation and repurposing of metals like cadmium, Lithium and Zinc from used or spent batteries is the only viable scheme. This is both environmentally friendly and economically feasible. An alternative is the selective chemical leaching in the presence of Sulfuric acid and Sodium metabisulfite. In this paper, the effect of these chemicals as well as the solid-to-liquid ratio and time of retention is comprehensively studied. Experiments are designed for the recovery of Zinc and cadmium from the spend Lithium-ion batteries mix. To maximize the recovery of Zinc and cadmium, the combined genetic programming and simulated annealing approach is proposed. Genetic programming is used for the formulation of functional relationship between recovered metals Zinc and cadmium and the inputs (Solid/Liquid ratio, concentration of Sulfuric acid, mass of Sodium metabisulfite and retention time). The optimal input conditions determined using the simulated annealing algorithm includes Solid/Liquid ratio of 11.7%, 0.86 M Sulfuric acid, 0.56 g/g of Sodium metabisulfite and 45 min of retention time. Three dimensions surface analysis reveals that a lower value of Solid/Liquid ratio favours a better yield. The optimal conditions are validated using experiments. This confirms the efficacy of simulated annealing aided genetic programming techniques as well as the optimal conditions of the metal extraction.

Introduction

Cleaner energy storage systems such as Lithium ion batteries have propelled society to become more mobile and portable (Nemecek, 1994). Despite their considerable advantages, they still pose significant environmental and health hazards. Most of these hazards arise from improper disposal and storage of end-of-life batteries. Global production and consumption of batteries has increased disproportionately to present waste management measures, causing both short and long term issues.

Battery packs are extremely flexible in their design and use, being composed of individual smaller and usually identical cells (Battery pack, 2018). They have longer life span of 2–3 years, and their usage in electric vehicles have resulted in decreased environmental impact when compared to traditional internal combustion (IC) engine-run vehicles when compared using a life cycle assessment (Notter et al., 2010). Regulations have also been passed limiting the amount of dangerous chemicals in batteries, especially mercury (U.S. Environmental Protection Agency, 1997). The end product has become more environmentally friendly than before while being more efficient and resistant to failure. Lithium ion batteries have a very small environmental cost to bear (Boyden, 2014). Other battery chemistries like Ni-Cd pose more significant environmental threats and rising production levels imply higher rates of their consumption. Materials like Cadmium and Cobalt have very adverse effects on both health and the environment (World Health Organisation, 2010; Leyssens et al., 2017). There are several regulations in place limiting the use of these materials in most products. Their disposal and repurposing after they have reached their end-of-life is severely lacking (Official Journal of the European Union, 2006).

In some countries, upwards of 250,000 tonnes of batteries were deemed as waste in 2014 (Eurostat, 2018). In 2016, worldwide consumption of lithium for battery use was 77,821 metric tons of lithium carbonate equivalent (Statista, 2018a). Demand for the metal is projected to reach 422,614 metric tons of lithium carbonate equivalent (Statista, 2018b) by the year 2025. Producers are not currently capable of meeting this demand. In some countries, <2% of all lithium batteries are recycled while the rest are put to landfill (Boyden, 2014). This represents a high threat to public health (Rall and Pope, 1995) and the environment via the leakage of dangerous chemicals (Andresen and Küpper, 2012). It also represents a waste of reusable resources. There is a 30% decrease in overall cost by using recycled materials (Rabah et al., 2008).

Rising production demands can be alleviated by using materials from spent batteries that have undergone a set of recovery and extraction processes. Each process must start with the sorting of various batteries based on their chemical or energy contents (Tonteri et al., 2000). This can be done manually or through some degree of automation (Bernardes et al., 2004). The mix so obtained must undergo extraction to obtain metals like Li, Cd, Ni etc. which are used in further production. These extraction procedures are usually hydrometallurgical for lower value metals, but can also by pyrometallurgical, physical, chemical or biochemical in nature (Li et al., 2009). The set of production treatments depends on the battery chemistry in question (Wang, 2014). One must factor in transport and energy requirements to see the economic feasibility of recycling spent batteries (Niu et al., 2014).

Metal extraction via hydro and pyrometallurgical methods involves a heavy energy intake, as well as high security and pollution risks (Rocchetti, 2013). An alternative to this is chemical and biochemical methods of metal extraction. Bioleaching is one biochemical technique which uses bacteria (like Acidithiobacillus ferrooxidans for iron pyrites (Zhang et al., 2008) and Penicillium citrinum for low grade manganese ores (Acharya et al., 2002)) to react with the metal to yield soluble products. These soluble products then undergo further filtration to extract metal. This technique provides high yields but requires significant improvements before it can be considered commercially viable (Olson et al., 2003). Metal solubilisation via H2SO4 can be performed in a single step leaching process with yields of up to 81% for Cadmium, 96% of Cobalt, 94% of Manganese, 68% of Nickel and 99% of Zinc from a mix generated from spent batteries.

Previous research focussed on the use of response surface methodology (RSM) for modelling and optimizing the metal yields (Tanong et al., 2017). RSM is based on assumption of model structure followed by an estimation of coefficients in the model using optimization methods. This method works satisfactorily if the information about the system behaviour is known. Actual engineering problems are often complex, multidimensional, and incomplete information. RSM is no longer suitable. Predictive modelling methods based on Artificial intelligence (AI) seems a better alternative. Among AI methods, evolutionary approach of genetic programming (GP) has the ability to automate the model structure and coefficients estimation resulting in the evolution of the best model (Woodward et al., 1999). The GP model has a free non-linear form that has the best fits. It can adapt to the system behaviour. A number of diverse applications for GP techniques have been found, which shows its effectiveness and efficacy to model the systems of any given complexity.

This study aims to propose a combination of GP and simulated annealing (SA) approach to maximize the recovery of Zinc and Cadmium. The specific works are listed as follows. Firstly, the effect of concentration of H2SO4, mass of Na2S2O5 as well as the solid-to-liquid ratio and time of retention is comprehensively studied. Secondly, experiments are firstly designed for the recovery of Zinc and cadmium from the spend Lithium-ion batteries mix. Thirdly, GP is used for the formulation of functional relationship between recovered metals Zinc and cadmium and the inputs (Solid/Liquid ratio, concentration of Sulfuric acid, mass of Sodium metabisulfite and retention time). A comparative study between GP, the Box-Behnken model and analysis of variance (ANOVA) analysis has also been performed. Then, the optimal input conditions are determined and validated using experiments. Finally, conclusions are then drawn upon the efficacy of the proposed approach, as well upon metal extraction.

Section snippets

Research problem undertaken

This section discusses the research problem statement for the combined GP and SA approach for the study of chemical metal extraction from a spent battery mix. A disproportionate amount of spent batteries is not recycled, in spite of various public programmes for the same. Recycling spent batteries to recycle valuable metals is one way to reduce rising demands on production. Recycling batteries consists of sorting, metal extraction and reprocessing. Existing pyrometallurgical and

Design of experiment

Samples of spent batteries were collected, manually disassembled and sorted according to the following concentrations (Tanong et al., 2017): 0.28% Li-ion, 0.80% lithium iron sulphide, 1.60% Ni-MH, 15% Zn-C, 14.3% Ni-Cd and 68% alkaline battery. The mix then underwent screening for alien particles including non-metallic components and other contaminants. Metallic composition of the resultant was then determined using inductively coupled plasma-atomic emission (ICP-AE) spectroscopy (Melville, 2014

Genetic programming approach

Genetic programming (Gandomi et al., 2015), an AI approach stem from the principle of Darwinian evolution i.e. “Survival of the fittest”. The procedure involves randomly initialising candidate solutions, which are probabilistically chosen to reproduce basing on their fitness on the output data. Each generation has a fixed population size, where each member is one model. During the initialisation, the initial input and output sets (terminal set), the function space with which to compose model

Statistical modelling using linear regression and GP

The experimental output is dependent on the four correlated parameters: Solid/Liquid ratio (x1), concentration of H2SO4 (x2), Mass of Na2S2O5 (x3) and the Retention time of the mixture (x4). The correlation matrix is given in Table 2. From Table 2, it can be seen that each parameter has some degree of correlation with each other. The linear modelling was unlikely to be successful. Multiple linear regression models were formulated from the data, and the results justify the findings of the

Conclusions

The present work proposes the comprehensive study to optimise the chemical metal leaching of valuable metals from a mix of spent batteries. The optimization of the chemical metal leaching process has been carried out using combined using Combined genetic programming and simulated annealing Approach. Experiments were conducted to validate this approach. The optimal conditions obtained are: Solid/Liquid ratio = 11.7%, molarity of H2SO4 = 0.86 M, g/g of Na2S2O5 = 0.56 g/g and 45 min of retention

Acknowledgement

Authors acknowledge Grant DMETKF2018019 by State Key Lab of Digital Manufacturing Equipment and Technology (Huazhong University of Science and Technology). Authors also like to acknowledge Shantou University Youth Innovation Talent Project (2016KQNCX053) supported by Department of Education of Guangdong Province. This study is also supported by Shantou University Scientific Research Fund (NTF 16002).

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