Leaching behavior of metals from a limonitic nickel laterite using a sulfation–roasting–leaching process

doi:10.1016/j.hydromet.2009.07.012

Hydrometallurgy

Volume 99, Issues 3–4, November 2009, Pages 144-150

https://doi.org/10.1016/j.hydromet.2009.07.012 Get rights and content

Abstract

The leaching behavior of metals from a limonitic laterite was investigated using a sulfation–roasting–leaching process for the recovery of nickel and cobalt. The ore was mixed with water and concentrated sulfuric acid followed by roasting and finally leaching with water. Various parameters were studied including the amount of acid added, roasting temperature and time, sample particle size, addition of Na₂SO₄ and solid/liquid ratio in leaching process. More than 88% Ni, 93% Co and < 4% Fe are extracted under the determined conditions. Simultaneously, about 90% Mn and Cu, 70% Mg, 45% Al, 25% Zn, 4% Cr and Ca are extracted respectively. The pH of the leach solution is about 2. The leaching efficiency is independent of sample particle size due to decomposition of ferric sulfate formed during roasting. The roasted mass was characterized by various physico-chemical techniques such as DSC/TGA, XRD and SEM. This process provides a simple and effective way for the extraction of nickel and cobalt from laterite ore.

Introduction

Nickel is a strategic metal and mainly used in the preparation of stainless steel and non-ferrous alloys with impact strength, corrosion resistance and other electrical, heat and magnetic properties. Nickel is also used in batteries, fuel cells, electroplating etc (Park and Nam, 2008). About two-thirds of the nickel is consumed by the stainless steel industry which has been growing at the rate of 5–6% in per annum over the last 20 years (Anderson, 1996, Anthony and Flett, 1997). Commercially nickel is recovered from sulfide as well as laterite (Moskalyk and Alfantazi, 2002). Before the 1960s, most nickel was produced commercially from sulfide ores. However due to the rapid increase in the world consumption of nickel, coupled with decreasing reserves of sulfide ores, laterites are becoming a significant source for nickel.

Both pyrometallurgical and hydrometallurgical processes are applied commercially to recover nickel and cobalt from laterite. Pyrometallurgical techniques are suited to treat saprolite (high magnesium laterite) with processes typically involving drying, calcining/reduction and electric furnace smelting to produce a ferro–nickel or nickel sulfide matte. The disadvantages of these processes include the requirement for high grade ores, substantial energy inputs and poor cobalt recovery (Georgiou and Papangelakis, 1998). Hydrometallurgical processes are more applicable to the limonite (high iron laterite), and include ammonia–ammonium carbonate leaching (Caron process) (Panda et al., 1980, Valix and Cheung, 2002), atmospheric leaching with sulfuric acid (AL) (Canterford, 1978, Arroyo and Distin, 2001) and high pressure acid leaching (HPAL) (Georgiou and Papangelakis, 1998, Rubisov and Papangelakis, 2000, Johnson et al., 2005a, Johnson et al., 2005b). The Caron process has the disadvantages of low extraction of nickel and cobalt and large energy and reagent requirements. McDonald and Whittington (2008) reviewed the processes reported in the past 30 years that can be used to extract nickel and cobalt with the focus on AL and HPAL. The AL process is simply controlled and maintained with lower costs, but produces leach liquor with significant concentrations of iron and aluminium which complicates downstream processing (Chander, 1982, Neudorf, 2007). The HPAL process provides high recoveries of nickel and cobalt, allows acceptable acid consumption and produces low residual iron in solution, but requires expensive autoclaves and has high maintenance costs (Canterford, 1979, Anthony and Flett, 1997).

To overcome the problems of AL and HPAL processes, there is also interest in the recovery metal values using a sulfation–roasting process due to its ease of operation (Nicolas, 1968, Kar and Swamy, 2000, Swamy et al., 2003). In this process, nickel and cobalt are converted into respective sulfates which are highly soluble in water leaving most of the iron and aluminium in the residue as insoluble oxides. This process includes three steps: mixing with concentrated sulfuric acid, roasting and water leaching. Due to the proprietary nature of the process, most of the publications lack detailed information concerning the various process steps. Furthermore, information relating to co-extraction of metals like aluminium, manganese and magnesium is rather scant. In some instances, a sulfation process without roasting was proposed (Xu et al., 2005, Neudorf, 2006). However, for these processes high iron dissolution and filtration difficulties were indicated.

In this work, the leaching behavior of metals from a limonitic laterite was investigated using a sulfation–roasting–leaching process for the purpose of nickel and cobalt recovery. The change in the mineralogy of laterite with roasting condition was studied using DTA/TGA, XRD and SEM techniques. This study explored the effects of amount of sulfuric acid added, roasting temperature and time, sample particle size and salt addition in roasting process on the leaching efficiency of various metals including nickel, cobalt, iron, manganese, aluminium, magnesium, zinc and chromium.

Section snippets

Chemical composition

The lateritic ore was collected from the Tubay region, Mindanao, Philippines. The raw material used in this study was a typical limonitic laterite ore with high iron content and was ground to − 60 mesh after drying. Table 1 shows the quantitative chemical assays of the sample.

DSC–TGA, XRD and SEM analysis

For mineralogical characterization, thermo-gravimetric and differential scanning calorimetry (DSC–TGA) analyses (maker: TA, American) were conducted on the laterite samples from 20 to 900 °C with a linear heating rate of

Effect of addition of sulfuric acid

A series of sulfation experiments were carried out by varying the addition of sulfuric acid from 10 to 90 wt.% at a roasting temperature of 700 °C and roasting time of 30 min. The results, shown in Fig. 4, found that the nickel extraction efficiency increases with an increase of sulfuric acid added up to 50 wt.%, though with further increase the effect is marginal. Manganese shows a similar extraction behavior to nickel. The extractions of the low levels of cobalt and magnesium are more than

Conclusions

The sulfation–roast–leaching process used on a limonitic laterite ore extracted about 90% Ni, Co and Mn — mainly influenced by the amount of acid added and the roasting temperature and time. The sulfation process was enhanced by increasing the roasting temperature to about 700 °C, while increasing the roasting time reduces Fe and Cr dissolution to < 4%. Sample particle size has no influence on the metal extractions due to the effective formation and decomposition of ferric sulfate. The

Acknowledgements

The authors wish to express sincere thanks to other colleagues of non-ferrous metallurgy and resource recycling division in CSU for their active co-operations and supports. One of the authors, Kyung-Ho Park is grateful to KIGAM, Korea for sanctioning of sabbatical leave to carry out this work.

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