Nanoscale Zero-Valent Iron (nZVI) for Heavy Metal Wastewater Treatment: A Perspective

Shaolin Li , Lei Li , Weixian Zhang

Engineering ›› 2024, Vol. 36 ›› Issue (5) : 18 -22.

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Engineering ›› 2024, Vol. 36 ›› Issue (5) :18 -22. DOI: 10.1016/j.eng.2023.08.012
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Nanoscale Zero-Valent Iron (nZVI) for Heavy Metal Wastewater Treatment: A Perspective
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Abstract

Industries such as non-ferrous metal smelting discharge billions of gallons of highly toxic heavy metal wastewater (HMW) worldwide annually, posing a severe challenge to conventional wastewater treatment plants and harming the environment. HMW is traditionally treated via chemical precipitation using lime, caustic, or sulfide, but the effluents do not meet the increasingly stringent discharge standards. This issue has spurred an increase in research and the development of innovative treatment technologies, among which those using nanoparticles receive particular interest. Among such initiatives, treatment using nanoscale zero-valent iron (nZVI) is one of the best developed. While nZVI is already well known for its site-remediation use, this perspective highlights its application in HMW treatment with metal recovery. We demonstrate several advantages of nZVI in this wastewater application, including its multifunctionality in sequestrating a wide array of metal(loid)s (> 30 species); its capability to capture and enrich metal(loid)s at low concentrations (with a removal capacity reaching 500 mg·g−1 nZVI); and its operational convenience due to its unique hydrodynamics. All these advantages are attributable to nZVI’s diminutive nanoparticle size and/or its unique iron chemistry. We also present the first engineering practice of this application, which has treated millions of cubic meters of HMW and recovered tons of valuable metals (e.g., Cu and Au). It is concluded that nZVI is a potent reagent for treating HMW and that nZVI technology provides an eco-solution to this toxic waste.

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Keywords

Nanoscale zero-valent iron / Wastewater / Heavy metal / Resource recovery

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Shaolin Li, Lei Li, Weixian Zhang. Nanoscale Zero-Valent Iron (nZVI) for Heavy Metal Wastewater Treatment: A Perspective. Engineering, 2024, 36(5): 18-22 DOI:10.1016/j.eng.2023.08.012

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1. Introduction

Nanoscale zero-valent iron (nZVI) is particulate metallic iron (Fe(0)) with a particle size of less than 1 μm. nZVI primarily consists of an Fe(0) core coated in an iron (hydro)oxide shell, with a specific surface area that is typically greater than 20 m2·g−1 [1], [2], [3], [4]. It is well-known for its power in chemical reduction; the Fe(0) core serves as an electron source, the shell works as an electron tunnel, and its large surface area permits the quick release of electrons. These properties and the environmentally benign nature of iron make it an ideal reagent for environmental cleanup [5], [6], [7].

The use of nZVI for environmental cleanup began in the late 1990s, when it was used for the in situ remediation of contaminated sites in North America; the nZVI was injected into the subsurface in order to clean sites contaminated by chlorinated hydrocarbons [1], [5], [8]. The use of nZVI quickly became popular in this area, with the publication of numerous research articles and review papers on its use in remediation [4], [5], [6], [9], [10], [11], [12], and nZVI has been exclusively tagged for site remediation ever since. In this perspective, we demonstrate that nZVI is a robust reagent for the treatment of heavy metal wastewater (HMW) that provides an eco-solution for this hazardous waste, based on our 25 years of experience in laboratory research on nZVI and full-scale engineering practices involving its use and applications [1], [2], [3], [5], [13], [14], [15], [16], [17], [18], [19], [20], [21], [22], [23], [24], [25], [26], [27]. This treatment application may open up a new avenue in the research and development of nZVI after its applications in contaminated site remediation.

2. Background

This work started with an investigation of the highly hazardous wastewater produced by non-ferrous metal smelting [17], [19], [20]. This wastewater is heavily contaminated and contains a number of metal ions and metalloid oxyanions, such as copper (Cu), nickel (Ni), cadmium (Cd), arsenic (As), selenium (Se), and thallium (Tl) [17], [20] (Fig. 1(a)). Their concentrations range from grams per liter (e.g., Cu(II)) to a few parts per billion [17], [20]. The wastewater also contains high contents of salt (primarily NaCl, at 8% w/w), organic substances, and ammonium [17], which may add up to 100 g·L−1 in total [17]. In China alone, billions of gallons of such wastewater are discharged every year [28].

Treating this wastewater is complex and difficult, especially to the level required by discharge standards. Such wastewater has traditionally been treated via chemical precipitation using lime, sulfide, and/or ferric salt, through which the target ions are precipitated [19], [20]. Their effluents often contain considerable amounts of heavy metals (typically in the range of 1-100 mg·L-1 and occasionally reaching 500 mg·L-1) and do not meet discharge standards [20], [29]. This technological incompetence is due to the limitations of the precipitate solubility, the re-dissolution of the amphoteric metal, the poor settleability of the precipitates, and the vulnerable stability of the hydroxide precipitation [17], [20]. Moreover, treating this wastewater has recently become more challenging, because more elements (e.g., Tl) have been added to the list of concern for discharge standards [30], and the acceptable concentrations of heavy metals in effluent have been lowered (e.g., for Ni2+, lowered from 0.5 to 0.1 mg·L-1) [31], [32] (Fig. 1(a)).

3. Mechanism of nZVI for wastewater treatment

Since 2005, a number of research groups—including ours—have conducted a series of studies to examine the sequestration of metal(loid)s in aqueous solutions using nZVI [2], [3], [4], [9], [13]. These studies have shown that nZVI can react with metal(loid)s via chemical reduction, adsorption, and (co)precipitations [2], [3], [4], [9], [13] (Fig. 1(b)). It can act as an electron donor to reduce metal(loid)s such as Cu(II) or Cr(VI), which form metallic nano-islands/dendrites or Fe composites on the nZVI particles after reacting [14], [25], [33]. nZVI can also sequestrate metal cations (e.g., Pb(II) and Zn(II)) and oxyanions (e.g., As(V)) via chemical adsorption and (co)precipitation, which are performed by the oxide shell of nZVI and the reaction products (e.g., Fe(II) and the hydroxyl ion) from nZVI corrosion [3], [4], [17], [22], [34] (Fig. 1(b)). At present, more than 30 different inorganic elements or species [3], [4], [9], [13] have been found to react with nZVI, covering all the metal(loid)s on the list of concern [31], [32] for discharge standards, as well as certain other elements that are currently not on the list but are still of environmental concern due to their toxicity (e.g., uranium (U), tellurium (Te), and rhodium (Rh)) [24], [35], [36] (Fig. 1(a)).

On the basis of these promising laboratory results, we were invited to assess the feasibility of applying nZVI to treat smelting wastewater via a few pilot-scale studies [17], [19]; the success of the pilot studies then led to a number of large-scale treatment applications [20], [23], which now treat a total of approximately 1000 m3 of this wastewater daily. These practical applications demonstrate the high efficacy and several other advantages of nZVI in treating HMW, as discussed below.

nZVI is a robust reagent for removing the heavy metals or metalloids in wastewater. In the aforementioned applications, it simultaneously removed all eight targeted metal(loid)s (e.g., Cu, As, and Ni) and outperformed conventional reagents such as lime and ferric salt: The removal efficiency of the targeted metals reached 96% using nZVI, in comparison with only 37% using Ca(OH)2 and 83% using FeCl3 and NaOH [19], [20]. The removal capacity of nZVI reached about 500 mg·g−1 nZVI for these pollutants, despite the large quantities of impurities that coexisted in the wastewater [16], [20]. This capacity is higher than those of most known resins/adsorbents or conventional bulk ZVI [9], [34]. Such a high capacity is technically enabled by the reuse of nZVI and ultimately attributable to the high surface-to-mass ratio of nZVI, which allows the quick release of its reducing power and better utilization of its Fe(0) content before its surface becomes passivated due to surface precipitation (e.g., of Cr(III) and As(V)) [14].

nZVI can remove some critical metals (e.g., Cu(II) and Pb(II)) in the wastewater to levels lower than those achieved using conventional precipitants. Concentrations of redox-sensitive species such as Cu(II) can be reduced to < 0.1 mg·L-1 after nZVI treatment, which can be explained by the large redox potential differences between the Fe(0) and these ions that give the removal a large driving force or equilibrium constant [16], [20]. Levels of amphoteric metal ions (e.g., Zn(II) and Pb(II)) can be reduced to lower concentrations using nZVI than using lime [19]; this capability is related to the mild alkalinity of nZVI and the slow release of the precipitants (Fe(II) and hydroxide ions) from the nZVI-water reaction [16]. As particulate solids, nZVI particles can act as seeds in the treatment and facilitate the quick formation of settling-separable products [19], [20], [23], which is meaningful when the concentration of the targeted ion is low. Some nZVI reactions produce Fe(II) and Fe(III) ions that can combine with the chelate in the wastewater, releasing the targeted heavy metals from the chelation that may otherwise prevent them from precipitating [37]. All these attributes give nZVI additional advantages for HMW treatment.

4. Hydrodynamics, unit operation, and process

nZVI particles have favorable hydrodynamic properties that assist in their wastewater treatment applications. Due to their low surface charge in solutions with near-neutral pH [26], [38] and their typically high particle concentration conditions in practical applications (e.g., stock solution), nZVI particles occur primarily as microscale aggregates in water treatment [20], [26] (Fig. 2(a)). The aggregates have low bulk densities (∼1.05 g·cm−3), are low in fluidization velocity, and can easily be suspended in water; a condensed slurry of nZVI aggregates also has a low packing density (∼1.2 g·cm−3) and is low in apparent viscosity [26] (Fig. 2(a)). Thus, the aggregates and their concentrated slurries are readily moved with the flow (Fig. 2(a)) and are hydrodynamically similar to coagulation flocs or activated sludge to some extent [26].

Due to these hydrodynamic properties, nZVI is easily handled in water using conventional unit operations and equipment in wastewater treatment, which are scalable and in turn offer nZVI technological advantages for wastewater treatment. For example, the easy suspension of nZVI in water makes possible the use of mechanical mixing during the reaction [20] (i) in Fig. 2(b), which is otherwise inapplicable for bulk ZVI particles [15], [39]. The applicability of mechanical mixing brings several operational conveniences, such as quick adjusting of the reactor performance via the fast mixing of newly added nZVI [16], [17], [19], [20] in response to quality fluctuation of the influent (ii) in Fig. 2(b); the creation of extra buffering capacity from the mixing; the enhancement of mass transfer and alleviation of cementation on the nZVI particle surface; and, most importantly, facile discharge of solids (i.e., the sequestrated metal(loid)s, nZVI corrosion products, and influent suspended solid) from the reactor [16], [17], [19], [20] (iii) in Fig. 2(b). The last of these benefits makes the reactor immune to permeability loss or the reactor clogging that is fatal to a fixed-bed ZVI reactor [39], [40], [41], [42]. Another benefit is that the low viscosity of concentrated nZVI slurries allows their conveyance via pumping and pipeage (i) and (ii) in Fig. 2(b), which greatly facilitates the dosing and reuse of nZVI in large-scale operation [16], [17], [19], [20]. Most of the nZVI in water is separable via gravitational settling after 1-2 h, due to its dominating form of microscale aggregates [18], [26] (iv) in Fig. 2(b). This settleability enables the recirculation and reuse of nZVI during the application, which can increase the material efficiency of the nZVI, reduce its dosage, and bring down the treatment cost.

By combining the abovementioned unit operations, we developed a simple but reliable process using nZVI to treat wastewater (Fig. 2(b)). The process uses a mixing reactor to mix nZVI with wastewater, where the reactor is dosed with a condensed stock slurry of nZVI. Following the mixing reactor is a gravitational settling tank that separates the nZVI and the treated wastewater and condenses the settled nZVI. The condensed slurry on the bottom of the settling tank is pumped back to the reactor for further use of the nZVI. These processes in multiple can be arranged sequentially or in parallel [17], [20] (e.g., R1 and R2 in Fig. 2(c)). This process is compatible with ordinary water treatment processes (e.g., the coagulation process with dosing, mixing, and sedimentation); therefore, it can be applied by utilizing existing facilities or equipment (e.g., the mixer and/or the settling tank) with little or no additional upgrades.

Since 2012, the nZVI process has been used as an advanced treatment for the effluent from lime/sulfide precipitation in a smelting wastewater treatment plant (Figs. 2(c) and (d)). Nearly 80 000 kg of nZVI is used to treat 400 000 m3 of smelting wastewater each year [20], [23]. Years of application show that the process is easy to operate and has stable performance. The process is now becoming popular in this field for advanced heavy metal(loid)s removal.

5. Future outlook

The nZVI application outlined here gives birth to a more promising future for HMW treatment. In the abovementioned operation, the reacted nZVI from the wastewater reactor was found to comprise nearly 10% copper; it also contained 41 g·t−1 of gold (where the gold was at the parts per billion level in the wastewater influent) and several other elements, such as silver (Ag) and Ni [20], [23] (Fig. 2(e)). The reacted nZVI was then send to the smelter to extract these valuable metals. Kilograms of gold were recovered along with tons of copper each year—these metals were completely lost previously [23]. These recovered metals partially offset the treatment cost; such an exchange that uses iron to obtain valuable metals may always be an economical option, because iron is abundant on earth. The recovery capability of nZVI is due to its extraordinarily high capacity for heavy metal sequestration, which results from its high surface-to-mass ratio, the redox nature of the sequestration reaction, and the repetitive reuse of the nZVI [20], [21], [23]. By transforming highly hazardous HMW into a valuable resource, nZVI provides an eco-solution for this form of wastewater, and its technology may revolutionize HMW treatment.

Our practical experience with this treatment has demonstrated that more research is still needed to make nZVI wastewater treatment more efficient and competitive. For example, reactions between nZVI and ambient water or oxygen during its application (e.g., during nZVI production, storage, and use) may decrease its material efficiency and cause safety problems [43]. Therefore, efforts are now being made to solve these problems and upgrade the technology. Recent advances in modifying and compositing nZVI with species such as phosphate and oxalate [44], [45], [46], [47], [48], [49], [50], [51] can enhance its treatment capability. nZVI sulfidation may be an ideal solution to improve the electron selectivity of nZVI and secure its application in HMW treatment [43]. The nZVI production method is continuously being optimized to make it more environmentally benign and economical [43], [52]. The technological development of online real-time analyses of wastewater pollutants may help to fine-tune nZVI dosing and increase nZVI’s treatment efficiency. In addition, combining nZVI with bio-treatment may produce synergic effects that benefit both technologies and further expand the application of nZVI in wastewater treatment [27], [53]. This technology, which has grown from the laboratory scale to full-scale applications, can serve as an example of and provide experience for the research and development of other functional materials for environmental engineering purposes.

Compliance with ethics guidelines

Shaolin Li, Lei Li, and Weixian Zhang declare that they have no conflict of interest or financial conflicts to disclose.

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