Assessing heavy metals and developing a fingerprint for Mahikeng paints using ICP-MS analysis: implications for environmental health

doi:10.21203/rs.3.rs-5013484/v1

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Assessing heavy metals and developing a fingerprint for Mahikeng paints using ICP-MS analysis: implications for environmental health

https://doi.org/10.21203/rs.3.rs-5013484/v1

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Despite global efforts to mitigate lead in paints, studies reveal persisting lead levels above safety thresholds in household paints in many nations. Alongside lead, other heavy metals (HMs) in paints pose health risks. The study aims to assess lead content and heavy metals levels, and develop a fingerprint for paints in Mahikeng, the capital of North West Province, South Africa, using ICP-MS analysis. We purchased and analyzed 30 paint samples from Mahikeng. The most prominent and nontoxic elements detected are Nitrogen (N), Calcium (Ca), Iron (Fe), Carbon (C), Aluminum (Al), and Phosphorus (P). Lead concentrations ranged from 0 ppm to 4.17 ppm, below South Africa's 600 ppm MPLL. Other HMs detected included Beryllium (Be), Chromium (Cr), Nickel (Ni), Arsenic (As), Cadmium (Cd), Antimony (Sb), Mercury (Hg), as well as radionuclides Barium (Ba), Strontium (Sr), Thorium (Th), and Uranium (U). Their concentrations range from 0 ppm to 810.57 ppm, with most elements found at relatively low levels. The obtained Pb isotopic ratios and rare earth elements (REE) patterns were used to develop a fingerprint. These findings offer insights into the environmental health implications of lead and heavy metals contamination by the paints, as well as the identification of their sources. This research contributes to sustainable cities and communities by promoting responsible consumption and production practices, enhancing quality education on environmental health, and supporting good health and well-being through the reduction of hazardous exposures.

Lead

Heavy metals (HMs)

Paints

ICP-MS analysis

South Africa

Environmental health

The harmful impacts of lead on human health, particularly in children, have reduced the justification for the extensive use of lead-based paints, despite their advantages in durability, color stability, and moisture resistance. Children are at a higher susceptibility to lead poisoning because they tend to put their hands in their mouths more frequently, have a faster breathing rate, and possess a more absorbent digestive system compared to adults (Ahamed & Siddiqui, 2007). Children's exposure to lead (Pb) through paints has been a worldwide concern for the past fifty years. Although regulatory and safety measures for paint manufacturers, as well as litigation promoting lead-free paints, have been in place for over half a century, lead-based paints continue to be widely used around the globe (Ewers et al., 2011; Njati & Maguta, 2019; Megertu & Bayissa, 2020).

Researchers have traditionally focused on lead (Pb) levels in paints, but few studies have shown that paints also contain other heavy metals (HMs) (Muluneh et al., 2023; Turner & Filella, 2023). Therefore, it is crucial to determine the levels of these other heavy metals in paints due to their harmful effects on human health. Heavy metals present considerable health risks to humans, especially when found in high concentrations in the environment. This study aligns with Sustainable Development Goals (SDGs) 3 (good health and well-being) and 11 (sustainable cities and communities) by addressing the health and environmental impacts of heavy metals in paints, promoting responsible consumption and production (SDG 12) practices, and contributing to the creation of sustainable and healthy living environments.

Heavy metals (HMs) are naturally occurring elements characterized by an atomic number (Z) greater than 20 and a density exceeding 5 g/cm³ (Shi et al., 2019). Based on this definition, there are 51 HMs in the periodic table (Ali & Khan, 2018). Numerous scientific publications and governmental records have documented studies and regulations concerning heavy metals. These include their sources in the environment, transport, bioaccumulation in biota, as well as their toxicity and harmful effects on living organisms, including humans (Abd Elnabi et al., 2023).

The ecosystem's natural and human-induced sources of heavy metals (HMs) are steadily growing, leading to increased environmental accumulation. Human exposure to these metals has surged, mainly due to twentieth-century industrial activities. The bioaccumulation of HMs leads to various toxic effects on tissues and organs (Abd Elnabi et al., 2023; Oladejo et al., 2021). Two major environmental chemical disasters of the twentieth century, Minamata disease and the Donana mining catastrophe, were associated with the release of heavy metals into the environment (Ali & Khan, 2017). Heavy metals can become highly toxic when interacting with various environmental elements such as water, soil, and air (Mitra et al., 2022). Paints are major contributors to environmental heavy metal pollution, including lead, especially within residential settings (Ewers et al., 2011; Megertu & Bayissa, 2020; O’Connor et al., 2018). Figure 1 shows the principal pathway of heavy metals to man (Abd Elnabi et al., 2023).

Studies have shown that several heavy metals (HMs) can persist in the environment for extended periods. For instance, cadmium (Cd) can persist in soil for 75 to 380 years, mercury (Hg) for 500 to 1000 years, and copper (Cu), nickel (Ni), zinc (Zn) and lead (Pb) for 1000 to 3000 years (Wu et al., 2022). Excessive heavy metals in soil can upset the ecological balance and spread to other environmental compartments, including the atmosphere and water bodies. This poses risks to animals and humans through the food chain, inhalation, drinking water, and direct contact (Lu et al., 2015).

The heavy metals lead (Pb), cadmium (Cd), and mercury (Hg) are common pollutants largely released from diverse industrial activities. Even though their atmospheric concentrations are low, they contribute to soil deposition and accumulation. These elements remain in the environment and can bioaccumulate within food chains. Lead exposure, in particular, is associated with various health hazards, including hypertension, anemia, and impaired reproductive, respiratory, nervous, and immune system functions. Children exposed to lead may suffer from a dose-dependent decrease in brain volume, resulting in lower academic performance and intelligence levels, with these effects potentially continuing into adulthood (Fatmi et al., 2017; Mazumdar et al., 2011). Lead poisoning can result in cognitive impairments, neurological issues, difficulties with focus, behavioral challenges, and excessive activity in infants.

Blood tests are used to evaluate blood lead levels (BLL) in children, which is a valuable technique for diagnosing lead exposure (Ladele et al., 2019; Naranjo et al., 2020). According to the World Health Organization (WHO, 2012), it is estimated that more than 800 million children have blood lead levels (BLLs) exceeding 5 µg/dL, which is considered a standard reference level. Nevertheless, the most recent information from the Centers for Disease Control and Prevention (CDC) indicates that no level of lead in blood is deemed safe (CDC, 2024).

South Africa is one of the few African countries that has tightened its regulations regarding lead in paints. Since 2009, the Hazardous Substances Act of South Africa has established a maximum permissible lead level (MPLL) of 600 ppm of lead in household paint. Figure 2 displays a map of African countries with and without lead paint regulations as of December 2021 (WHO, 2021). This regulatory action aligns with Sustainable Development Goal 4 (quality education) by ensuring that children are protected from lead exposure, which can have detrimental effects on their cognitive development and academic performance.

Additionally, cadmium exposure is associated with damage to the kidneys and bones, and it is classified as a possible human carcinogen, notably increasing the risk of lung cancer. While mercury is harmful in both its inorganic forms and elemental, it is particularly concerning in its organic compounds, such as methylmercury. Methylmercury accumulates in the food chain, especially in predatory fish from lakes and oceans, and represents a major pathway for human exposure (Abd Elnabi et al., 2023; Briffa et al., 2020; Jadaa & Mohammed, 2023; Kafayat Kehinde Lawal et al., 2021; Mahurpawar, 2015; Mitra et al., 2022).

This study assesses the lead and other heavy metals (HMs) content in South African paints using ICP-MS to understand their environmental impact and enhance future traceability. It innovatively uses lead isotopic ratios and REE patterns to create paint fingerprints, aiding traceability when necessary. Lead isotopic ratios can trace the sources of lead pollution in the environment, helping identify potential contamination sources and understand lead pathways. Additionally, examining the REE pattern normalized to chondrite values provides insights into environmental pollution origins. Comparing these patterns with known sources allows scientists to pinpoint pollution sources, aiding environmental protection (Moody et al., 2014). The research contributes to understanding the chemical composition of South African paints, highlighting their compliance with regulations and offering insights into environmental health. The findings enhance paint traceability efforts, ensuring regulatory compliance and environmental safety.

Sampling, samples’ preparation and samples’ digestion

We visited major building hardware shops in Mahikeng, the capital of North West Province, South Africa, where we purchased commonly used six (6) brands of paint (labelled as SF-A – SF-F), and three brands of paint tints (labelled as SF-G – SF-I). We sampled the bright colors of each brand, having 30 samples, labelled as SF-A1, 2, 3…. SF-I1, 2, 3… respectively. Figure 3 presents the picture of the purchased paints and paint tints.

A single-use clean stirrer was used to thoroughly stir each paint in its can. Subsequently, a single-use clean brush was used to apply each sample to clean pre-labelled polycarbonate plastic (A4 size). The applied samples were dried at room temperature, then each sample was scraped and placed in an individual labelled zip-lock plastic bag.

Each paint scraping was digested at 95^oC in a heated block for 15 minutes with 1.25 mL of HCl acid, then allowed to cool for 5 minutes. It was subsequently heated at 95°C for 15 minutes with 1.25 mL of HNO₃ acid (Kambarami et al., 2022; Siddiqui et al., 2023). It was allowed to cool and then diluted to a final volume of 50 mL.

ICP-MS measurement

Each final solution was analyzed for total Pb content, other heavy metals (HMs) levels, REE elements and Pb isotopic ratio using PerkinElmer NexION 2000 ICP-MS spectrometer at CARST in North-West University, Mahikeng Campus, South Africa.

ICP-MS determines the concentration of particular elements in a solution. In ICP-MS, the components of the sample are broken down into their atomic forms as a result of ionization in the argon plasma, which operates at temperatures ranging from approximately 6000 to 8000 K (Perkin, 2011; Wilschefski & Baxter, 2019). The positively charged ions are picked from the plasma and directed into the vacuum chamber of the mass spectrometer. Within the vacuum chamber, the charged ions are separated by filters before being detected and measured. Each sample is analyzed in two runs, with each run lasting approximately 60 seconds.

The TotalQuant method, along with PerkinElmer Pure Plus NexION Dual Detector Calibration Solution standard, was used to enhance the analytical accuracy of the results. Calibration for TotalQuant was performed using 200 µg/L concentrations of Al, Ba, Ce, Co, Cu, In, Li, Mg, Mn, Ni, Pb, Tb, U, and Zn (John et al., 2024). For quality control purposes, replicate samples were analyzed alongside the standard and blank solutions (Kamunda et al., 2016, 2018). Figure 3 shows the flowchart of the sample preparation and analysis.

Table 1 outlines the concentrations of the most prominent elements found in the samples. Figure 4 displays the lead concentration of each sample, excluding Sample SF-C3, which exhibited the highest concentration at 4.17 ppm. Table 2 lists other heavy metals (HMs) and some radionuclides detected in the samples. Additionally, Fig. 5 depicts the conventional plot of ²⁰⁸Pb/²⁰⁶Pb versus ²⁰⁷Pb/²⁰⁶Pb ratios for the samples, while Figs. 6, 7, and 8 show the REE patterns normalized to chondrite for various sample groups.

Lead (Pb) and other heavy metals (HMs) concentration

Among the 30 analyzed samples, the most prominent and nontoxic elements detected are Nitrogen (N), Calcium (Ca), Iron (Fe), Carbon (C), Aluminum (Al), and Phosphorus (P), with their concentrations ranging from 0 ppm to 584.74 ppm, 0.04 ppm to 171.78 ppm, 2.49 ppm to 14.95 ppm, 0 ppm to 3.67 ppm, and 0 ppm to 1.80 ppm, respectively. Table 1 shows the concentration range and the samples with the highest value for each of the elements.

The lead concentrations found in the samples range from 0 ppm to 4170 ppb, with a mean concentration of 139.79 ppb, and a median of 0.2 ppb, and sample SF-C3 having the highest concentration of 4.17 ppm. These concentrations are comfortably well below the 600 ppm Maximum Permissible Lead Levels (MPLL) allowed in paints in South Africa. Figure 4 shows the lead concentration of each of the samples, except for Sample SF-C3, which has the highest concentration of 4.17 ppm. This finding is consistent with the results of a study on six paints manufactured in South Africa and used in Botswana (Kambarami et al., 2022). Kambarami et al. (2022) reported on the lead (Pb) concentrations in paint samples from Zimbabwe and Botswana. In Zimbabwe, 70% of the samples had Pb levels exceeding 90 ppm, 60% were over 600 ppm, and 20% surpassed 10,000 ppm, with an average concentration of 4863 ppm, a median of 6900 ppm, and a maximum of 12,000 ppm. These concentrations significantly exceed the limits set by the World Health Organization and the United Nations. Conversely, in Botswana, the 19 samples tested were all below the laboratory detection limit, and of the seven brands analyzed, six were produced in South Africa, where a 600-ppm lead limit for paint is enforced.

The low lead concentration in the paints may reflect the efforts of various agencies such as the South African Paint Manufacturing Association (SAPMA), the South African Medical Research Council, and the promulgation of legislation in 2010 to control the use of lead in paint (Mathee, 2014; SAPMA, 2022). However, while the detected lead concentrations in the paints are lower than the MPLL, no BLL is considered safe.

In the analysis of the samples, it was found that besides lead (Pb), the samples also contained several other heavy metals (HMs). These heavy metals included Beryllium (Be), Chromium (Cr), Nickel (Ni), Arsenic (As), Cadmium (Cd), Antimony (Sb), Mercury (Hg), Barium (Ba), Strontium (Sr), Thorium (Th), and Uranium (U). Table 2 details the concentrations of various heavy metals (HMs) and radionuclides found in the samples. Beryllium (Be) exhibited a low mean concentration of 0.016 ppm, with a maximum value of 0.09 ppm in sample SF-G1. Chromium (Cr) showed significant variability, with a mean concentration of 52.636 ppm and a peak of 810.57 ppm in sample SF-C3. Nickel (Ni) also varied widely, averaging 17.317 ppm and reaching 322.27 ppm in sample SF-F1. Arsenic (As) levels were generally low, averaging 0.113 ppm and maxing out at 0.76 ppm in sample SF-D2. Cadmium (Cd) and Antimony (Sb) presented mean concentrations of 0.034 ppm and 0.660 ppm, respectively, with notable peaks in sample SF-C3. Mercury (Hg) levels were consistently low across all samples. Barium (Ba) and Strontium (Sr) showed broader ranges, with maximum concentrations of 516.44 ppm and 90.44 ppm, respectively. Thorium (Th) and Uranium (U) were present in low concentrations, with maximum values of 0.86 ppm and 0.45 ppm. The variability in these concentrations highlights localized contamination and suggests the need for targeted remediation in areas with high levels of specific elements. This analysis of heavy metals is important, as these elements, even at low levels, can have significant environmental and health implications. Understanding their presence and concentrations in the samples can help in assessing potential risks and implementing appropriate mitigation measures.

Table 1

The most prominent elements in the samples
s/n	Element	Concentration range (ppm)	Mean concentration (ppm)	Median (ppm)	Sample with Highest Value
1	Nitrogen (N)	0–27866.06	3219.173 ± 864.941	2673.758	SF-H1
2	Calcium (Ca)	0–584.74	90.509 ± 28.423	10.454	SF-H1
3	Iron (Fe)	0.04–171.78	13.427 ± 6.739	0.590	SF-G6
4	Carbon (C)	2.49–14.95	6.541 ± 0.595	5.403	SF-F1
5	Aluminum (Al)	0–3.67	1.067 ± 0.181	0.626	SF-C1
6	Phosphorus (P)	0–1.80	0.287 ± 0.079	0.113	SF-D2

Table 2

Other heavy metals (HMs) and some radionuclides found in the samples
s/n	Toxic Element	Concentration Range (ppm)	Mean Concentration (ppm)	Median (ppm)	Sample with Maximum Value
1	Beryllium (Be)	0–0.09	0.016 ± 0.005	0.000	SF-G1
2	Chromium (Cr)	2.02–810.57	52.636 ± 28.735	3.380	SF-C3
3	Nickel (Ni)	0–322.27	17.317 ± 11.287	0.195	SF-F1
4	Arsenic (As)	0–0.76	0.113 ± 0.027	0.050	SF-D2
5	Cadmium (Cd)	0–0.49	0.034 ± 0.018	0.000	SF-C3
6	Antimony (Sb)	0–19.27	0.660 ± 0.064	0.000	SF-C3
7.	Mercury (Hg)	0–0.02	0.010 ± 0.001	0.010	SF-A1
8	Barium (Ba)	0.01–516.44	33.821 ± 20.273	1.035	SF-I5
9	Strontium (Sr)	0–90.44	18.058 ± 4.449	5.355	SF-C3
10	Thorium (Th)	0–0.86	0.223 ± 0.050	0.070	SF-G5
11	Uranium (U)	0–0.45	0.139 ± 0.014	0.135	SF-G4

Fingerprint development

Figure 5 displays the conventional plot of ²⁰⁸Pb/²⁰⁶Pb versus ²⁰⁷Pb/²⁰⁶Pb ratios for the samples. The plot reveals variations in the ratios of different lead isotopes (²⁰⁷Pb and ²⁰⁸Pb) to the common lead isotope ²⁰⁶Pb, which are crucial for environmental studies aiming to understand the sources and histories of lead in the samples. These variations indicate diverse lead sources or processes that have influenced the lead isotopic composition in the samples. For instance, samples with higher ²⁰⁷Pb/²⁰⁶Pb ratios may have different sources or histories compared to those with lower ratios. Notably, Sample SF-H3 exhibits extremely high isotopic ratios (5.399 for ²⁰⁷Pb/²⁰⁶Pb and 6.264 for ²⁰⁸Pb/²⁰⁶Pb), suggesting a unique lead source or a process that significantly altered its lead isotopic composition. By comparing these ratios with known values from different lead sources, it is possible to potentially identify the origins of the lead, aiding in tracing the sources of lead pollution in the environment. The correlation coefficient of the trend line is 0.92.

The normalized Rare Earth Element (REE) concentrations in the samples (SF-A1 to SF-I5) can offer valuable insights into the geological and environmental conditions of the sampled locations (Moody et al., 2014). The REE concentrations in these samples exhibit diverse patterns, reflecting the complex interplay of geological processes and environmental factors.

In Fig. 6, samples SF-A1 and SF-A2 show low concentrations of most REEs, while SF-A3 and SF-A4 exhibit higher concentrations (enrichment) of Nd compared to the other samples. With slight variations in cerium (Ce), praseodymium (Pr), and neodymium (Nd) concentrations. These samples suggest a similar geochemical signature, possibly indicating a common source. The REE concentrations in samples SF-B1, SF-B2, and SF-B3 of Fig. 7 show similar patterns, with relatively low concentrations across most REEs. However, there are slight variations in the concentrations of certain elements, indicating potential differences in the source or geological processes affecting these samples. Samples SF-C1, SF-C2, and SF-C3 exhibit varying concentrations of REEs, with SF-C3 showing slightly higher concentrations of Ce, Pr, and Nd compared to the other two samples. These variations suggest different geochemical conditions or sources for these samples. Samples SF-D1 to SF-D4 show varying patterns in REE concentrations, with SF-D1 and SF-D2 exhibiting higher concentrations of La, Ce, Pr, and Nd compared to SF-D3 and SF-D4. This indicates potential enrichment of these Light REE elements in SF-D1 and SF-D2, as in Fig. 7. In Fig. 8, samples SF-E1, SF-F1, SF-G1 to SF-G6, SF-H1 to SF-H3, and SF-I1 to SF-I5 also exhibit distinct patterns in REE concentrations, indicating a wide range of geological and environmental influences across the sampled locations. Figure 6, 7, and 8 display the normalized Rare Earth Element (REE) plots for three brands of paint samples, showing a consistent pattern among each brand's samples, with Nd, Gd and Tb, and Gd anomalies, respectively. The HREE (Tb – Lu) are not enriched nor depleted in all samples.

The findings of this study provide valuable insights into the environmental and health implications of lead and other heavy metals (HMs) in household paints. The study reveals that lead concentrations in the analyzed samples from South Africa are below the Maximum Permissible Lead Levels (MPLL), as mandated by the South Africa’s Hazardous Substances Act. This indicates compliance with regulatory measures and reflects the effectiveness of initiatives aimed at reducing lead exposure. Furthermore, the study highlights the presence of other HMs in paints, including Beryllium, Chromium, Nickel, Arsenic, Cadmium, Antimony, Mercury, as well as some radionuclide, Barium, Strontium, Thorium, and Uranium. While they were found at relatively low levels in the samples, their presence underscores the importance of monitoring and regulating HMs in paints to protect human health and the environment. The development of fingerprints using lead isotopic ratios and Rare Earth Element (REE) patterns is a novel approach that enhances traceability efforts and provides valuable information on the sources of lead and other HMs in paints. By comparing these patterns with known sources, it is possible to identify potential contamination sources and understand the pathways of heavy metal pollution. Overall, the study emphasizes the need for continued monitoring and regulation of heavy metals in paints to ensure environmental and human health protection. The findings can inform policy-making and regulatory efforts to reduce heavy metal exposure and enhance environmental sustainability. It highlights the need for sustainable practices in paint manufacturing and usage to reduce the environmental and health impacts of heavy metals.

All authors have read, understood, and have complied as applicable with the statement on "Ethical responsibilities of Authors" as found in the Instructions for Authors

Conflict of interest

The authors declare no competing interests

Funding

This research was conducted under the Postdoctoral Research Fellowship (PDRF) with funding from the NWU PDRF Fund NW.1G01487

Author Contribution

SFO: Conceptualization, sample collection and preparation, methodology, data analysis, result interpretation, manuscript writing; SOOJ: Sample collection and preparation, methodology, content review; TGK: Guidance, methodology, ICP-MS analysis, content review; OFO: Sample collection and preparation (other African countries), content review; JM: Sample collection and preparation; HOS: Sample collection and preparation (other African countries), content review; MM: funding acquisition, recruitment, supervision, sample collection, methodology, results analysis, content review.

Acknowledgments

The authors thank the entire staff of Center for Applied Radiation Science and Technology (CARST), North-West University, Mahikeng Campus, South Africa under the Directorship of Prof. Hellen Drummond. CARST admin officer Ms. Monde Kakula and Technologist Ms. Desiree Mokgele are also highly appreciated.

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Assessing heavy metals and developing a fingerprint for Mahikeng paints using ICP-MS analysis: implications for environmental health

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