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. 2022 Jan 8;24(1):100. doi: 10.3390/e24010100

Thermodynamic Rarity Assessment of Mobile Phone PCBs: A Physical Criticality Indicator in Times of Shortage

Jorge Torrubia 1,*, Antonio Valero 1, Alicia Valero 1
Editors: Jean-Noël Jaubert1, Attila R Imre1
PMCID: PMC8774590  PMID: 35052126

Abstract

Rising prices in energy, raw materials, and shortages of critical raw materials (CRMs) for renewable energies or electric vehicles are jeopardizing the transition to a low-carbon economy. Therefore, managing scarce resources must be a priority for governments. To that end, appropriate indicators that can identify the criticality of raw materials and products is key. Thermodynamic rarity (TR) is an exergy-based indicator that measures the scarcity of elements in the earth’s crust and the energy intensity to extract and refine them. This paper uses TR to study 70 Mobile Phone (MP) Printed Circuit Boards (PCBs) samples. Results show that an average MP PCB has a TR of 88 MJ per unit, indicating their intensive use of valuable materials. Every year the embedded TR increases by 36,250 GWh worldwide -similar to the electricity consumed by Denmark in 2019- due to annual production of MP. Pd, Ta and Au embedded in MP PCBs worldwide between 2007 and 2021 contribute to 90% of the overall TR, which account for 75, 600 and 250 tones, respectively, and increasing by 11% annually. This, coupled with the short lifespan of MP, makes PCBs an important potential source of secondary resources.

Keywords: thermodynamic rarity, resource scarcity, critical raw materials, printed circuit boards, mobile phones

1. Introduction

The whole world is experiencing soaring energy and raw material costs. Europe is particularly vulnerable to this situation which must import a large part of the raw material domestically consumed by industry and households [1]. Rising energy prices -driven by fossil fuel prices [2]- (electricity [3,4,5,6], natural gas [7] and gasoline and diesel [8]), food [9,10] (fertilizers [11]) and livestock feed [12]), shipping [13,14] and even the lack of microchips for factories [15,16], are examples of this. These supply issues occur when the transformation to a low-carbon economy driven by renewables, electric vehicles, and digitization is beginning to accelerate. This situation could jeopardize the transition since a low-carbon economy requires a large quantity and variety of raw materials. For example, to produce one gigawatt (GW) of electrical power equivalent to that which a natural gas-fired power plant could supply would imply the use of approximately 160,000 tons of steel, 2000 of copper, 780 of aluminum, 110 of nickel, 85 of neodymium and 7 of dysprosium for its construction [17]. These are not negligible amounts if it is estimated that in the future, the power provided by wind turbines in 2050 could be around 2200 GW [18].

Another example is that demand for some minerals for batteries could increase dramatically by 2040 -with respect to 2020-lithium 42 times, cobalt 21 times, nickel 19 or Rare Earth Elements (REE) 7, as the International Energy Agency (IEA) warns [19]. Thus, the use of scarce minerals -needed in a low-carbon economy- could pose a problem for future generations due to their eventual depletion and unavailability in the future [20]. Furthermore, these raw materials are mainly extracted from mines that need fossil fuels to operate. The IEA’s World Energy Outlook 2021 indicates that oil and natural gas production could fall by 8–9% per year without new investments [2]. They have fallen from $779 billion in 2014 to $328 billion in 2020 [21], i.e., they have halved in 6 years. The combination of these factors could lead to bottlenecks of raw materials needed for decarbonization. Therefore, it is essential to strengthen raw material supply chains seeking alternative sources such as e-waste. According to Henckens 2021 [20], if the most stringent resource-saving measures were applied, it would be possible to extend the depletion periods of certain materials required for the energy transition by four times, even if the global service level increases.

This paper examines the raw materials embedded in printed circuit boards (PCBs) in Mobile Phones (MP) as a potential source of secondary resources. These devices have become, in recent years, irreplaceable devices for communication worldwide. The rapid growth in their sales evidences this. MP sales began to proliferate from 2009, reaching approximately constant annual sales of 1.5 billion phones between 2016 and 2020. Resulting in cumulative sales between 2007 and 2020 of almost 14 billion phones and almost doubling the world’s population [22]. The large number of MP, coupled with their short lifespan of around four years [23], contributes to the continuous increase of e-waste, which according to some projections, reach 52.2 million tons in 2021 [24] with an annual growth of 3–5%, a rate three times faster than the increase of municipal solid waste [25]. The most polluting part of a MP is the Printed Circuit Board (PCB) it contains. PCBs account for more than 70% of the carbon footprint of production [26]. In addition, it is the most heterogeneous and complicated fraction [24] as it is composed of a high diversity of elements -more than 40- and elemental concentrations [27]. Some of these elements -such as Pd, Ga or Ta- are scarce in nature [28] or a few countries control their production. Such is the case of Rare Earths Elements (REE), mainly controlled by China.

This issue has been studied by the European Commission (EC), which has been drawing up a list of Critical Raw Materials (CRMs) for the EU every three years since 2011 [29]. The EC criteria point to the economic importance for the EU economy and the supply risk of raw materials to assess criticality [28]. Such criteria are mainly based on geopolitical and economic aspects that are variable over time. For example, Si has soared 300% in less than two months [30], the volatility of Pd has been evidenced by the International Energy Agency [19], the price of Cu has increased 300% in 15 years [31] or REE prices increased 10-fold between 2009 and 2011 and then fell [32]. Moreover, the EC list has not stopped growing, the 2014 list contained 20 CRMs, the 2017 list 26 and the 2020 list 30 [33]. In addition, the list could expand in the future due to these price trends-characteristic in times of shortage-and the growing demand for metals needed for the energy transition [19].

In addition to economic and geopolitical factors, the criticality of an element is determined by its geological scarcity, as the first link in the supply chain of most CRM is mining, which will be one of the decisive factors for the success of renewable transition [19]. As mines become depleted and their ore grade decreases, the energy costs to extract the metal increase exponentially [34,35]. In the limit, a complete exhaustion of all mines would imply that the planet’s mineral wealth would be dispersed, reaching the maximum level of entropy. This state of the planet has been called Thanatia by Valero and Valero [36]. Using this reference, Thermodynamic Rarity (TR) is presented as an exergy-based indicator capable of measuring the thermodynamic criticality of raw materials based on their geological scarcity and the energy intensity required to extract, beneficiate, and refine commodities. Thus, TR is a long-term indicator decoupled from political and economic factors but constrained by mining technology and geological knowledge of the earth’s crust. More information about this indicator and its applications can be found in the following references [37,38,39,40]. TR has been proposed previously as a criticality indicator. For example, Calvo et al., 2018 [28] proposed to add Mo, Te, li, Ta, and V to the list of the 2014 EC CRMs due to their geological scarcity measured by TR. The last three have been added to the 2020 list of these elements. In addition, this indicator has already been successfully used in the study of Electrical and Electronic Equipment [41] and vehicles. Vehicle papers concluded that although Fe, Al and Cu contribute to more than 90% of the car by weight, they only account for 60% of the TR [42] and that many high TR elements end up downcycled as part of alloys or in landfills. Downcycled elements represent 4.5% of the vehicles, while in TR terms, it would be 27% [43]. Currently, EC legislation for End of Life Vehicles requires the recovery of 95% of the vehicle by weight. This can be met by recovering major metals, yet the minor ones become lost or downcycled, losing their functionality. Horta Arduin et al., 2020 [44] has also highlighted this problem in the case of display waste. They state that there is a contradiction between the EC criteria, which on the one hand is concerned with the criticality of CRMs through the publication of lists, but on the other hand, the WEEE recycling regulations focus on weight, causing many critical elements to be lost due to their low contribution in weight. This makes new indicators necessary to reinforce current regulations.

This paper is structured as follows. First, TR indicator is explained. Second, the sources used to calculate the composition of the MP PCBs, the assumptions for calculating the TR and the estimation of resources embedded worldwide are shown. Third, the results of the mass composition, TR and resources worldwide are presented. Finally, the main conclusions are discussed.

2. Materials and Methods

2.1. Thermodynamic Rarity Indicator

TR is an indicator, based on exergy, used to measure the thermodynamic criticality of raw materials, depending on their scarcity in the earth’s crust and the energy intensity associated with mining, beneficiation, and refining processes. Exergy is a property of a system relative to an associated reference state. It is the maximum work a system can deliver as it interacts with another large, but real, system, namely, a reservoir. Such a reservoir attracts the system toward degradation or entropy creation. The reference state selected for the exergy assessment of minerals is a planet, called “Thanatia” (from Greek Thanatos, meaning “death”) with the following characteristics [39]:

  • Crust: there are no concentrated mineral deposits (the upper continental crust can be approximated to the average mineralogical composition of the current earth’s crust), fossil fuels have been depleted, and fertile soils are entirely degraded.

  • Hydrosphere: its composition can be approximated to seawater since freshwater constitutes about 2.5% of global water, of which the most important part is composed of glaciers and ice sheets (68.7%) and groundwater (30.1%).

  • Atmosphere: CO2 concentration is comparable to the complete burning of all remaining fossil fuels.

This imaginary state of the planet does not need to be “reachable”, but it is a baseline to assess the quality of any resource physically. It further allows us to objectively identify which resource is closer to depletion in the race to exhaustion. Any mineral resource with a concentration higher than that found in Thanatia has exergy, and therefore, its quality can be quantified in energy terms [39]. TR incorporates two aspects. The first is the embedded exergy cost (kJ), i.e., the useful energy required to extract and process a given mineral from the cradle to the gate (i.e., until it becomes a raw material for the manufacturing industry). The second is, in fact, an avoided cost for having minerals concentrated in mines and not dispersed throughout the crust (i.e., it can be seen as a natural bonus). As mines become depleted, it becomes exponentially harder to obtain commodities (embedded costs increase), whereas the bonus reduces. This bonus is calculated as a hypothetical exergy cost required if the given mineral would be restored to its initial composition conditions and concentration in the original mines from an utterly dispersed state, i.e., its state in Thanatia. This is the exergy replacement cost (ERC) (kJ) and can be seen as a grave-to-cradle-approach [36] or as a natural avoided exergy cost, i.e., as a natural bonus. Thus, the TR is presented as a physical indicator, stable over time, based on thermodynamic fundamentals. However, it is conditioned by mining technology, as it could reduce the exergy costs of mineral extraction and the knowledge of the earth’s crust that would modify the composition established for Thanatia. Another advantage is that it allows classifying the elements in order of criticality since each element has a unique value, measured in exergy terms.

TR values (Ri) of the analyzed elements, measured in GJtoni are shown in Table 1 [28]. Nevertheless, TR values could be higher than those used. As an example, Palacios et al. [45] obtained TR values 2 to 3 orders of magnitude higher than previous values for Cu and Au, using metallurgical process simulation, more specifically the HSC Chemistry software.

Table 1.

Embedded exergy, exergy replacement cost and thermodynamic rarity of the chemical elements that compose a mobile phone PCB. * Average between ores [28].

Element (ore) Embedded Exergy
(GJ/ton)
Exergy Replacement Cost
(GJ/ton)
Thermodynamic Rarity
(GJ/ton)
Ag 1566 7371 8938
Al (Bauxite-Gibbsite) 54 627 682
As (Arsenopyrite) 28 400 427
Au 110,057 553,250 663,308
Ba 1 38 39
Be (Beryl) 457 253 710
Bi (Bismuthinite) 56 489 545
Cd (Greenockite) 542 5898 6440
Ce (Monazite) 523 97 620
Co (Linnaeite) 138 10,872 11,010
Cr (Chromite) 36 5 41
Cu (Chalcopyrite) 57 292 349
Fe (Hematite) 14 18 32
Ga (in Bauxite) 610,000 144,828 754,828
Gd (Monazite) 3607 478 4085
Ge (in Zinc) 498 23,750 24,248
Hf 11,183 21,814 32,997
Hg (Cinnabar) 409 28,298 28,707
In (in Zinc) 3320 360,598 363,917
K (Sylvite) 2 665 667
La (Monazite) 297 39 336
Li (Spodumene) 433 546 979
Mg (from Ocean) 10 26 36
Mn (Pyrolusite) 58 16 74
Mo (Molibdenite) 148 908 1056
Na (Halite) 43 44 87
Nd (Monazite) 592 78 670
Ni (Pentlandite and Garnierite) * 265 465 729
P (Apatite) 5 0 5
Pb (Galena) 4 37 41
Pd 583,333 8,983,377 9,566,710
Pr (Monazite) 296 577 873
Pt 291,667 4,491,690 4,783,357
Sb (Stibnite) 13 474 487
Si (Quartz) 77 1 77
Sn (Cassiterite) 27 426 453
Sr 72 4 78
Ta (Tantalite) 3091 482,828 485,919
Ti (Ilmenite and Rutile) * 196 7 203
W (Scheelite) 594 7430 8024
Y (Monazite) 1198 159 1357
Zn (Sphalerite) 42 155 197
Zr (Zircon) 1372 654 2026

2.2. Mobile Phone PCB Data: Composition, Thermodynamic Rarity Calculation and Resources Embedded Worldwide

PCB composition has been obtained by reviewing the literature. A total of 70 samples were taken from Chancerel et al., 2009 [46] (3 samples), Kasper et al., 2011 [47] (3 samples), Oguchi et al., 2011 [48] (2 samples), Yamane et al., 2011 [49] (1 sample), Silvas et al., 2015 [50] (1 sample), Ueberschaar et al., 2017 [51] (1 sample), Ueberschaar et al., 2017 [52] (2 samples), Arshadi et al., 2018 [53] (1 sample), Holgersson et al., 2018 [54] (10 samples), Li et al., 2018 [24] (1 sample), Gu et al., 2019 [27] (12 samples), Korf et al., 2019 [55] (14 samples), Sahan et al., 2019 [25] (19 samples). All data have been transformed to mg element per kg PCB and the complete results have been compiled in Appendix A. Analyzed MP were manufactured between 2004 and 2014. PCBs were subjected to mechanical processing (shredding, comminution or milling), and then the resulting powder was analyzed using different techniques such as ICP-AES, ICP-OES, ICP-MS o XRF.

The TR of a mobile phone (MP) PCB has been calculated through Equation (1). First, the TR of a kg of PCB is calculated (in parentheses). To do this, the product of the TR of an element (Ri) by its concentration in the PCB is done and then the units of kg of PCB are transformed into units of MP.

RPCB(unit)=(i=1nRi·mgikgPCB·11e9) ·kgPCBkgMP·kgMPUnitMP (1)

Therefore, it is necessary to know its average weight and the percentage of PCBs it contains in relation to its weight. In this paper, as indicated in Equation (1), an average phone weight of 100 g and a PCB percentage by weight of 20% have been used to obtain conservative results. Table 2 shows the percentage of PCBs in phones according to different references. Equation (1) is also used to calculate the contribution of each element to the total TR to analyze the thermodynamic criticality of each element.

Table 2.

Percentage by weight of PCB in a Mobile Phone.

Source [24] [46] [54] [48] [51] [56] [57]
Minimum 20% 22% 21% 12.6% 29.5% 21% 21.1%
Maximum 30% 30.3%

To estimate the mass of elements embedded in MP PCBs worldwide, the annual sales of 2020 -around 1.5 billion- and the cumulative sales between 2007 and 2021 -around 14.8 billion units- are taken [22].

Finally, the ratio between the amount of elements embedded in MP PCBs worldwide and the annual extraction of the elements is calculated. For this purpose, the quantity of each element is divided by its extraction. Thus, two percentages are obtained depending on the number of MP considered. On the one hand, the cumulative quantity is considered, i.e., 14.8 billion units between 2007 and 2021; and, on the other hand, the annual sales are considered, i.e., 1.5 billion units. Thus, the first percentage represents the annual production that could be provided if that element were recovered from all the accumulated PCBs. In addition, the second percentage of annual production could be covered with the PCBs of one year. In other words, it would be approximately the percentage of the annual production that is used to produce MP PCBs. The extraction data for the elements were obtained from the U.S. Geological Survey 2021 commodity summaries [58]. In 2020, 210 tons of Pd, 1700 tons of Ta, 3200 tons of Au, 300 tons of Ga, 20,000,000 tons of Cu, 170 tons of Pt and 900 tons of In were mined.

3. Results

3.1. Composition and Thermodynamic Rarity of Mobile Phone PCBs

The 70 MP PCBs samples reviewed are composed of 55 different chemical elements, of which 31 are considered as CRMs by the EC (Figure 1). Although the EC list contains 30 commodities, some of them are groups of elements such as light REE or platinum group metals (PGM), so the number obtained is greater than 30. Taking this into account, 25 elements in the MP PCB are considered critical by the EC. Nevertheless, the contribution by weight of these elements to the total PCBs is very different. Figure 2a,b shows the results of the mass contribution of each element. As can be seen, more than 90% of the weight of PCBs is made up of 8 elements: Cu, Si, Fe, Br, Sn, Ni, Al and Zn, being two CRMs according to the EC: Si and Al. Using the CE criterion, the remaining 47 elements constitute 10% of the overall weight, concentrating up to 23 CRMs. Therefore, most of the critical elements are characterized by low mass concentrations.

Figure 1.

Figure 1

Periodic table showing the elements embedded in Mobile Phone PCBs. Elements considered critical by EC are highlighted in red.

Figure 2.

Figure 2

Results of composition (a,b) and thermodynamic rarity (c,d) per element.

To measure criticality, this paper uses the TR indicator. Thus, Figure 2c shows the results of the TR contribution of each element in kJ per unit of MP and Figure 2d the results in percentage, according to the data and assumptions outlined in Section 2.2. If the TR of an element is unknown, it has been counted as 0, as for Te or Br (see Table 1). Taking TR as a criterion, the results are radically different. There are now 3 elements that contribute to almost 90% of the TR: Pd, Ta and Au, 4 others that account for 8%: Ga, Cu, Pt, and In, and remaining 48 for only 2%. Thus, seven elements account for 98% of the TR, being all of them CRMs according to the EC except Au and Cu -the most abundant in PCBs-.

Summing the contribution of each element as shown in Equation (1), the results indicate that the TR of a PCB is 88 MJ per MP unit. This result does not include other parts of the MP, such as the display, camera, or battery, so the TR of the complete MP is higher than obtained. Considering that between 2016 and 2020 mobile sales stagnate at around 1.5 billion mobiles per year (Figure 3b), the TR embedded in MP PCBs worldwide would increase by 1.305·1011 MJ o 36,250 GWh per year, an amount comparable to the electricity consumed by Denmark in 2019 [59].

Figure 3.

Figure 3

Mobile Phone sales worldwide since 2007. (a) Annual sales. (b) Cumulative sales [22].

3.2. Resources Embedded in Mobile Phone PCB Worldwide

In order to estimate the amount of resources embedded in the PCBs of MP, two sources of information have been taken. On the one hand, the number of MP sold between 2007 and 2021 is 14.8 billion, doubling the world population (Figure 3a). On the other hand, the number of MP put on sale annually considered is 1.5 billion units, which since 2016 has stagnated as shown in Figure 3b.

Figure A1 (Appendix A) shows the results for each element, and Table 3 shows the results for the highest TR (rows A and B). It indicates that these elements’ quantity embedded in MP PCBs increases by approximately 11% each year.

Table 3.

Annual increase in resources embedded in MP PCBs worldwide. Comparison between annual element production and quantity embedded in Mobile Phone PCBs. Extraction data from reference [58].

Elements Pd Ta Au Ga Cu Pt In
(A) Tons embedded [Tons] 74 602 254 46 98,423 5.2 25
(B) Tons embedded 2020 [Tons/yr] 8 64 27 5 10,500 0.6 2.7
(A)/(B) Annual increase [%] 10.8% 10.6% 10.6% 10.9% 10.7% 11.5% 10.8%
(C) Annual primary extraction 2020 [Tons/yr] 210 1700 3200 300 20,000,000 170 900
(A)/(C) [%] 35% 35% 7.9% 15.3% 0.49% 3.1% 2.8%
(B)/(C) [%] 3.8% 3.8% 0.8% 1.7% 0.05% 0.4% 0.3%

This strong annual increase and the short lifespan of the MP -of around four years [23]- make such devices an interesting source of valuable raw materials. Accordingly, we now explore how much of the annual production could -theoretically- be covered by the resources embedded in the MP PCBs. Table 3 shows the annual primary extraction of each element in row C. In the last two rows, the ratios between row A and C, and, B and C are calculated. These ratios indicate the percentage of a year’s global extraction that could be replaced if all of the embedded mass between 2007 and 2021 (A/C) could be recovered, or if all of the mass produced in one year could be recovered (B/C). It is important to emphasize that recovering the entire PCBs from MP is impossible. For example, in Reuter et al., 2018 [60], they only recover 22% of the metals from a MP in the best case. However, they achieve very high recovery rates for some elements such as Au (90–100%), Pd (10–100%) or Ga (80–90%), but much lower for others -Ta (0–10%). Another example is found in Valero-Navazo et al., 2014 [61], in which Pd, Au, Ag, Cu, Ni, Pb and Sn are recovered with recovery rates between 80 and 95%. As can be observed, the elements with higher TR are not always recovered, for example, Valero-Navazo et al., 2014 does not recover Ta or Ga, while in Reuter et al., 2018, the recovery efficiencies of Pd and Ta are 10% and Ga 80% in the worst cases. Therefore, the percentages in Table 3 should be interpreted as a theoretical maximum -unreachable- or, from another perspective, as the percentage of the extraction hoarded by the MP PCBs. In addition to the physical limitations, separate collection rates are very low, ranging from 2 to 16% [61], so high recovery rates are still far from being achieved.

Coincidentally, most elements with the highest ratios are those with the highest TR, i.e., Pd, Ta, Ga, Au, Pt and In, except for Cu. This may be due to the relationship between geological scarcity and low extraction rates. However, this should not necessarily be the case, as it is a result that depends on the composition of the devices to be analyzed. What is important to note is that the recovery of these elements should be prioritized, as they are not only the most critical from the point of view of TR, but if they were recovered, they could make an important contribution to world production. For example, in the case of Pd and Ta, their contribution to world production could theoretically reach 35% if the tons incorporated between 2007 and 2021 could be fully recovered. This figure would be 15% and 8% for Ga and Au, respectively. Considering only the tons embedded in a year, the contribution would drop to 3.8% for Pd and Ta; and to 1.7% and 0.8% for Ga and Au, respectively.

4. Conclusions

The volatility and increase in raw material prices and even the unavailability of some components may jeopardize the energy transition. The search for secondary raw materials and their recovery becomes necessary to alleviate this shortage situation, which could worsen in the future due to ore grade decline, among other factors. In addition, reducing primary extraction would provide other benefits such as less environmental deterioration and greater availability of resources for future generations. To this end, identifying new sources of secondary resources is essential.

This article analyzes the PCBs of the MPs, through the TR. These devices are promising candidates due to their large sales and their short useful life. The use of TR-a physical indicator based on thermodynamics allows obtaining stable values of material criticality in the medium to long term, which can only be influenced by mining technology and knowledge of the earth’s crust. This physical point of view is an essential reinforcement of the criticality assessment of any government, based on the importance of the elements for the given economy’s region and the supply risks. Being decoupled from these time-varying factors, the TR can help establish long-term policies. Another advantage of the TR is that it allows to classify and quantify the elements in order of criticality, as each element has a unique value. This helps identify products and parts with a high content of critical and valuable materials and is helpful for eco-design.

The results show that Pd, Ta, Au, Ga, Cu, Pt and In are the highest contribution to TR in MP. All are considered critical by the EC, except for Cu and Au. In addition, a considerable percentage of the world’s production of Pd, Ta, Ga and Au is hoarded in MP PCBs. These results show the need for the recovery of these elements, not only for the conservation of TR, (i.e., of the exergy embedded in the most geologically scarce elements) but also for their significant contribution to the world’s commodity production. However, 100% recovery of the resources embedded in the equipment is impossible, so to achieve the maximum recovery rate, it is necessary to develop and promote recycling processes that allow it. However, these processes are energy-intensive and require further thermodynamic analysis. This will be analyzed in a forthcoming paper.

Appendix A

Table A1.

Samples composition (from Ag to Cu) in mg of element per kg of PCB.

References (mg/kg PCB) Ag Al As Au Ba Be Bi Br Ca Cd Ce Cl Co Cr Cu
Chancerel et al., 2009 2244 50
Chancerel et al., 2009 3573 368
Chancerel et al., 2009 5540 980
Kasper et al., 2011 600 3100 600 395,600
Kasper et al., 2011 600 9900 1000 383,300
Kasper et al., 2011 500 6100 900 378,100
Oguchi et al., 2011 2400 67,000 4700 400 100 96,000
Oguchi et al., 2011 3800 15,000 1500 19,000 440 280 330,000
Yamane et al., 2011 2100 2600 344,900
Silvas et al., 2015 2100 2600 1600 900 355,000
Ueberschaar et al., 2017 (a)
Ueberschaar et al., 2017 (b) 1580 19,741 0.0438 529 14,778 6 0.044 38,851 0.044 0.071 0.044 255,100
Ueberschaar et al., 2017 (b) 1597 42,979 21 1038 19,466 66 66 27,837 2 7 253 464,000
Arshadi et al., 2018 1470 57,930 480 3990 37,950 32,760 5310 1590 210,000
Holgersson et al., 2018 2640 22,736 93.3 1051 2152 98.8 39.6 1556 2.1 952.9 342,667
Holgersson et al., 2018 2773 23,003 141 1083 2662 138 60.6 762 1306.7 395,000
Holgersson et al., 2018 2500 1200 1 2000 250,000
Holgersson et al., 2018 4000 400 1 3000 200,000
Holgersson et al., 2018 4000 800 1 700 200,000
Holgersson et al., 2018 5000 1100 45 4000 120,000
Holgersson et al., 2018 5081 19 5 801 272,402
Holgersson et al., 2018 2100 10 344,900
Holgersson et al., 2018 6091 1591 590,909
Holgersson et al., 2018 3301 570 234,700
Li et al., 2018 1380 10,000 350 130,000
Gu et al., 2019 5200 600 273,700
Gu et al., 2019 600 800 385,700
Gu et al., 2019 1000 200 566,800
Gu et al., 2019 500 100 398,600
Gu et al., 2019 2300 1400 428,000
Gu et al., 2019 300 900 417,900
Gu et al., 2019 300 100 360,000
Gu et al., 2019 1100 100 408,000
Gu et al., 2019 3400 319,500
Gu et al., 2019 300 200 657,400
Gu et al., 2019 80,500
Gu et al., 2019 1300 1000 479,000
Korf et al., 2019 8118 14,949 18 10,739 5.6 33,901 5.6 64 1792 333,228
Korf et al., 2019 4125 18,333 28 6768 5.6 40,984 5.6 39 139 232,163
Korf et al., 2019 2100 2600 344,900
Korf et al., 2019 600 3100 600 395,600
Korf et al., 2019 600 9900 1000 383,300
Korf et al., 2019 500 6100 900 378,100
Korf et al., 2019 2400 67,000 4700 400 100 96,000
Korf et al., 2019 3800 15,000 1500 19,000 440 280 330,000
Korf et al., 2019 1000 32,700 600 1600 56,700 45,200 1300 200 241,900
Korf et al., 2019 430 25,200 145 1280 18,000 1.8 53.8 9480 1.7 1.7 500 123 371,000
Korf et al., 2019 310 10,600 258 1410 19,000 0.8 39 12,300 0.6 4.9 540 42,000 306,000
Korf et al., 2019 370 17,300 111 552 20,300 15.5 8340 0.9 2.1 270 650 494,000
Korf et al., 2019 2640 22,736 93.3 1051 2152 98.8 39.6 1556 2.1 952.9 342,667
Korf et al., 2019 2773 23,003 141 1083 2662 138 60.6 762 1306.7 395,000
Sahan et al., 2019 2500 8900 2400 140 190 324,700
Sahan et al., 2019 1700 13,200 650 50 110 370,400
Sahan et al., 2019 2000 10,400 2900 270 3900 227,500
Sahan et al., 2019 2000 11,500 1400 110 330 378,000
Sahan et al., 2019 4700 12,900 1300 190 510 404,000
Sahan et al., 2019 8300 10,700 1800 110 130 206,000
Sahan et al., 2019 5100 11,800 1600 120 290 287,500
Sahan et al., 2019 3700 14,900 1500 370 460 305,200
Sahan et al., 2019 3200 16,600 820 230 170 451,400
Sahan et al., 2019 3900 16,300 1100 700 440 313,100
Sahan et al., 2019 2600 20,100 530 50 440 397,700
Sahan et al., 2019 5900 15,900 1600 300 140 282,400
Sahan et al., 2019 1700 19,700 170 100 15,000 409,800
Sahan et al., 2019 6100 378,000
Sahan et al., 2019 2100 2600 344,900
Sahan et al., 2019 8500 17,700
Sahan et al., 2019 1060 65 408,000
Sahan et al., 2019 540 43 398,600
Sahan et al., 2019 4700 15,200 1400 200 400 326,200
Average 2557 17,628 148 859 9626 69 138 47,325 18,228 6 3 3305 199 2985 332,464
St deviation 1886 15,301 137 616 7663 59 178 13,258 17,311 13 3 2835 174 7838 116,836
Minimum 300 2600 0.044 10 1600 0.8 0.044 37,950 762 0.044 0.071 1300 0.044 110 17,700
Maximum 8300 67,000 480 2900 20,300 138 440 56,700 45,200 45 7 5310 700 42,000 657,400
Number of samples 66 43 10 58 18 8 15 2 14 12 5 2 27 31 66

Table A2.

Sample composition (from Dy to Na) in mg of element per kg of PCBs.

References (mg/kg PCB) Dy Eu Fe Ga Ge Hf Hg In K La Li Mg Mn Mo Na
Chancerel et al., 2009
Chancerel et al., 2009
Chancerel et al., 2009
Kasper et al., 2011 14,200
Kasper et al., 2011 65,300
Kasper et al., 2011 48,500
Oguchi et al., 2011 150,000
Oguchi et al., 2011 18,000 140
Yamane et al., 2011 105,700
Silvas et al., 2015 124,900
Ueberschaar et al., 2017 (a) 140
Ueberschaar et al., 2017 (b) 0.088 0.09 13,640 0.02 0.5 0.5 0.088 0.088
Ueberschaar et al., 2017 (b) 68 1 166,360 207 39 40 3093 997
Arshadi et al., 2018 47,090 510 5900 5150 10
Holgersson et al., 2018 8608 0.6 205 602 16.2 7.7 139
Holgersson et al., 2018 11,481 0.3 234 1164 23.4 8.8 753
Holgersson et al., 2018 10,000
Holgersson et al., 2018 15,000
Holgersson et al., 2018 20,000
Holgersson et al., 2018 30,000
Holgersson et al., 2018 8434 8
Holgersson et al., 2018 26,300
Holgersson et al., 2018 35,000
Holgersson et al., 2018 23,500
Li et al., 2018 50,000
Gu et al., 2019
Gu et al., 2019 42,700
Gu et al., 2019 2400
Gu et al., 2019
Gu et al., 2019 46,000
Gu et al., 2019
Gu et al., 2019 10,500
Gu et al., 2019 2800
Gu et al., 2019 19,400
Gu et al., 2019 15,100
Gu et al., 2019 500
Gu et al., 2019 5000
Korf et al., 2019 15,089 210 12 5.6 236 13 635 654 897
Korf et al., 2019 5366 184 7 5.6 347 15 947 569 1197
Korf et al., 2019 105,700
Korf et al., 2019 14,200
Korf et al., 2019 65,300
Korf et al., 2019 48,500
Korf et al., 2019 150,000
Korf et al., 2019 18,000 140
Korf et al., 2019 1600 300 1900
Korf et al., 2019 157,200 180 12.4 17.9 141 4.6 35 701 2407 244 412
Korf et al., 2019 251,000 267 20 23 0.34 134 6.3 41 1680 4900 265 400
Korf et al., 2019 18,900 103 3.9 28.2 144 2.9 37 2000 480 75 391
Korf et al., 2019 8608 0.6 205 602 16.2 7.7 139
Korf et al., 2019 11,481 0.3 234 1164 23.4 8.8 753
Sahan et al., 2019 23,600
Sahan et al., 2019 20,400
Sahan et al., 2019 37,200
Sahan et al., 2019 33,900
Sahan et al., 2019 48,400
Sahan et al., 2019 10,000
Sahan et al., 2019 5000
Sahan et al., 2019 14,800
Sahan et al., 2019 6400
Sahan et al., 2019 11,900
Sahan et al., 2019 46,300
Sahan et al., 2019 10,100
Sahan et al., 2019 34,200
Sahan et al., 2019 48,500
Sahan et al., 2019 105,700
Sahan et al., 2019
Sahan et al., 2019 2800
Sahan et al., 2019
Sahan et al., 2019 14,600
Average 34 1 40,675 157 15 23 4 86 284 11 28 1568 1270 78 565
St deviation 48 1 50,004 72 15 5 5 74 104 16 13 1529 1882 111 358
Minimum 0.088 0.09 500 0.02 0.5 17.9 0.3 5.6 205 0.5 13 0.088 0.088 7.7 139
Maximum 68 1 251,000 267 39 28.2 12 144 510 40 41 5900 5150 265 1197
Number of samples 2 2 61 10 5 3 8 5 8 5 5 13 12 8 9

Table A3.

Sample composition (from Nd to Sr) in mg of element per kg of PCBs.

References (mg/kg PCB) Nd Ni P Pb Pd Pr Pt Rh S Sb Sc Si Sm Sn Sr
Chancerel et al., 2009 241
Chancerel et al., 2009 287
Chancerel et al., 2009 285 7
Kasper et al., 2011 34,200 11,700 20,900
Kasper et al., 2011 16,700 12,600 31,100
Kasper et al., 2011 25,400 12,300 25,500
Oguchi et al., 2011 19,000 34,000 300
Oguchi et al., 2011 13,000 300 35,000 430
Yamane et al., 2011 26,300 18,700 33,900
Silvas et al., 2015 34,100 18,700 33,900
Ueberschaar et al., 2017 (a)
Ueberschaar et al., 2017 (b) 0.088 8390 3707 103 0.088 1.75 1858 108,492 0.088 17,640
Ueberschaar et al., 2017 (b) 1162 37,628 132 56 85 1 10 112,800 8 26,948
Arshadi et al., 2018 400 2790 1000 11,190 1900 2660 94,250 23,540 400
Holgersson et al., 2018 9.7 11,600 910 3747 119 4.3 5.7 543 0.4 66,150 19,267 108
Holgersson et al., 2018 60.7 15,433 1441 260 55.4 0.8 8.5 30.4 0.6 56,971 32,200 82.5
Holgersson et al., 2018 12,000 200 1000
Holgersson et al., 2018 17,000 1100 200
Holgersson et al., 2018 9000 300 500
Holgersson et al., 2018 11,000 3 2500
Holgersson et al., 2018 1618 5 22
Holgersson et al., 2018 18,700
Holgersson et al., 2018 13,636 955
Holgersson et al., 2018 9900 294 30
Li et al., 2018 1000 3000 210 5000
Gu et al., 2019 400
Gu et al., 2019 25,400 12,200 25,800
Gu et al., 2019 100 14,000
Gu et al., 2019 4000
Gu et al., 2019 6000 600 100 26,000
Gu et al., 2019 300 200
Gu et al., 2019 8600 12,100 600
Gu et al., 2019 3900 13,600 100 16,000
Gu et al., 2019 27,100 17,800
Gu et al., 2019 19,800 10,700 100
Gu et al., 2019 100 6100 8600
Gu et al., 2019 8000 100 20,000
Korf et al., 2019 13,454 1405 5,6 44 334
Korf et al., 2019 6870 2495 5,6 8 372
Korf et al., 2019 26,300 18,700 33,900
Korf et al., 2019 34,200 11,700 20,900
Korf et al., 2019 16,700 12,600 31,100
Korf et al., 2019 25,400 12,300 25,500
Korf et al., 2019 19,000 34,000 300
Korf et al., 2019 13,000 300 35,000 430
Korf et al., 2019 100 2900 4000 8900 1900 104,800 14,200 500
Korf et al., 2019 44 41,500 283 99 7.3 12.2 11 60,000 38,100 284
Korf et al., 2019 32 57,000 610 178 25 9.8 12 80,200 31,400 233
Korf et al., 2019 9.5 82,900 597 100 5.3 3.16 17 45,300 41,700 372
Korf et al., 2019 9.7 11,600 910 3747 119 4.3 5.7 543 0.4 66,150 19,267 108
Korf et al., 2019 60.7 15,433 1441 260 55.4 0.8 8.5 30.4 0.6 56,971 32,200 82.5
Sahan et al., 2019 32,300 1600 10 32 62,700
Sahan et al., 2019 13,600 1000 DL 22 34,300
Sahan et al., 2019 23,800 7300 40 26 51,800
Sahan et al., 2019 21,000 2600 260 28 28,300
Sahan et al., 2019 37,700 16,700 220 50 26,200
Sahan et al., 2019 11,000 16,300 360 33 29,600
Sahan et al., 2019 15,800 17,900 400 19 35,500
Sahan et al., 2019 31,900 14,600 820 7 29,700
Sahan et al., 2019 59,300 23,300 120 12 25,300
Sahan et al., 2019 27,000 10,000 470 15 13,000
Sahan et al., 2019 17,000 27,300 DL 26 33,000
Sahan et al., 2019 15,000 15,600 390 36 27,100
Sahan et al., 2019 20,100 1900 140 26 13,700
Sahan et al., 2019 25,400 12,300 25,500
Sahan et al., 2019 26,300 18,700 33,900
Sahan et al., 2019 30,200 5800
Sahan et al., 2019 3900 13,600 50 16,000
Sahan et al., 2019 3960
Sahan et al., 2019 29,300 15,500 400 20 23,700
Average 172 21,068 1617 10,234 251 43 18 7 1900 587 6 77,462 4 26,677 289
St deviation 347 16,147 1193 6859 245 60 13 2 0 895 7 23,840 6 10,939 138
Minimum 0.088 100 910 132 3 0.088 0.8 5.7 1900 3.16 0.4 45,300 0.088 200 82.5
Maximum 1162 82,900 4000 27,300 1100 85 50 8.5 1900 2660 17 112,800 8 62,700 500
Number of samples 11 52 6 59 42 2 25 4 2 17 7 11 2 50 15

Table A4.

Sample composition (from Ta to Zr) in mg of element per kg of PCBs.

References (mg/kg PCB) Ta Tb Te Th Ti V W Y Zn Zr Measured % of total PCB mass
Chancerel et al., 2009 0.25%
Chancerel et al., 2009 0.42%
Chancerel et al., 2009 0.68%
Kasper et al., 2011 34,300 51.52%
Kasper et al., 2011 9700 53.02%
Kasper et al., 2011 18,200 51.55%
Oguchi et al., 2011 8600 38.25%
Oguchi et al., 2011 2600 5000 44.45%
Yamane et al., 2011 59,200 59.34%
Silvas et al., 2015 59,200 63.30%
Ueberschaar et al., 2017 (a) 0.01%
Ueberschaar et al., 2017 (b) 897 0.088 0.044 3061 4412 0.088 49.28%
Ueberschaar et al., 2017 (b) 1006 1 10 6648 16,154 630 93.14%
Arshadi et al., 2018 210 3060 9310 370 56.12%
Holgersson et al., 2018 1640 1 111 5 5642 225 49.37%
Holgersson et al., 2018 712 0.7 122 4.1 6743 298 55.50%
Holgersson et al., 2018 27.89%
Holgersson et al., 2018 24.07%
Holgersson et al., 2018 23.53%
Holgersson et al., 2018 17.36%
Holgersson et al., 2018 28.84%
Holgersson et al., 2018 39.20%
Holgersson et al., 2018 64.82%
Holgersson et al., 2018 27.23%
Li et al., 2018 20.09%
Gu et al., 2019 27.99%
Gu et al., 2019 20,700 51.39%
Gu et al., 2019 2200 58.67%
Gu et al., 2019 4600 40.78%
Gu et al., 2019 100 51.05%
Gu et al., 2019 41.96%
Gu et al., 2019 8000 40.02%
Gu et al., 2019 4100 44.97%
Gu et al., 2019 11,900 39.91%
Gu et al., 2019 2200 70.58%
Gu et al., 2019 100 9.59%
Gu et al., 2019 51.44%
Korf et al., 2019 1508 1011 43.83%
Korf et al., 2019 708 960 32.26%
Korf et al., 2019 59,200 59.34%
Korf et al., 2019 34,300 51.52%
Korf et al., 2019 9700 53.02%
Korf et al., 2019 18,200 51.55%
Korf et al., 2019 8600 38.25%
Korf et al., 2019 2600 5000 44.45%
Korf et al., 2019 1500 700 300 52.48%
Korf et al., 2019 2800 6450 140 1110 43 3770 692 74.29%
Korf et al., 2019 2000 7100 187 860 40 5600 910 83.76%
Korf et al., 2019 2330 7300 12.8 1740 230 69,000 1280 81.70%
Korf et al., 2019 1640 1 111 5 5642 225 49.37%
Korf et al., 2019 712 0.7 122 4.1 6743 298 55.50%
Sahan et al., 2019 28,100 48.72%
Sahan et al., 2019 8200 46.36%
Sahan et al., 2019 21,200 38.83%
Sahan et al., 2019 2300 48.17%
Sahan et al., 2019 17,800 57.07%
Sahan et al., 2019 3500 29.78%
Sahan et al., 2019 7200 38.82%
Sahan et al., 2019 30,200 44.82%
Sahan et al., 2019 67,000 65.39%
Sahan et al., 2019 5100 40.30%
Sahan et al., 2019 26,900 57.19%
Sahan et al., 2019 13,600 38.81%
Sahan et al., 2019 18,900 53.54%
Sahan et al., 2019 18,200 51.40%
Sahan et al., 2019 59,200 59.34%
Sahan et al., 2019 1000 6.32%
Sahan et al., 2019 4100 44.96%
Sahan et al., 2019 4570 40.77%
Sahan et al., 2019 17,000 44.86%
Average 2033 1 5 210 3234 49 597 47 16,164 475 64.35%
St deviation 782 1 7 - 2641 79 654 82 18,616 369
Minimum 897 0.088 0.044 210 708 0.7 111 4.1 100 0.088
Maximum 2800 1 10 210 7300 187 1740 230 69,000 1280
Number of samples 7 2 2 1 13 7 7 7 54 11

Figure A1.

Figure A1

Approach of the element mass (a) and its annual increase (b) in Mobile Phone Printed Circuit Boards worldwide.

Author Contributions

Conceptualization, J.T.; Investigation, J.T.; Methodology, A.V. (Antonio Valero) and A.V. (Alicia Valero); Writing—original draft, J.T.; Writing—review & editing, A.V. (Antonio Valero) and A.V. (Alicia Valero). All authors have read and agreed to the published version of the manuscript.

Funding

This research has been funded by the Spanish Ministry of Science and Innovation [grant number PID2020-116851RB-I00].

Conflicts of Interest

The authors declare no conflict of interest.

Footnotes

Publisher’s Note: MDPI stays neutral with regard to jurisdictional claims in published maps and institutional affiliations.

References


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