JOM, Vol. 74, No.

2, 2022
https://doi.org/10.1007/s11837-021-05038-6
 2022 The Author(s)

TECHNOLOGY METALS IN THE CIRCULAR ECONOMY OF CITIES

Waste Pharmaceutical Blister Packages as a Source

of Secondary Aluminum

SUGAM SHUKLA,1 PETTERI HALLI,1 MUHAMMAD KAMRAN KHALID,1

and MARI LUNDSTRÖM1,2

1.—Department of Chemical and Metallurgical Engineering (CMET), School of Chemical

Engineering, Aalto University, Vuorimiehentie 2 K, 02150 Espoo, Finland.
2.—e-mail: mari.lundstrom@aalto.fi

Waste pharmaceutical blister packages (WPBs) are a source of solid waste,

which are composed of plastics and aluminum, therefore acting as a potential
source for secondary aluminum. The structure of WPBs makes the recycling of
aluminum notably more complex than typical aluminum recycling. Currently,
WBPs are disposed of as municipal solid waste; thus, aluminum is lost from
the circulation during incineration. In this work, three types of WPBs were
studied, each with two plastic layers and a metallic layer. Delamination of
WPBs to separate aluminum and plastic(s) was investigated by using a solu-
tion of organic solvents. The effects of temperature (30–50C), acetone to
isopropanol ratio (0–100 vol.%) and different types of WPBs on delamination
behavior were investigated. The results suggest that aluminum separation
and recovery from WPBs is 100% at optimum conditions. Moreover, an overall
indicative flowsheet for recycling and post-processing of segregated aluminum
from the plastic is also suggested.

tablets are packed in blister packaging.1 These

INTRODUCTION
blisters not only provide an efficient physical pro-
The packaging industry is one of the largest tection for the drugs but also a barrier in terms of
industrial verticals in the world, with an overall moisture, light and/or oxygen. Currently, the han-
value of €250 billion.1 In the 1960s, packaging of dling of waste pharmaceutical blisters (WBPs) is
solid pharmaceuticals such as tablets and capsules done by either using landfill or treating them in
in blister packaging became popular. Compared incinerators.4 The main drawback of the incinera-
with other alternatives such as plastic and glass tion process is the loss of aluminum from circulation
bottles, blister packaging exhibits better sealing along with its oxidation.5 In addition, the genera-
properties.2 Other benefits of blister packages have tion of toxic gases can occur.
been suggested, such as product integrity, product Generally, pharmaceutical blister packages are
protection, being tamper proof, reduced possibility composed of various plastics and metallic foil, as
of accidental misuse and patient compliance.1 How- shown in Fig. 1. This type of structure, consisting of
ever, the increase in environmental concern, not aluminum (lidding material) and plastics (forming
only about the generation of medical and pharma- film), such as polyvinyl chloride PVC, polypropylene
ceutical waste, but also the waste generated from (PP), polystyrene (PS) and/or polyethylene (PE),
packaging material and its handling, has resulted makes the recycling of aluminum from WBPs
in strict EU rules and regulations.3 Globally, the notably more difficult and complex compared to
packaging of pharmaceuticals and drugs accounts typical aluminum recycling.6,7 Two types of WPBs
for approximately 4% of the whole packaging indus- are commonly utilized by the pharmaceutical pack-
try. In Europe, nearly 85% of drugs in the form of aging industry: Type I: aluminum and a single layer
of plastic; Type II: aluminum and a multilayer of
(Received July 29, 2021; accepted November 9, 2021;
plastic.
published online January 12, 2022)

612
Waste Pharmaceutical Blister Packages as a Source of Secondary Aluminum 613

Fig. 1. Schematic of medical blister packages.

The PVC present in WPBs is known to complicate fractions by applying electrodynamic fragmenta-
the incineration process. Incineration of PVC with tion. The recovery of aluminum was up to 88% with
mixed municipal waste may lead to the generation a purity of approximately 99.4%.5
of hazardous pollutants such as nitrous oxide, sulfur In contrast to the mechanical route for the
oxides, dusts and Cl-containing dioxins.8 In addi- separation of the aluminum and plastic fractions,
tion, the hydrogen chloride gas formed can react the chemical route has also been studied extensively
with moisture within the incinerator, resulting in in recent years. Wang et al.7,17 studied the leaching
the formation of hydrochloric acid. The hydrochloric of aluminum from WPBs with two different leaching
acid generated during the process can cause damage agents, viz., sodium hydroxide and hydrochloric
through corrosion of incinerator refractories, reduc- acid. The results of both the studies, under opti-
ing the lifetime of the incinerator. However, when mized conditions, showed high recovery rates of
mixed plastic waste including PP, PS, PE along with aluminum (up to 100%). However, there are certain
PVC is fed into the incinerator, the hydrochloric drawbacks with the selection of the leaching agents,
acid formed during the process reduces the recycling as both sodium hydroxide and hydrochloric acid are
ratio of other plastics because of chemical corrosive in nature and can cause harm to the
deterioration.8,9 environment.18 Moreover, further processing is
The PVC or chlorine present in waste promotes required to recover aluminum from the pregnant
the cyclization of organics and formation of aromatic leaching solution, therefore adding further cost to
compounds during incineration. PVC or chlorine the process. Yousef et al.18 investigated the delam-
promotes the cyclization of long-chain alkenes ination process by using N, N-dimethyl-cyclohexy-
through dechlorane reactions and generates aro- lamine (DMCHA) as a switchable hydrophilicity
matic organics, chloro-aromatic hydrocarbons or solvent along with ultrasonic treatment to enhance
char.10 Under oxygen-deficit conditions, metal chlo- the adhesive bonding between the aluminum and
rides promote the thermal decomposition of PS plastic in WPBs. The approach suggested by Yousef
plastic and subsequently react with benzene, which et al.18 consists of several steps, hence complicating
ultimately favors the formation and growth of the overall process. This leads to an increase in
chlorinated polycyclic aromatic hydrocarbons (Cl- energy consumption and an increase in the cost of
PAHs).11 These PAH compounds are known to be the recycling and recovery process of aluminum and
carcinogenic, mutagenic and teratogenic and may plastic. Moreover, the utilization of DMCHA in this
cause cardiovascular disease.12 approach is not preferred as a sustainable and green
Instead of incineration of plastics such as PP, PS, process because of its high corrosiveness and toxi-
PE and PVC, which is already partially restricted in city. Therefore, it is considered a safety and envi-
many European countries, mechanical and chemical ronmental hazard.18 Finally, Nieminen et al.2
recycling can provide an advantage due to the presented a study in which they investigated deep
generation of few pollutants and wide variety of eutectic solvents (DES) consisting of lactic acid and
recycled products.13,14 Gente et al.15,16 conducted a choline chloride (molar ratio 1:9) and pure lactic
mechanical separation study by employing cryo- acid for separating aluminum and plastic. However,
comminution on WPBs and further separation of after pure DES treatment, the recovered aluminum
aluminum (conducting fraction) and plastic (non- was highly oxidized consisting of 65 wt.% aluminum
conducting fraction) through electrostatic separa- and 23 wt.% oxygen because of the formation of
tion. The results of their study showed a high aluminum lactate, whereas after lactic acid treat-
aluminum (conductor fraction) recovery rate (ap- ment, the aluminum foil surface contained 95 wt.%
proximately 80%) and a high plastic (non-conductor aluminum. Also, the solvent purification methods
fraction) recovery rate (approximately 90%) in opti- and recovery of the dissolved aluminum require
mal conditions. However, according to the method further research.2
they suggested in another study, the presence of Several organic solvents in various research
plastics in the conducting fraction and aluminum in studies have been investigated for the delamination
the non-conducting fraction implies that each frac- process and for interaction between the organic
tion is still impure and hence requires further solvents and plastics. According to Summers and
treatment.15,16 Agarwal et al.5 studied the mechan- Rabinovitch, acetone swells the PVC very rapidly
ical separation of WPBs into aluminum and plastic but only up to a certain extent and attains an
equilibrium after a certain residence time due to the
614 Shukla, Halli, Khalid, and Lundström

penetration of acetone into the amorphous PVC A, B and C. This was ensured by ascertaining that
only, without destroying the crystalline PVC, which all the Sample As were from the same manufac-
acts as the crosslink.19 Similarly, in another study turer; all the Sample Bs were from the same
performed by Papaspyrides and Tingas,20 they manufacturer(s) (different from Sample A) and of
suggested that isopropanol penetrates PVC with the same drug. Sample C followed the same pattern.
ease and hence has higher rates of sorption than The differences among the three sample sets, A, B
isooctane, therefore facilitating delamination of and C, were first that they all were from different
WPBs. Additionally, the aluminum present in manufacturer.s Second, they all were for different
WPBs reacts with neither acetone nor isopropanol drugs and different drug delivery methods, viz.,
under atmospheric conditions.21 Sample A was in the form of capsules; Sample B and
The purpose of this study is to investigate and Sample C were tablets. Lastly, the main difference
develop a hydrometallurgical process to resolve the in all three samples was the thickness of the plastic
challenges in recycling of aluminum from waste layers and aluminum layer.
pharmaceutical blister packs, thereby reducing med-
ical waste. Moreover, the proposed process can be Characterization of WPBs
considered environmentally benign as green solvents
Fourier transformation infrared spectroscopy
(acetone and iso-propanol) are used. In addition, the
(FTIR, Nicolet Magna 380, Smart Orbit, USA) was
process can provide not only an efficient and sustain-
used to analyze the plastic material present in WPB
able method for the recovery of aluminum but also
sample types A and B. A total of 32 scans were
potentially for plastics from waste without the gen-
completed and integrated for each spectrum at a
eration of hazardous pollutants.
resolution of 4 cm 1 in the wavenumber range from
400 cm 1 to 4000 cm 1. The cross-section measure-
EXPERIMENTAL SECTION
ment and surface morphology of WPBs were ana-
Sample Collection and Types of WPBs lyzed using scanning electron microscope (SEM,
Tescan Mira3 GM, Czech Republic) coupled with
Samples of different types of WPBs were collected
energy-dispersive spectroscopy (EDS, UltraDry 50
from a machine dose dispenser of Pharmac Finland
mm2 EDS detector and NSS software, Thermo
Oy pharmaceutical company, as shown in Fig. 2.
Scientific, USA).
The collected WPB samples were sorted manually
The WPB sample preparation for SEM analysis
into two types based on the color profile, i.e., two
was performed by cutting small pieces of WPB
samples, A and B: silver-colored WPBs with translu-
Samples A, B and C using a sharp cutter. These
cent plastic film (Sample A and) and white-colored
small pieces of WPBs were then cast in epoxy. Once
WPBs with opaque plastic film (Sample B). Sample
the epoxy containing the samples had hardened,
C was used for the verification of parameter opti-
polishing was performed (with 1 lm multi-crystal
mization experiments. The selection was based on
diamonds, Struers, Denmark), and the polished
visual appearance; Sample C was a silver-colored
samples together with the epoxy holder were carbon
WPB. Additionally, Sample C had similar structure,
coated (EM SCD050, Leica, Japan) to provide a
i.e., two plastic layers and one aluminum layer, with
conductive layer on top of the samples. EDS was
poly-acrylic based adhesive.
also performed on the same epoxy-embedded car-
Sample selection was based on the homogeneity
bon-coated samples to analyze the metallic and
and similarity among all the samples, i.e., Sample

Fig. 2. Types of waste pharmaceutical blisters: Samples A, B and C, used as raw materials in the experiments.
Waste Pharmaceutical Blister Packages as a Source of Secondary Aluminum 615

plastic composition of the lidding material and A12–A15 were carried out to ascertain the effect of
forming film in WPBs. temperature and the acetone concentration (v/v%),
whereas experiments A16–A20 were performed to
Delamination Experiments study the effect of residence time on the delamina-
tion of WPBs.
The experiments were performed in batches using
After performing the delamination experiments
250-ml beakers made of borosilicate glass. Prior to
for Samples A and B, the experiments shown in
every experiment, all the WPB samples were
Table I for the Sample C were performed to
weighed. The delaminating agents used were ace-
investigate and verify the optimized parameter
tone (C3H6O, > 99% Technical Grade, VWR Chem-
levels.
icals) and iso-propanol (C3H8O, 99.5%, anhydrous,
After each experimental run time, the separated
Sigma-Aldrich). The delamination medium was
aluminum and plastic layers were carefully col-
prepared by measuring the required amount of
lected from the delamination medium. The collected
acetone (v/v%), which was diluted by iso-propanol
aluminum layers were dried overnight at room
(v/v%). A total volume of 200 mL of the delamination
temperature and then weighed. The aluminum
medium was used. The beakers were sealed with
recovery was then calculated based on the wt.% of
parafilm. The beakers were heated to the target
the aluminum layer in each sample of WPBs
temperature by using a magnetic hot plate stirrer
varying between 10 wt.% and 15 wt.%. The wt.%
(Magnetic Stirrer, IKA RT10, Germany), and the
of aluminum layer in Sample A was 15 wt.%, in
agitation speed was set at 600 rpm. Agitation was
Sample B was 10 wt.% and in Sample C was 13
conducted to ensure that all the solids were sus-
wt.%. The aluminum layers were then analyzed
pended in the solvent. WPB samples of known
using a scanning electron microscope (SEM, Tescan
weight were then added into the delamination
Mira3 GM, Czech Republic) coupled with energy-
medium once the target temperature had been
dispersive spectroscopy (EDS, UltraDry 50 mm2
reached. Since the boiling point of acetone is 56C,
EDS detector and NSS software, Thermo Scientific,
the temperature range used for the experiments
USA) wherever needed.
was set to 30–50C.
The experiments shown in Table I were per-
RESULTS AND DISCUSSION
formed for Samples A and B. Experiments A1, A6
and A11 were conducted to ascertain whether iso- Characterization of WPB Samples
propanol can delaminate WPBs on its own and
The characterization of WPBs was performed
whether a higher temperature is required for
using chemical analysis by employing inductively
delamination. Experiments A2–A5, A7–A10 and
coupled plasma-optical emission spectroscopy (ICP-

Table I. Experiments and their parameter levels utilized in this study for WPB Sample A, B and C

Experiment codes* Temperature (C) Time (min) Acetone (v/v%) Iso-propanol (v/v%)

A1, B1 30 120 0 100

A2, B2 30 120 25 75
A3, B3 30 120 50 50
A4, B4 30 120 75 25
A5, B5 30 120 100 0
A6, B6, C1 40 120 0 100
A7, B7, C2 40 120 25 75
A8, B8, C3 40 120 50 50
A9, B9, C4 40 120 75 25
A10, B10, C5 40 120 100 0
A11, B11 50 120 0 100
A12, B12 50 120 25 75
A13, B13 50 120 50 50
A14, B14 50 120 75 25
A15, B15 50 120 100 0
A16, B16 40 30 50 50
A17, B17 40 60 50 50
A18, B18 40 90 50 50
A19, B19 40 120 50 50
A20, B20 40 120 50 50
*Experiment codes for Sample B are B1–B20 and for Sample C are C1–C5.
616 Shukla, Halli, Khalid, and Lundström

OES, PerkinElmer Optima 7100 DV, USA). The Furthermore, the SEM micrographs showed the
purity of the aluminum in samples A and B was > cross sections of Samples A and B in Fig. 4a and b
99.4%. The results indicated that the aluminum respectively. It was observed that in both samples
layer constitutes 15 wt.% and 10 wt.% of the total there were two layers of plastics present in the
weight of Samples A and B, respectively. However, forming film and a metallic layer of aluminum as
for Sample C, the aluminum layer constitutes the lidding material. As also shown in Fig. 4, the
13 wt.% of the total weight of the WPBs. The overall thickness of WPBs ranged from 280–365 lm
investigated WPB Samples A and B were charac- and comprised two plastic layers (D1 and D2) in the
terized by FTIR (Fig. 3). The prominent distinctive range of 260–330 lm and an aluminum layer (D3) in
bands found in the spectra were at a wavelength of the range of 20–35 lm. Therefore, based on the
2906 cm 1, which represents C-H stretching of the FTIR results, the chemical composition of the
CH-Cl group, and at 1425 cm 1 because of CH2 forming films of blister packaging indicates the
deformation; at 1234 cm 1, which demonstrates C-H presence of PVC and PVDC. Additionally, according
deformation corresponding to a CH-Cl group; at 960 to further analysis of the FTIR results (Fig. 3)
cm 1, which displays the rocking of the CH2 group; performed on Sample A (Plastic Layer 1) and
and at 605 cm 1 because of CH-Cl stretching.22–24 Sample A (Plastic Layer 2), the best fitted results
The FTIR analysis for the material used for the were with polyvinyl chloride/polyvinyl acetate
adhesion of aluminum and plastic layers closely copolymer with 10% polyvinyl acetate and
matched the spectrum of poly-acrylic cyanoacrylate, polyvinylidene chloride/polymethyl methacrylate
as reported by Han et al.25 Hence, it can be copolymer with 10% of polymethyl methacrylate,
concluded that the material used for the adhesion respectively. However, for Sample B (Plastic Layer
of aluminum and plastic layers was a poly-acrylic 1) and Sample B (Plastic Layer 1), the best fitted
based glue. results were with polyvinyl chloride/polyvinyl

Fig. 3. FTIR spectra for (a) sample A and (b) sample B.

Waste Pharmaceutical Blister Packages as a Source of Secondary Aluminum 617

Fig. 4. SEM micrographs of cross-sectional measurement and EDS analysis of plastic layers and metallic layer for (a) Sample A and (b) Sample
B.

Table II. Elemental composition (wt.%) for both Sample A and B (average composition)

Element O Na Al Si P S Cl Zn Ca Ti Pd Sn Fe Total

Sample A
Spot 1 11.6 0.1 0.3 0.2 – 0.4 81.5 – 0.03 – 4.6 1.4 – 100
Spot 2 16.1 1.3 0.3 0.1 0.4 0.8 76.6 0.2 – – 4.3 – – 100
Spot 3 1.6 – 95.8 1.1 – 0.04 1.1 – 0.02 – – – 0.4 100
Sample B
Spot 1 15.8 – 0.5 0.2 – 0.4 73.0 – 0.1 4.6 4.6 0.9 – 100
Spot 2 12.5 1.6 0.3 0.1 0.4 0.8 80.1 – – – 4.3 – – 100
Spot 3 1.8 – 97.3 – 0.1 – 0.1 – – – – – 0.8 100

acetate copolymer with 2% polyvinyl acetate and Effect of Acetone Concentration, Temperature
polyvinyl chloride, respectively. The FTIR spectra and Time on Delamination
before and after the delamination of Samples A, B
Experiments A1–A5 at 30C, A6–A10 at 40C and
and C closely matched the PVC and PVDC spectra
A11–A15 at 50C were performed on Sample A. The
(see supplementary Figs. S1, S2 and S3).
run time for all the experiments was 120 min. No
The elemental composition of the plastic and
delamination was observed for acetone concentra-
metallic layers as shown in Table II is the average
tions < 50 v/v%, i.e., A1, A2, A6, A7, A11 and A12.
composition of three points for each layer, i.e., Spot
Also, no delamination was observed at 50 v/v%
1 for Sample A is an average of EDS performed for
acetone concentration, i.e., A3. However, for all the
three different points on Plastic Layer 1 of Sample
other experimental operating conditions, i.e., A4,
A. The elemental composition (wt.%) also confirms
A5, A8–A10 and A13–A15, total delamination was
that after delamination the metallic layer of all the
achieved, as shown in Fig. 5a.
samples mainly comprises aluminum (see supple-
The experiments on Sample B were performed in
mentary Tables S1, S2 and S3). Moreover, the
similar operating conditions, i.e., B1–B5, B6–B10
presence of a significant amount of chlorine in the
and B11–B15. For Sample B, delamination was
plastic layers clearly suggests that the plastic layers
observed at acetone concentrations of 50 v/v% and
are composed of PVC and PVDC.
higher, i.e., B3–B5, B8–B10 and B13–B15. How-
ever, for Sample B, delamination was also observed
at an acetone concentration of 25 v/v% at 50C, i.e.,
618 Shukla, Halli, Khalid, and Lundström

Fig. 5. Aluminum recovery at different acetone concentrations for (a) Sample A and (b) Sample B.

B12, as shown in Fig. 5b. The total delamination of if the residence time was< 120 min. After 120 min,
WPBs with 100% aluminum recovery was attained the total delamination of both plastic layers along
at the acetone concentration of 50 v/v% at 40C for with aluminum was achieved. The results from the
both Samples A and B. residence time experiments suggest that the time
The investigated process temperatures were 30, required to penetrate through different plastic
40 and 50C for both Samples A and B, as shown in layers varies because of the plastic layer structure,
Fig. 5. The operating temperature had a significant chemical composition and thickness of plastic lay-
effect on both the delamination process as well as on ers. Therefore, delamination behavior is different
the recovery of aluminum from the delaminated for Samples A and B. However, the time required for
samples. A 100% recovery of aluminum was total delamination for both Sample A and B was 120
achieved for an acetone concentration of 50 v/v% min.
and at a temperature of 40C for both Samples A Experiments A20 and B20 (Table I) were per-
and B, i.e., A8 and B8. However, with an increase in formed to ascertain whether these investigated
acetone concentration at 40C, the aluminum recov- experimental conditions were the optimal operating
ery decreased. The higher temperature, i.e., > 40C, parameters for the delamination of Samples A and
facilitates the decomposition of plastic layers and B. Based on the results, it is suggested that the
adhesive. Moreover, when higher concentration of mechanism for the delamination process involves
acetone, i.e., > 50 v/v%, is used, the plastic layers the depolymerization of the acrylic adhesive present
and adhesive start to decompose and remain as between the aluminum and plastic layers of WPBs
residual within the solvent, whilst during the in the presence of a delaminating agent and that the
overnight drying of samples in atmospheric condi- depolymerized monomer remains in the medium.
tions, the residuals from the decomposed plastic and The acetone swells the plastics layers but reaches a
adhesive tend to reattach at aluminum surface limit because of the crosslinked structure of the
resulting the decrease in aluminum recovery. plastic layers.
The effect of residence time, i.e., 30 min, 60 min, According to the studies reported by Summers
90 min and 120 min, on the delamination of WPBs and Rabinovitch19 and Perry et al.,26 this is due to
and aluminum recovery was studied at 40C and the diffusion of acetone through the amorphous
with an acetone concentration of 50 v/v%. The plastic but not the crystallites/crystalline PVC,
experiment codes for Sample A were A16–A19 and thereby constructing porous channels for the ace-
for Sample B were B16–B19 (Table I). No delami- tone to diffuse toward the interface between the
nation observed at 30 min for Sample A. However, plastic layers and aluminum glued together with
for Sample B, the first plastic layer was completely acrylic adhesive. As the acetone is diffused toward
delaminated within 30 min, whereas for Sample A, the interface, it allows the depolymerization of the
the first plastic layer was delaminated after 60 min. acrylic adhesive, leading to delamination.19,26 Han
It was also observed that the second plastic layer et al.25 mentioned a similar phenomenon and
was partially delaminated for both Samples A and B reported that various poly-alkyl-cyanoacrylate
Waste Pharmaceutical Blister Packages as a Source of Secondary Aluminum 619

(PACA) polymers used as adhesives in the pharma- observed for experiments with an acetone concen-
ceutical industry undergo rapid depolymerization in tration < 50 v/v%, i.e., C1 and C2. However, for an
the presence of acetone. Bruze et al.27 also reported acetone concentration ‡ 50 v/v%, total delamination
similar findings while performing patch testing for of sample C was achieved, i.e., C3–C5, with 100%
occupational allergic contact dermatitis for ethyl- aluminum recovery at C3 and C4, as shown in
cyanoacrylate, which is used as an adhesive. They Fig. 6. Hence, the parameters for experiment C3
reported that results were false-negative for a test were suggested as the optimized parameters
when a different acetone concentration was added because of the lower acetone concentration com-
into the chambers for the Finn Chambers patch pared to C4 and C5, allowing better recovery of
test technique since, in Finn Chambers, the aluminum from all of sample C.
chambers are constructed from aluminum and filled The recovery and reuse of delaminating agent
with the allergen, i.e., ethyl-cyanoacrylate adhesive were carried out to establish and reduce the amount
dissolved in acetone, for testing the allergic reac- of solvent waste generated. Additionally, to support
tion. After 2 days, the results for allergic reactions the principles of circular economy and green chem-
were false negative because of the denaturing of the istry along with the potential commercial applica-
ethyl-cyanoacrylate. Hence, when comparing the tion, the reuse of the delaminating agent was
study from Bruze et al.,27 it is suggested that a studied by reusing it six times. The reuse of the
similar mechanism occurs during the delamination delaminating agent was carried out in optimized
of WPBs. Therefore, the results elucidate the reason conditions for sample C, i.e., at 40C, for 120 min at
for required retention time, temperature and ace- 600 rpm agitation. The initial volume of delaminat-
tone concentration for the total delamination of ing agent was 200 mL with an acetone concentra-
different WPBs. Moreover, the results also show tion of 50 v/v%. After each cycle, the remaining
that the structure and chemical composition volume of the delaminating agent was measured
(amount of amorphous and crystalline PVC) of and visually inspected. The loss in volume after
plastic layers are different in Sample A and Sample each cycle was 7 ± 2 mL. The loss in volume after
B, which is similar to the claims made by Summers each cycle was observed because of the volatile
and Rabinovitch19 that acetone swells the PVC nature of the delaminating agent and because the
because of the penetration of acetone into the experimental setup was not hermetically sealed.
amorphous PVC without altering the crystalline Although the time required for total delamination
PVC. remained unchanged, the visual inspection per-
formed after each cycle revealed an accumulation
Verification of Parameter Optimization, of residuals.
Reuse of Solvent and Laboratory Scale-Up Furthermore, to ascertain the laboratory scale up
of the delamination process, four pieceseach from
To ascertain that the parameters were optimized
Sample A, B and C were used for the experiments
for any type of WPBs, delamination was performed
under optimized parameters, i.e., at 40C for 120
for sample C at 40C for 120 min with 600 rpm
min, at 600 rpm agitation and an acetone concen-
agitation. No delamination for sample C was
tration of 50 v/v%. However, the total volume of the
delaminating agent used was 800 mL with overhead
stirring to ensure that the WPBs were well sus-
pended in the delaminating agent. The laboratory
scale-up experiment resulted in total delamination
of all 12 WPBs (four pieces each from Sample A, B
and C), with 100% aluminum recovery at the end of
laboratory scale-up experiment.

Discussion
The delamination experiments showed that alu-
minum separation from the plastic fraction was
achieved at optimized operating parameters for
different types of WPBs. However, for feasibility of
the process, effective solid liquid separation of
aluminum and plastics (solid) from the delaminat-
ing agent (liquid) is needed, e.g., by using a
horizontal belt vacuum filtration unit. The sepa-
rated delaminating agent can be reused, while the
aluminum and plastics can be fed for drying (op-
tional) prior to further processing. The segregation
of aluminum and plastic can be achieved through an
Fig. 6. Parameter optimization experiments and aluminum recovery eddy current separator. In the current study, the
for Sample C.
620 Shukla, Halli, Khalid, and Lundström

Fig. 7. Overall indicative flowsheet for delamination of WPBs for recycling.

application of eddy current separation was ensured obtained for all the investigated samples, A, B and
by using a laboratory-scale eddy current separator C, in the optimized parameters, i.e., at 40C with an
for the segregation of aluminum and plastics from acetone concentration of 50 v/v% (200 mL) and
delaminated WPBs. The eddy current separator retention time of 120 min.
provided complete segregation of aluminum and
plastics. The separated aluminum can be recycled ACKNOWLEDGEMENTS
via a secondary aluminum smelter, whereas plastics The authors acknowledge the SUDDEN Project
could potentially be subjected to further processing. (Decision No. 320219) funded by the Strategic Re-
An overall indicative flowsheet for the entire pro- search Council at the Academy of Finland and
cess is shown in Fig. 7. Pharmac Finland Oy is gratefully acknowledged for
The advantages of the proposed process are high providing the support and WPBs investigated in
aluminum separation ( 100%) using green solvent, this study. This work also made use of Raw-
at low temperature and with heterogenous feed MatTERS Finland Infrastructure (RAMI) funded by
material, i.e., different WPBs. The process requires the Academy of Finland.
no pre-processing of the raw material. However,
acetone and iso-propanol are highly volatile and FUNDING
flammable and can cause mild irritation if exposed Open Access funding provided by Aalto Univer-
to them for a longer period. Once these issues are sity.
resolved, the then proposed methodology may
provide increased efficiency for aluminum recycling
from WPBs and can be both environmentally and CONFLICT OF INTEREST
economically attractive in an industrially scaled-up On behalf of all authors, the corresponding author
operation. states that there is no conflict of interest.

CONCLUSION OPEN ACCESS

The current study presents, for the first time to This article is licensed under a Creative Commons
our knowledge, a novel application of the delami- Attribution 4.0 International License, which per-
nation technique for separating the aluminum layer mits use, sharing, adaptation, distribution and
from the plastic layer in WPBs. This allows recy- reproduction in any medium or format, as long as
cling of aluminum and potential plastics obtained you give appropriate credit to the original author(s)
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using acetone and iso-propanol (50 v/v%) as the made. The images or other third party material in
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optimized for a heterogeneous feed of WPBs. The Commons licence, unless indicated otherwise in a
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Waste Pharmaceutical Blister Packages as a Source of Secondary Aluminum 621

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