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Article history: Anthropogenic litter (AL) distribution was assessed on beaches presenting different levels of urban
Received 7 April 2021 occupation at Santos Estuarine System. Plastics and cigarette butts were the items most found at
Received in revised form 1 June 2021 sampling sites. Plastic items sub-categories, such as cotton buds, lids, microcentrifuge tubes, pellets,
Accepted 19 June 2021
and polystyrene foam, presented sources related to industrial, tourism and port activities, and sewage
Available online 21 June 2021
discharges. The contamination gradient already reported for hazardous chemical levels was also
Keywords: observed for AL. Litter categories related to local and allochthonous sources presented a gradient of
Plastic spatial distribution. Although touristic activities are an impactful and variable factor, the number of
Cigarette butts inhabitants was positively correlated with most AL categories. The semi-urban beach (S1) was classified
Contamination gradient as extremely dirty, and it was mostly covered by hazardous AL. The semi-remote (S2) and remote (S3)
Hazardous items beaches were classified as moderate and clean with some or few hazardous AL, respectively. Therefore,
Tourism urban and hydrodynamic gradients drive marine litter distribution on studied zone.
© 2021 Elsevier B.V. All rights reserved.
https://doi.org/10.1016/j.rsma.2021.101902
2352-4855/© 2021 Elsevier B.V. All rights reserved.
V.V. Ribeiro, C.A.Y. Harayashiki, A. Ertaş et al. Regional Studies in Marine Science 46 (2021) 101902
toxic metals, polycyclic aromatic hydrocarbons (PAHs), polychlo- Oceanographic Commission (Cheshire et al., 2009). These cate-
rinated biphenyls (PCBs), organochlorine pesticides and steroidal gories were plastic, polystyrene foam (XPS), metal, glass, paper,
estrogens have been reported in environmental samples from and processed wood. Although Cheshire et al. (2019) and Gal-
SES (Abreu et al., 2020; Begliomini et al., 2017; Buruaem et al., gani et al. (2013) recommend including cigarette butts (CBs) as
2013; Gouveia et al., 2019; Kim et al., 2017; Oliveira et al., 2020; paper/cardboard or plastic items, they were considered in a sep-
Pusceddu et al., 2019). Overall, these studies have found higher arated category due to their high occurrence, mixed composition,
contaminant concentrations inside the estuary, which flows to- and elevated environmental impact (Araújo and Costa, 2019). In
wards Santos Bay influenced by mixed tides, cold fronts, and in- addition, litter that presented high incidence (>3% of all AL) were
tense rainfall regime and are diluted towards the ocean, forming separately categorized, as pellets, cotton swabs and plastic lids. In
a contamination gradient. this sense, those items with mixed composition or low occurrence
The beaches from SES located at Guarujá City present dif- (<0.5% of all AL), such as food packaging, were categorized as
ferent levels of urban occupation, providing an opportunity to others. After separating all AL by category, the items were in-
investigate possible relationships between AL occurrence and dividually counted. The AL density was expressed by items/m2
population densities in an urban gradient. Moreover, inputs from (mean ± standard deviation). The Clean-Coast Index (CCI) was
estuarine discharges can be elucidated by AL categorization con- calculated per site, using the following equation: CCI = (Σ litter
sidering, for instance, buoyancy properties and use categories on transect/total area of transect) × K, where K is a constant equal
(Munari et al., 2016). Despite this, no studies so far have as- to 20 (Alkalay et al., 2007). Then, the results were categorized
sessed potential sources and the existence of AL gradients in by cleanliness according to the scale described by Alkalay et al.
this estuary. Therefore, based on spatial distribution of chemical (2007) (Table S1, supplementary material). Despite originally de-
contamination already demonstrated in SES, we hypothesized a sign only for plastic items, the CCI is currently used to assess
similar behavior for AL. Thus, the present study aimed to simulta- AL contamination (Ribeiro et al., 2021). In addition, Hazardous
neously investigate the occurrence of anthropogenic waste along Anthropogenic Litter Index (HALI) was calculated by the relation
the contamination gradient as well as to identify potential sources between Hazardous Anthropogenic Litter (HALs) occurrence and
of AL. all collected items by a logarithmic (log10) scale (Rangel-Buitrago
et al., 2019). Herein, the following items were considered HALs:
2. Materials and methods CB, condoms, cotton swabs, glass, metal, MT, processed wood
with nails, and sharp ceramic. The HALI values were classified
2.1. Study area and sampling according to five categories (Table S2, supplementary material).
The SES houses a high population density at Santos (1494.2 2.2. Data analyses
inhabitants/km2 ) and Guarujá (2026.8 inhabitants/km2 ) cities
(Ibge, 2020). The present study was undertaken in three beaches The normality and homogeneity of data (AL categories and
with different uses (based on beach activities) located at Guarujá number of residents) were verified using Shapiro–Wilk and Lev-
city (Fig. 1). S1 (Santa Cruz dos Navegantes Beach - 23◦ 59′ 45.3′′ S ene tests, respectively. Differences in AL amounts, among beaches,
46◦ 18′ 22.2′′ W) is a semi-urban beach with 750 m of extension were analyzed by one-way ANOVA followed by Tukey multiple
and approximately 5000 inhabitants, receiving daily public clean- comparisons. Alternatively, non-parametric statistics (Kruskal–
ness (Ribeiro and Santos, 2020) and tourists mostly during vaca- Wallis test followed by the Dunn’s analysis) were applied when
tions, festivities and weekends (Ferreira and Lopes, 2013). This ANOVA assumptions were not achieved. Spearman non-
beach is geographically sheltered from winds and waves, with parametric correlation analysis was used to investigate the re-
limited access by roads and boats, but it does not have an efficient lationships between AL categories and number of residents in
basic sanitation system and tourist infrastructure (Ferreira and each sampled site. All statistical analyses were performed using
Lopes, 2013). S2 (Góes Beach - 23◦ 59′ 55.3′′ S 46◦ 18′ 51.8′′ W) is a Statistica⃝R
(version 13.0 Statsoft) with a significant level of 0.05.
250 m long semi-remote beach with low hydrodynamics and ap-
proximately 300 inhabitants composed mostly by fisherman and 3. Results and discussion
woman economically dependent on tourism activities (Quevedo
et al., 2011). The access to S2 is only possible by boats and poorly The three sampling sites together (3600 m2 ) accounted for
preserved trails (Souza, 2015). S2 is east–west orientated, north- a total of 4416 items (1.227 ± 1.49 items/m2 ). Overall, the AL
facing and completely sheltered from the direct incidence of open found was mostly comprised of plastics (65.5%), followed by CB
sea wave trains, but influenced only by diffraction, refraction, (23.7%), pellets (16.4%) and XPS (10.9%) (Table 1). According to
and reflection waves from Santos Bay (Souza, 2015). S3 (Sangava CCI results, the sites S1, S2 and S3 were classified as extremely
Beach - 24◦ 00′ 04.9′′ S 46◦ 19′ 12.4′′ W) is a remote and inhabited dirty (58.8 ± 24.2), moderate (9.9 ± 1.8) and clean (4.9 ± 0.9),
beach, where diving and other tourism activities are held (Silva, respectively (Table 1). The HALI values calculated for S1 (HALI
2011). The access to S3 is limited by boats and a long and = 5.9), S2 (HALI = 1.14) and S3 (HALI = 0.62) categorized the
poorly preserved trail, which may be the most likely reason to studied sites as type V, III and II, respectively (Table 1).
the restricted number of beachgoers in comparison to S1 and S2 The semi-urban site (S1) represented 80% of all collected AL,
(Silva, 2011). followed by semi-remote S2 (13%) and remote S3 (7%). In general,
AL sampling was performed accordingly to the European Com- S1 presented a higher AL quantity than both S2 (p < 0.05) and
mission/OSPAR adapted methodology (Galgani et al., 2013). More S3 (p < 0.05) (Fig. 2a). Similarly, higher amounts of CB, cotton
specifically, plastic pellets (1–5 mm of diameter or length) and all swaps, metals, MT, pellets, plastic and XPS were found at S1 in
AL > 3 cm were collected between December 2020 and January comparison to S2 (p < 0.05) and S3 (p < 0.05) (Fig. 2b, c, d, e, f,
2021 during a single sampling campaign held in each area. At h and j). No differences among sites (p > 0.05) were observed
each site, three transects of 400 m2 (20 x 20 m) were equidis- for ceramics, cloth/textile, glass, plastic lids, paper/cardboard,
tantly distributed along the beach and sampled (Kaviarasan et al., processed wood, and others (Fig. 2g, i, k, l, m, n and o).
2020), considering each transect as a replicate. All collected items The correlation results (Table S3, supplementary material)
were separated into categories adopted by the United Nations En- showed that CB (r = 0.95), cotton swabs (r = 0.93), glass (r =
vironment Program in collaboration with the Intergovernmental 0.85), plastic lids (r = 0.90), metal (r = 0.79), paper/cardboard (r
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V.V. Ribeiro, C.A.Y. Harayashiki, A. Ertaş et al. Regional Studies in Marine Science 46 (2021) 101902
Fig. 1. Sampling sites in the Guarujá beaches - Brazil). S1 = Santa Cruz dos Navegantes Beach, S2 = Góes Beach, S3 = Sangava Beach.
Fig. 2. Quantity (mean ± sd) of (a) total anthropogenic litter (AL) and (b–o) different AL categories sampled in beaches located in Guarujá beaches (Brazil) during
the summer of 2020 and 2021. Letters indicate significant difference among sites (p < 0.05).
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V.V. Ribeiro, C.A.Y. Harayashiki, A. Ertaş et al. Regional Studies in Marine Science 46 (2021) 101902
Table 1
Anthropogenic litter (AL) density (items/m2 - mean ± SD) and percentage, and Hazardous Anthropogenic Litter Index (HALI) in
beaches located in the left margin of Santos Estuarine System (Guarujá City - Brazil). The italic and underlined lines indicate
sub-categories and their main categories, respectively.
Sampling site Navegantes (S1) Góes (S2) Sangava (S3) Total
Area (m2 ) 1200 1200 1200 3600
Items Items/m2 % Items/m2 % Items/m2 % %
Mixed polymers 0.916 ± 0.63 31.1 0.088 ± 0.01 17.9 0.050 ± 0.02 21.6 28.6
Polystyrene foam (XPS) 0.252 ± 0.09 8.5 0.073 ± 0.03 14.7 0.078 ± 0.02 34.2 10.9
Lids 0.095 ± 0.09 3.2 0.023 ± 0.01 4.6 0.008 ± 0.00 3.4 3.4
Pellets 0.542 ± 0.05 18.4 0.057 ± 0.02 11.5 0.006 ± 0.01 2.4 16.4
Condoma 0.001 ± 0.00 0.1 0.001 ± 0.00 0.2 0.000 ± 0.00 0.0 0.1
Cotton swabsa 0.113 ± 0.02 3.8 0.015 ± 0.01 3.0 0.003 ± 0.00 1.0 3.5
Microcentrifuge tubes (MT)a 0.075 ± 0.04 2.5 0.008 ± 0.00 0.1 0.009 ± 0.00 3.8 2.3
Plastic Total 1.993 ± 0.86 67.7 0.263 ± 0.04 53.5 0.154 ± 0.03 66.4 65.5
Cigarette buttsa 0.755 ± 0.32 25.6 0.078 ± 0.02 15.7 0.041 ± 0.01 16.4 23.7
Metala 0.074 ± 0.02 2.5 0.024 ± 0.01 4.9 0.019 ± 0.01 5.1 3.2
Glassa 0.023 ± 0.01 0.8 0.006 ± 0.00 1.2 0.003 ± 0.00 1.0 0.8
Sharp ceramic a 0.004 ± 0.00 0.1 0.027 ± 0.04 5.4 0.000 ± 0.00 0.0 0.8
Ceramic 0.008 ± 0.00 0.2 0.105 ± 0.11 21.3 0.000 ± 0.00 0.0 3.0
Cloth/textile 0.005 ± 0.00 0.2 0.002 ± 0.00 0.3 0.001 ± 0.00 0.3 0.2
Paper/cardboard 0.056 ± 0.06 1.9 0.008 ± 0.00 1.7 0.008 ± 0.09 3.1 1.9
Processed wood (with nails)a 0.003 ± 0.00 0.1 0.001 ± 0.00 0.2 0.003 ± 0.00 1.0 0.2
Processed wood Total 0.020 ± 0.02 0.7 0.006 ± 0.00 1.2 0.011 ± 0.01 4.4 1.0
Others 0.011 ± 0.01 0.4 0.007 ± 0.01 1.3 0.008 ± 0.00 3.1 0.7
Total 2.994 ± 1.21 100 0.493 ± 0.09 100 0.243 ± 0.04 100 100
CCI 58.9 ± 24.2 9.9 ± 1.8 4.9 ± 0.9
CCI Classific. Extremely dirty Moderate Clean
HALI 5.91 1.14 0.62
HALI type V III II
a
Categories used for HALI calculation.
= 0.74), pellets (r = 0.95), and plastic (r = 0.95) were positively 2021). Therefore, an accurate identification of plastic sources is
correlated with the number of residents in each sampling site (p a challenge to overcome. For instance, cotton swabs are floating
< 0.05). In contrast, no significant correlations (p > 0.05) were items commonly found on highly urbanized beaches with poor
seen among total AL, cloth/textile, ceramic, MT, processed wood, sewage treatment (Poeta et al., 2016), which were also seen in the
XPS, and others. studied area (Fontes et al., 2019; Roveri et al., 2020). Similarity,
Among all sampled sites together, plastics (65.5%) and CB plastic lids are also floating items that are connected mostly with
(23.7%) were the most frequent items. It is important to highlight tourism activities and can reach up 9.4% of all AL when combined
that, among plastic polymers, pellets and XPS accounted for 16.4% in categories including plastic caps and cups (Simeonova and
and 10.9% of the total AL, respectively. In addition, plastic lids, Chuturkova, 2019; Vlachogianni et al., 2018). Ribeiro et al. (2021)
cotton swabs, condoms, and MT were present at lower frequen- found MT accounting a maximum of 0.9% of total AL in 2019
cies (<5%). The presence of plastic items amounts were similar at Santos and São Vicente beaches. This item is linked to both
to those reported by several studies around the world at similar tourism and poor domestic sewage treatment (Simeonova et al.,
beaches, in which have been found amounts ranging from 61% to 2017).
87% (Asensio-Montesinos et al., 2020; Corraini et al., 2018; Gjyli Currently, it is well-known that CB compose between <1%
et al., 2020; Munari et al., 2016; Nachite et al., 2019; Sarafraz and 20% of all AL monitored beaches worldwide (Pieper et al.,
et al., 2016; Šilc et al., 2018; Terzi et al., 2020). Nevertheless, some 2019; Suciu et al., 2017). However, CB amounts reaching up to
of those studies considered CB within the plastic category, which 53.2% of total AL have been reported in Italy (Munari et al., 2016),
is a misconception, since those residues are made of different Morocco (Maziane et al., 2018), Bulgarie (Simeonova et al., 2017),
materials, including tobacco, paper, ashes, and cellulose acetate Chile (Hidalgo-Ruz et al., 2018), Hawaii (Blickley et al., 2016) and
filter (Araújo and Costa, 2019). In addition, the frequency of plas- Argentina (Becherucci et al., 2017). According to Andrades et al.
tic litter was similar to the one reported by Ribeiro et al. (2021) (2020), this item represents 10.8% of all AL found on 44 Brazilian
on nearby Santos and São Vicente beaches in 2019 (67.45%). beaches. CB has been pointed out with great ecotoxicological
Considering only S1, plastic was 67.7% of all AL, which is a slightly potential for coastal ecosystems, especially due to the large load
smaller than values (72.2%) found by Ferreira and Lopes (2013) on of hazardous chemicals (e.g., toxic metals, PAH and nitrosamines)
the same site in 2011. Andrades et al. (2020) found that plastic that can be leached into the water column and sediments after in-
was the most abundant material in 97.7% of 44 Brazilian beaches, adequate disposal (Araújo and Costa, 2019). In this regard, a core
representing 69.5% of all AL. Higher plastic occurrence, reaching set of factors including oceanographic features, meteorological
95% or more, have been measured in remote, urban and tourist parameters, beachgoers flow and efficiency of cleaning services
coastal areas (Pieper et al., 2019; Poeta et al., 2016; Prevenios may influence the occurrence of CB on beaches (Araújo and Costa,
et al., 2018; Wilson and Verlis, 2017). 2019).
The occurrence of plastic debris on beaches can have multiple Pellets are used to manufacture plastic products and were the
sources and is influenced by environmental factors such as coastal third most found items (16.42%) in the present study. According
currents, tides, river discharges, and winds (Cabral et al., 2019). to Pozo et al. (2020), pellets are spilled to the environment
In addition, there are important human dimensions that need to during production, packaging, and transportation, not being a
be considered such as tourist flows, proximity to urban centers, residue that reaches natural ecosystems from tourist or urban
cleaning services and local public policies into force (Ribeiro et al., sources. Due to the intense port and industrial activities, the
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V.V. Ribeiro, C.A.Y. Harayashiki, A. Ertaş et al. Regional Studies in Marine Science 46 (2021) 101902
occurrence of pellets has been frequently reported in monitoring CB, XPS, cotton swabs, and MT might present similar sources,
studies carried out in the region. Indeed, there are some records although contributions from local disposal can also occur.
of pellets contamination in S1 and S2, where amounts of up In addition to the chemical gradients, the studied sites also
to 255 pellets/m2 were found (Izar et al., 2019; Ribeiro, 2020; form a clear urban gradient, with a higher number of inhabitants
Ribeiro and Santos, 2020). Similarity, high pellets occurrence was and beachgoers flow at S1 and lower numbers at S2 and S3 due
also seen at Santos Bay beaches (Taniguchi et al., 2016; Turra to harder access to these areas. Therefore, the highest amounts
et al., 2014). Overall, such studies demonstrated that sites close and densities of AL were recorded at the semi-urban site S1,
to contamination sources presented higher pellet densities (Izar which also has the largest number of residents (5000 inhabitants).
et al., 2019; Moreira et al., 2016). The same pattern was observed Furthermore, relatively low litter quantities were seen in S2 (300
in the present study, with higher occurrence of pellets near to inhabitants) and S3 (uninhabited beach). In fact, the positive and
Santos Port in S1, and smaller amounts in S2 and S3. In addi- strong correlations observed between the number of residents
tion, pellets can act as vectors of several contaminants in the and CB, cotton swabs, glass, plastic lids, metal, paper/cardboard
marine environment and, therefore, pose as a threat to marine and total plastic suggest that at least some of these materials are
biota (Gorman et al., 2019; Rodrigues et al., 2019). Thus, it is locally sourced. In this regard, Leite et al. (2014) demonstrated
important to include this item during environmental monitoring significant higher densities and diversity of AL in areas nearby
of AL, especially in sites nearby potential contamination sources urban centers. Overall, our results corroborate with such findings
(Pozo et al., 2020). since a smaller amount of AL was collected in less populated
Polystyrene foam (XPS) is a widely used material recently zones. Moreover, condoms and ceramic were absent categories
identified as likely source and sink of contaminants to marine at the remote S3, reducing AL diversity in this site.
environments (Turner, 2021). It was the fourth most frequent In the present study, the highest CCI values was reported at
item in the present study (10.9% of total AL). In S1, XPS per- S1 (58.9 ± 24.2 - extremely dirty). In this same site, Ferreira and
centages were higher (8.5%) than previous report made in 2011 Lopes (2013) found a CCI of only 4.7 (clean) in 2011. This 10-
(0.03%) (Ferreira and Lopes, 2013). On the other hand, the XPS fold increase suggests a serious worsening of litter contamination
frequencies were similar to the ones seen during 2019 (9.6%) in the last decade at S1, which is a worldwide trend as pointed
in the nearby Santos and São Vicente beaches, which are more out by Nelms et al. (2020) and Weideman et al. (2020). The
urbanized and visited beaches in comparison to the three sites study conducted in 44 Brazilian beaches concluded that 29% of
from the current study (Ribeiro et al., 2021). The sources of XPS the beaches were classified as clean, 25% moderate, 22.7% very
are difficult to be distinguished due to a wide usage in construc- clean, and 11.3% extremely dirty and dirty (Andrades et al., 2020).
tion, fisheries, and packaging (Terzi et al., 2020). Since XPS is a Additionally, in the nearby highly urbanized Santos and São Vi-
floating material, it is possible that it reaches the studied areas cente beaches, Ribeiro et al. (2021) reported a CCI of 24.5 in
through estuarine discharges in addition to inadequate disposal 2019. Therefore, results from the present study showed that S1
by beachgoers (Poeta et al., 2017b). is dirtier than most Brazilian beaches, including beaches from
Ceramic, cloth/textile, glass, metal, and paper/cardboard are more urbanized areas such as Santos and São Vicente. Considering
known to be materials that normally have a local origin because that S1 is less frequented than Santos and São Vicente beaches,
they are not floating (Poeta et al., 2016; Topçu et al., 2013). the higher CCI found reinforces the hypothesis of contributions
Considering all studied beaches, those items represented up to from estuarine discharges as pointed out by Gorman et al. (2020)
3.2% of AL. However, they can reach up to 7% of AL on beaches based on pellet inputs. As seen for AL amounts and densities,
from Albania (Gjyli et al., 2020), Brazil (Ribeiro et al., 2021), and CCI values were progressively lower in S2 (9.9 ± 1.8 - moderate)
Spain (Asensio-Montesinos et al., 2019). According to Poeta et al. and S3 (4.9 ± 0.9 - clean), corroborating to gradient distribution.
(2016), there are three different potential sources of AL: beach According to Vlachogianni et al. (2018), several beaches located
usage, urban areas, and rivers influence. Thus, the beach usage in Adriatic and Ionian Seas presented moderate CCI values de-
by tourists and/or locals is the most likely source of those not spite different categorization as semi-urban, urban, and remote
floating items on the studied beaches. beaches. On the other hand, this was not the pattern seen by
Tides, rainfall regimes, and estuarine flushing are important the present study (extremely dirty, moderate, and clean) where
physical processes affecting the spatial distribution of contam- urban and hydrodynamic gradients drove AL distribution. Thus,
inants along estuarine systems. In these zones, pollutants may although the studied sites pose as an option for tourists that
be transported in solution or adsorbed to suspended particles. search for calm and clean beaches, the semi-urban beach (S1)
Highly hydrodynamics estuaries often export hazardous chemi- does not present these attractive characteristics. Moreover, in the
cals and materials towards open ocean, inducing contamination case of S2 and S3, the harder access and less inhabited status
levels in sites far from coastal sources (Castro, 2019). However, might be unappealing and confirm less tourist’s visitation, which
SES present low amplitude tides associated to high water resi- may confirm the lower AL abundance.
dence times originating clear gradients already demonstrated by The items categorized as HALs (i.e., CB, condoms, cotton swabs,
several studies assessing chemical levels and biological effects of glass, metal, MT, processed wood with nails, and sharp ceramic)
the contamination (Begliomini et al., 2017; Gouveia et al., 2019; in the present study were the same used by Ribeiro et al. (2021).
Oliveira et al., 2020; Pusceddu et al., 2019). In the present study, The HALI values found on studied beaches also followed the
a gradient pattern was seen considering significant spatial differ- contamination gradient (S1 > S2 > S3) already detected for haz-
ences in the amounts of total AL, total plastic, CB, pellets, XPS, ardous chemicals (Gouveia et al., 2019). In S1, the HALI was type
cotton swabs, metal, and MT. For such categories, higher amounts V (5.91), meaning that the beach is mostly covered with HALs.
and densities were observed in S1 with lower values in S2 and This HALI type was also seen in the remote Isla Arena (19.90) in
S3. In this sense, a study based on integrated rainfall data and Colombia (Rangel-Buitrago et al., 2020) and urban Playa Blanca
Lagrangian particle tracking models predicted the accumulation (9.40) in Chile (Maleki and Soria, 2020). Therefore, although S1
of pellets along the beaches of SES as observed in the present is not an urban nor remote beach, it may induce potential health
study (Gorman et al., 2020). These findings indicate that pellet risks for their beachgoers. The lower HALI values observed in S2
inputs on the studied sites are originated in internal portion of and S3 suggest progressively lower risks in these less frequented
SES where port and industrial facilities are installed. On the other beaches. In Latin America, most HALI types reported for urban
hand, it is important to highlight that plastics (other than pellets), and visited sites were between II and III (Rangel-Buitrago et al.,
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