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Trends in Food Science & Technology 83 (2019) 86–98

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Trends in Food Science & Technology


journal homepage: www.elsevier.com/locate/tifs

Review

Trends of research on polycyclic aromatic hydrocarbons in food: A 20-year T


perspective from 1997 to 2017
Yaqing Suna,b, Shimin Wua,b,c,∗, Guangyi Gonga,b
a
Department of Food Science and Technology, School of Agriculture and Biology, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai, 200240, China
b
Bor S. Luh Food Safety Research Centre, Shanghai Jiao Tong University, 800 Dongchuan Road, Shanghai, 200240, China
c
Key Laboratory of Urban Agriculture (South), Ministry of Agriculture, 800 Dongchuan Road, Shanghai, 200240, China

A R T I C LE I N FO A B S T R A C T

Keywords: Background: Polycyclic aromatic hydrocarbons (PAHs) are widely found in nature and accumulated, enriched, or
Vegetable oil produced in food through multiple paths, posing a great risk to human health. With more and more studies
Tea established on PAHs, it is essential to sort out the publications, analyze hotspots and indicate emerging trends as
Smoking well.
Oxygenated, Nitro-, Halogenated, and
Scope and approach: We investigated 1110 studies originating from the Web of Science Core Collection in the
alkylated PAHs
field of “Food Science Technology” from the year 1997–2017. These studies were analyzed using HistCite and
Degradation
Toxicity CiteSpace. This review included the trends and comparisons of literature outputs, "star" papers and hotspots,
Risk assessment describing the emerging trend of research on PAHs in food.
Key findings and conclusions: The results indicated that the number of studies on PAHs in foods has been growing
at an average annual rate of 13% from the initial 11 articles to 127 articles. The high yield of PAH-related
research in Europe may be attributed to concerns related to olive oil and smoked meats. Besides, hotspots also
included the formation of PAHs in food processing, the concentration of PAHs in edible oils and smoked pro-
ducts, and the GC-MS method for detecting PAHs. Based on articles we have analyzed, it is worth mentioning
that determination of PAHs and derivatives still needs improvement. Moreover, with collective efforts from all
researchers, we hope that more progress will be made in the limit standards and toxicological evaluation for PAH
derivatives, as well as methods for the green removal of PAHs in food.

1. Introduction pollution. As early as 1976, the United States Environmental Protection


Agency (US EPA) selected 16 PAHs to assess the health risks of drinking
Polycyclic aromatic hydrocarbons (PAHs) refer to a large group of water, named the “16 US EPA priority PAHs.” Since then, these 16
persistent organic pollutants that contain two or more fused benzene PAHs have been widely accepted and monitored all over the world and
rings in their chemical structural. They are produced by the pyrolysis of serve as reference standards for PAH research in many fields, especially
organic compounds or incomplete industrial combustion (Abbas et al., in environmental and food studies. In 2002, to highlight the strongly
2018; Li, Chen, Zhang, Song, Mu, Sun, et al., 2018). According to their carcinogenic PAHs, the European Commission's Scientific Committee
relative molecular weight and the number of benzene rings, PAHs can on Food (SCF) reported 15 types of PAHs that should be heavily mon-
be divided into light PAHs (LPAHs, 2–4 rings) and heavy PAHs (HPAHs, itored in food, of which eight were members of “16 US EPA priority
more than 4 rings). Most of the PAHs have been proved to have ter- PAHs.” In 2005, the Joint FAO/WHO Expert Group on Food Additives
atogenicity, carcinogenicity and mutagenicity, posing a great threat to (JECFA) added a PAH to the EU standards. These 16 EU PAHs are
human health (Kim, Jahan, Kabir, & Brown, 2013; Ramesh et al., 2004). commonly referred to as the “15 + 1 EU priority PAHs,” distinguishing
PAHs are a large family of over 10,000 compounds, of which more from those of the US EPA. In 2008, the US EPA proposed a series of
than 100 are detected in the atmosphere (Wenzl, Simon, Anklam, & priority control on hazardous pollutants, including 28 PAHs.
Kleiner, 2006). Because of the harmful effects of PAHs on human The research on PAHs first began in the field of environmental
beings, scientists urgently need a standard to assess the degree of studies and mainly analyzed the industrial sources of PAHs. Further


Corresponding author. Department of Food Science and Technology, School of Agriculture and Biology, Shanghai Jiao Tong University, 800 Dongchuan Road,
Shanghai, 200240, China.
E-mail address: wushimin@sjtu.edu.cn (S. Wu).

https://doi.org/10.1016/j.tifs.2018.11.015
Received 10 July 2018; Received in revised form 14 September 2018; Accepted 9 November 2018
Available online 13 November 2018
0924-2244/ © 2018 Elsevier Ltd. All rights reserved.
Y. Sun et al. Trends in Food Science & Technology 83 (2019) 86–98

studies indicated that PAHs can migrate from the environment to crops visualization work afterwards. Web of Science (WoS) is a science-based
and food, such as oils, fruits and vegetables, seafood, smoked food, and indexing service originally developed by the Institute for Scientific
bakery products (Hong et al., 2016; Silva, Torres, Almeida, & Sampaio, Information (ISI) based on online subscriptions and is currently oper-
2018; Wang et al., 2018). Food production processes, especially those ated by Clarivate Analytics. It provides multiple databases covering
using high temperatures, such as baking, smoking, frying and roasting, interdisciplinary research, explores areas of expertise in many dis-
are more likely to generate and accumulate large amounts of PAHs ciplines, and provides comprehensive citations (Chi & Glanzel, 2017).
(Bertinetti, Ferreira, Monks, Sanches-Filho, & Elias, 2018; Rose et al., The search terms for the data were set as “polycyclic aromatic hydro-
2015). As to PAH generation in high-temperature, pyrolysis and oxi- carbons” OR ″polycyclic aromatic hydrocarbon” OR ″PAHs” OR ″PAH”,
dation of fat, protein and carbohydrates are induced and accelerated. which included several common expressions of PAHs. The search scope
This is conducive to the formation of PAHs. In addition to being gen- was “topic”, including title, abstract, author keyword and keyword
erated from environmental pollution and food processing, PAH con- plus. On this basis, the results were refined by year (1997–2017) and
tamination in food can be caused by contact with contaminated the WoS subject classification (Food Science Technology).
packaging materials. Notably, food has a great impact on the non-oc- To ensure the accuracy of the data, the titles and abstracts of the
cupational exposure to PAHs. For non-smokers, more than 70% of PAH resulting literature were screened to ensure that the results were re-
exposure can be attributed to food (Phillips, 1999). To measure human levant to the topic of the study and those that were incorrect or du-
exposure to PAHs, some potential biomarkers such as 1-hydroxypyrene plicates were excluded. Validated data were exported as “full record
in human urine have been monitored (Srogi, 2007). Therefore, research and cited references” in the form of plain text. Finally, 1110 valid
on PAHs in food has received more and more attention, and the number publications were obtained as the data for this study, including 75 re-
of papers on PAHs in food continues to rise. view papers relevant to PAHs in food.
Much of the literature on PAHs lacks the analysis of their research Among these reviews, 23 reviews focused on the detection methods
difficulties and trends. How to effectively organize, summarize and for PAHs in food. Fourteen reviews concerned the risk and safety as-
analyze these papers has become a difficult problem for researchers. As sessment of PAHs in food. The third hot topic belongs to the con-
a subject, bibliometrics is an effective method and an important tool for centration of PAHs in different foods reviewed in 12 papers. In addition,
assessing academic progress in a field (Gutiérrez-Salcedo, Martínez, 11 reviews on the formation and mechanism of PAHs in foods were
Moral-Munoz, Herrera-Viedma, & Cobo, 2017). This method studies published. Ten reviews on the physiological toxicity and five reviews on
scientific publications stored or indexed in large databases as a measure the biodegradation of PAHs were available in the WoS. Table 3 has
of academic quality and scientific impact through a network of bib- reflected the above concerns in the 75 reviews. Furthermore, this study
liographies (co-words, co-citations or co-authors) and, to some extent, expanded other four hot topics, namely PAHs in olive oil, tea and fish,
predicts future developmental trends (Batagelj & Cerinsek, 2013; and alkylated PAHs which were neglected in the previous reviews. They
Martínez, Cobo, Herrera, & Herrera-Viedma, 2014). Based on biblio- were also fully discussed in this paper.
metrics, scientific knowledge mapping has emerged, which enables the
mining, analysis and clustering of knowledge in specific fields with the 2.2. Analysis tools
aid of visual tools. Through this emerging discipline, scientists can in-
tuitively analyze the development context in the field and build a Bibliometric indicators and scientific knowledge maps were used to
network of relationships among the publications (Osinska & Bala, analyze the literature output and knowledge structure. In terms of lit-
2015). Among the various tools, CiteSpace and HistCite are two com- erature output, major active years, countries, institutions, journals, and
monly used software programs. CiteSpace is a multivariate, time-divi- important documents with different characteristics were obtained
sion, and dynamic citation visual analysis software that focuses on through HistCite. In terms of knowledge structure, research hotspots
analyzing the potential knowledge contained in scientific literature and and co-citation analysis were obtained through CiteSpace.
gradually develops in the context of scientometric data and information
visualization. Through visualization, CiteSpace can present the struc- 3. Trends and comparison of literature outputs on PAHs in food
ture, regularity, and distribution of scientific knowledge (Chen, 2006).
HistCite is another citation analysis tool. Through a powerful analysis 3.1. Trends of research outputs and citation
of document output (journals, institutions, countries, years), it can map
out the development context of a certain research field and lock im- The span of research published during the last several years shows
portant papers based on different standards (Garfield, 2009). These two the development speed and progress of research and reflects the con-
tools are widely used in bibliometrics and scientific knowledge maps. centration and exciting periods of research in relevant fields (Huffman,
Tho, Yeung, Wei, Chan, and So (2017) used visual structures to study Baldridge, Bloomfield, Colantonio, Prabhakaran, Ajay, et al., 2013). As
the application of remote labs in science education. Yang et al. (2013) shown in Fig. 1, the number of papers published has been increasing
used HistCite to study the achievements and hotspots of research re- over time.
lated to China's municipal solid waste. Zhao, Zhang, Wang, Wang, and According to the overall development trend, the relevant research
Ouyang (2017) used CiteSpace to make qualitative and quantitative progress can be divided into three stages. The first stage was from 1997
analyses of the progress on the molecular modeling of cyclodextrin. to 2004, with research work still in its infancy. A total of 129 papers
In this study, we aim to analyze the research on PAHs in food from were issued in this period of seven years, accounting for 11.6% of the
both global and individual perspectives based on online databases and total. The average annual publication was approximately 18 papers for
with the use of scientific knowledge mapping software. This review this knowledge base and experimental exploration period. The second
includes the trends and comparisons of literature outputs, “star” papers stage was from 2005 to 2010. There was a great increase in the number
and hot research topics, describing the emerging trend of research on of published papers, which more than doubled that from the previous
PAHs in food. period. A total of 288 papers were issued in six years, accounting for
25.9% of the total papers, and an average of 48 papers were published
2. Literature sources and research methods annually. The third stage was from 2011 to 2017, with the number of
the literature citations increasing exponentially. A total of 693 articles
2.1. Literature sources were published in the past seven years, accounting for 62.5% of the
total and an average of 99 articles were published annually.
The data in this study originated from the Web of Science Core Between 1997 and 2017, the total number of citations was 16,667,
Collection, laying the foundation for the software processing and and each article was cited approximately 15 times. At the same time,

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Y. Sun et al. Trends in Food Science & Technology 83 (2019) 86–98

Fig. 1. Annual publication and citation number from 1997 to 2017 (January 22, 2018) at Web of Science.

Table 1 attracted much attention from Spanish scientists. In addition, smoked


Top eight countries, institutions and journals in terms of publication. food is a traditional Spanish cuisine, and all kinds of smoked foods are
Ranking Name Number Percentage% affected the most by PAH pollution (Domingo, 2017; Ledesma,
Rendueles, & Díaz, 2014). It is worth mentioning that European coun-
Countries tries accounted for half of the top eight countries conducting food PAH
1 China 196 17.66
research. This reflects their research interests or goals due to the PAH
2 Spain 140 12.61
3 USA 99 8.92
problem and more stringent standard limits. In comparison, the sixth
4 Italy 78 7.03 top country, Brazil, focuses on PAHs in rapeseed oil, sunflower oil, corn
5 Germany 59 5.32 oil, and cane sugar (Molle, Abballe, Gomes, Furlani, & Tfouni, 2017;
6 Brazil 46 4.14 Tfouni & Toledo, 2007). This indicates that the research hotspots of
7 Japan 43 3.87
PAHs in foods are closely related to local specialty foods and eating
8 France 41 3.69
8 Poland 41 3.69 habits.
8 South Korea 41 3.69 Second, the number of papers published by different research in-
Institutions stitutes was sorted. The Chinese Academy of Sciences ranked first with
1 Chinese Academy of Sciences (China) 27 2.43
27 publications. The University of Vigo in Spain was in second place
2 University of Vigo (Spain) 20 1.80
3 Dresden University of Technology (Germany) 19 1.71
with 20, while Dresden University of Technology in Germany and the
3 University of the Basque Country (Spain) 19 1.71 University of the Basque Country in Spain tied for third place with 19.
5 University of Udine (Italy) 16 1.44 This was basically the same order as that sorted by countries as dis-
6 Spanish National Research Council (Spain) 15 1.35 cussed previously.
7 Max Rubner-Institute (Germany) 13 1.17
Finally, the research outputs were then ranked by their source
7 Rovira i Virgili University (Spain) 13 1.17
Journals journals. According to the rankings, Analytical Methods ranked first and
1 Analytical Methods 174 15.68 was far ahead with 174 articles. Journal of Agricultural and Food
2 Journal of Agricultural and Food Chemistry 126 11.35 Chemistry (126 articles) and Food and Chemical Toxicology (105 articles)
3 Food and Chemical Toxicology 105 9.46 had more than 100 papers. The number of papers published in these
4 Food Chemistry 86 7.75
5 Food Control 47 4.23
three journals exceeded 35% of the total. According to the main re-
6 Journal of AOAC International 37 3.33 search areas of the journals, the research on PAHs in food mostly fo-
7 Food Additives and Contaminants Part A 36 3.24 cuses on the testing techniques and methods of food samples from
8 Food Analytical Methods 30 2.70 different sources and has some implications for the chemical properties,
toxicity, risk assessment and degradation of PAHs in food. There are
still significant challenges to the analysis and pretreatment of PAHs.
research results and quality were also greatly improved, with the total
number of citations rapidly growing.
4. “Star” and valuable papers on PAHs in food

3.2. Comparison of research outputs between different countries, institutions Through HistCite's powerful bibliometric analysis function, articles
and journals with higher research values can stand out from different perspectives.
Table 2 shows the top three “star” papers under four different in-
Table 1 shows the top eight countries, institutions and journals in dicators.
terms of publication in 1110 related articles. LCS refers to the number of citations of the paper within the col-
First, at the national level, China with 196 papers, Spain with 140 lection, representing the importance of the literature in the field of
and United States with 99 ranked first, second and third, respectively. research. An article with a high LCS value is likely to be groundbreaking
The number of papers published by Chinese researchers outnumbered in the field and cited by many scholars. The paper from Kazerouni,
that by Spanish researchers by nearly 40% and that by US researchers Sinha, Hsu, Greenberg, and Rothman (2001) ranked first because more
by 100%. Chinese researchers focus on environmental pollutants, in- than 200 different foods were reported. This large size of samples
cluding the distribution of PAHs in foods. This may be attributed to the served as an extensive PAH concentration reference for other studies.
Chinese government's attention to environmental pollution in recent The paper from Stołyhwo and Sikorski (2005) ranked second mainly
years. The extreme concern and enthusiasm about research on PAHs in because of its wonderful review, which summarized the production,
food in Spain is related to and affected by the local people's eating sources and changes of PAHs in smoked fish and common detection
habits and the level of PAH contamination. Among the articles, most techniques. In addition, the authors proposed a food safety limit stan-
focused on olive oil and meat foods. Olive oil is native to Spain and is dard based on benzo[a]pyrene, which is a carcinogenic marker, setting
representative of the Mediterranean diet. However, the presence of high a good example. The research from Chen and Lin (1997) ranked third.
concentrations of PAHs in olive oil, especially in olive pomace oil, has The authors used gas chromatography and ion-trap detection (GC-ITD)

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Table 2
Top three “star” papers under four different indicators.
Ranking Paper Value

a
LCS
1 Analysis of 200 food items for benzo[a]pyrene and estimation of its intake in an epidemiologic study. Food and Chemical Toxicology, 2001, 39(5), 423–436. 77
2 Polycyclic aromatic hydrocarbons in smoked fish - a critical review. Food Chemistry, 2005, 91(2), 303–311. 53
3 Formation of polycyclic aromatic hydrocarbons during processing of duck meat. Journal of Agricultural and Food Chemistry, 1997, 45(4), 1394–1403. 44
LCS/tb
1 Concentrations and dietary exposure to polycyclic aromatic hydrocarbons (PAHs) from grilled and smoked foods. Food Control, 2011, 22(12), 2028–2035. 5.14
2 Determination of polycyclic aromatic hydrocarbons in grilled meat. Food Control, 2010, 21(5), 606–610. 5.00
3 Profiling, distribution and levels of carcinogenic polycyclic aromatic hydrocarbons in traditional smoked plant and animal foods. Food Control, 2016, 59, 5.00
581–590.
LCRc
1 Polycyclic aromatic hydrocarbons' formation and occurrence in processed food. Food Chemistry, 2016, 199, 768–781. 51
2 Contamination of meat products during smoking by polycyclic aromatic hydrocarbons: Processes and prevention. Food Control, 2016, 60, 64–87. 41
3 Review of the quantification techniques for polycyclic aromatic hydrocarbons (PAHs) in food products. Critical Reviews in Food Science and Nutrition, 2017, 38
57(15), 3297–3312.
LCS(e/b)d
1 PAHs content in sunflower, soybean and virgin olive oils: Evaluation in commercial samples and during refining process. Food Chemistry, 2007, 104(1), 16.00
106–112.
2 Polycyclic aromatic hydrocarbons (PAHs) in coffee brew samples: Analytical method by GC-MS, profile, levels and sources. Food and Chemical Toxicology, 2009, 14.00
47(4), 819–826.
3 Analysis of polycyclic aromatic hydrocarbons in vegetable oils combining gel permeation chromatography with solid-phase extraction clean-up. Food Additives 12.00
and Contaminants, 2007, 24(7), 758–767.

a
LCS: Local Citation Score.
b
LCS/t: Local Citation Score per year.
c
LCR: Local Cited References.
d
LCS e/b: Ratio of local citations in the end to local citations at the beginning of the period.

to evaluate the effect of different processing methods on the con- Kim (2017) reviewed the extraction and detection of PAHs in foods and
centration of PAHs in duck meat. The results showed that the con- compared the quantitative performance of different methods. These
centration of PAHs was highest in charcoal-fired ducks and decreased results were also similar to those from previous analyses.
gradually in smoked, roasted, steamed, and liquid smoke-flavored LCSe indicates the number of times the article was cited in the last
ducks. This early research on smoked foods provided valuable refer- three years, and LCSb indicates the number of citations that were made
ences for further in-depth studies on PAH contamination from smoke. in the first three years of publication. A high ratio of LCS e/b shows that
This means that LCS is closely relevant to the quantity, range, and re- there has been a relative increase in citations in recent years, and the
view quality of the literature and that widely consumed foods tend to be paper has received more attention than before. The number one team,
contaminated by PAHs. Teixeira, Casal, and Oliveira (2007), evaluated changes in the PAH
LCS/t refers to the local citation score per year from initial pub- concentration in soybean, sunflower and olive oil samples during re-
lication to the end of the collection. The higher the value is, the higher fining, including neutralization, decolorization and deodorization. The
the annual citation of the article and the stronger its vitality. The top second group, Orecchio, Ciotti, and Culotta (2009), measured the
paper reported the effect of different grilling conditions on the con- concentration of 28 PAHs in roasted coffee and concluded, based on the
centration of PAHs in different foods and evaluated the dietary intake ratio of the isomers, that most of the PAHs originated from the high-
and carcinogenic risk in children/adolescents and adults, covering temperature process. The third panel, Fromberg, Højgård, and Duedahl-
several key points in the study of PAHs (Alomirah et al., 2011). The Olesen (2007), used gel permeation chromatography with solid-phase
second paper reported NaOH saponification extraction, diatomite and extraction and gas chromatography-mass spectrometry to determine
SPE purification, and high-performance liquid chromatography-fluor- PAH levels in edible oils. The detection limit of the method was below
escence detection for the analysis of PAHs in barbecued foods, forming 0.3 μg/kg, and the recovery rate was 50–120%. The entire process was
a complete detection method and obtaining the support and recognition semi-automated, which is receiving more attention recently. This sug-
of researchers (Farhadian, Jinap, Abas, & Sakar, 2010). The third paper gests that PAHs in edible oils, PAH analytical methods, and changes in
presented several traditional Spanish smoked foods, including bread, PAH concentration during food processing have recently become re-
cheese, sausages and paprika. The concentration of PAHs in these foods search hotspots.
increased in turn, and low-molecular weight PAHs (fluorene and phe- The above four sets of star papers are derived from different in-
nanthrene) dominated, supporting the need for studies on more food dicators calculated by HistCite and reflect the focus of the researchers.
types (Fasano, Yebra-Pimentel, Martínez-Carballo, & Simal-Gándara, These papers have pioneering, long-lasting vitality, close relevance, or
2016). Interestingly and coincidentally, the top three papers all focused recent attention in the PAH research. To sum up, PAHs in smoked and
on smoked or grilled meat, demonstrating the lasting vitality of this grilled meat have been continuously developed over the past 20 years
theme, and was in line with the LCS results. and have long-lasting vitality. The detection methods and changes of
LCR refers to the number of records in the collection that are cited PAHs in the processing have not only been comprehensively reviewed,
by the paper. This number is an indication of the relevance between the but also become an area of recent concern.
paper and the collection. The top three publications were all the latest
and most important review articles on PAHs in food, summarizing the 5. Hot research topics on PAHs in food
hotspots and frontiers of related research in recent years from one or
more aspects. Singh, Varshney, and Agarwal (2016) summarized the Scientific literature is not an independent system but is rather in-
mechanisms of and interventions for the production of PAHs in foods by terrelated and constantly extending. The mutual citation of scientific
different processing methods. Ledesma, Rendueles, and Díaz (2016) literature reflects the objective law of scientific development and em-
summarized the contamination process, standard limits, and preventive bodies the accumulation, continuity and inheritance of scientific
measures for PAHs in smoked meat products. Bansal, Kumar, Kwon, and knowledge, as well as the interdisciplinary nature and infiltration of

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Fig. 2. Co-citation analysis obtained by CiteSpace.

various subjects. In total, 648 nodes and 2089 connections were obtained, as shown
Co-citation analysis refers to the co-citation relationship between in Fig. 2. The central area of the network shows a rather dense red
two documents in the reference list of a third cited document, and the circle. This indicates a high level of burst references, which indicates a
process of mining the co-citation of documents in a spatial data set of significant increase in citations from other years. A total of 16 different
documents can be considered a co-citation analysis. Co-citation analysis hot clusters (#0 to #15) were obtained through cluster analysis. The
of documents became the highlight and the earliest use of CiteSpace detailed feature information is shown in Table 3. According to
when this tool was developed (Chen, 2006). In view of the co-citation Rousseeuw (1987), the Silhouette value in the table is a parameter for
network, the relationship between the clusters and their locations can evaluating the clustering effect. The closer it is to 1, the higher the
reveal the intellectual structure of a field and gives the reader a holistic network homogeneity. When the value is above 0.7, the clustering re-
view of the field. sult becomes highly reliable. In the following, a brief analysis of the
Fig. 2 shows the results of the citation analysis of 50 references with specific research groups was made, and the central or burst literature in
the most annual citations according to CiteSpace. In this network, each each cluster was presented in the order of its respective ID.
node represents a piece of literature, expressed in the form of “author's
name & publication year”. The “tree ring history” around the node Table 3
represents the citation history of the article: the overall size of the Cluster analysis and feature information.
annual rings represents the number of times each article is cited. The
Cluster ID Labela Size Silhouette
color of the annual rings represents the corresponding citation time
(blue for the earliest citations and red for the most recent citations). The #0 Olive oil 75 0.553
thickness of the annual ring is proportional to the number of citations in #1 Formation 58 0.764
the corresponding time zone. The connection between the nodes re- #2 Content 48 0.724
#3 Smoked meat food 41 0.826
presents a common reference, and the color of the line represents the
#4 Gas chromatography 40 0.793
first co-citation time (blue is the oldest and red is the nearest). The more #5 Alkylated derivative 39 0.831
connections a node has with other nodes, the more central the docu- #6 Various organic environmental pollutants 36 0.756
ment represented by that node is. On this basis, the nodes are clustered #7 Tea infusion 29 0.824
according to the results of the software calculation. Different nodes #8 Sample treatment 28 0.965
#9 Pelagic fish species 24 0.91
form different clusters according to their interconnectivity. Each cluster #10 Meat product 23 0.875
is a group of closely coupled documents, representing different research #11 Commercial liquid smoke flavoring 20 0.996
directions and backgrounds in the field. From the topics in this group of #12 Food contaminant 19 0.982
documents, representative keywords were extracted as the group's la- #13 Environmental analysis 12 0.99
#14 Salmo salar 12 0.945
bels through a log-likelihood ratio, expressed in the form of
#15 Toxicological issue 4 0.994
"# + cluster ID + keyword” in Fig. 2, according to a previous method
(Chen et al., 2009; Rorissa & Yuan, 2012). a
Label: Obtained by log-likelihood ratio.

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Table 4
Maximum levels and regulations for PAHs in foods worldwide.
Product Benzo[a]pyrene (μg/ Sum of PAH4a (μg/kg)
kg)

European Unionb
Oils and fats (excluding cocoa butter and coconut oil) intended for direct human consumption or use as an ingredient in food 2.0 10.0
Cocoa beans and derived products 5.0 μg/kg fat 30.0 μg/kg fat
Coconut oil intended for direct human consumption or use as an ingredient in food 2.0 20.0
Smoked meat and smoked meat products 2.0 12.0
Muscle meat of smoked fish and smoked fishery products 2.0 12.0
Smoked sprats and canned smoked sprats (Sprattus sprattus); Smoked Baltic herring ≤ 14 cm length and canned smoked Baltic 5.0 30.0
herring ≤ 14 cm length (Clupea harengus membras); Katsuobushi (dried bonito, Katsuwonus pelamis); bivalve molluscs
(fresh, chilled or frozen); heat treated meat and heat-treated meat products sold to the final consumer
Bivalve molluscs (smoked) 6.0 35.0
Processed cereal-based foods and baby foods for infants and young children 1.0 1.0
Infant formulae and follow-on formulae, including infant milk and follow-on milk 1.0 1.0
Dietary foods for special medical purposes intended specifcally for infants 1.0 1.0
Cocoa fibre and products derived from cocoa fibre, intended for use as an ingredient in food 3.0 15.0
Banana chips 2.0 20.0
Food supplements containing botanicals and their preparations; Food supplements containing propolis, royal jelly, spirulina or 10.0 50.0
their preparations
Dried herbs 10.0 50.0
Dried spices with the exception of cardamon and smoked Capsicum spp. 10.0 50.0
Chinac
Grain (Brown rice, rice, wheat, wheat flour, corn, cornmeal) 5.0 –
Meat products (Smoked, roasted, grilled meat products) 5.0 –
Aquatic products (Smoked, roasted aquatic products) 5.0 –
Fats and oils 10.0 –
Canadad
Olive pomace oil 3.0 –
Brazile
Olive pomace oil 2.0 –

a
PAH4: Benz[a]anthracene, benzo[b]fluoranthene, benzo[a]pyrene, chrysene.
b
European Union: According to Commission Regulation (EC) No 1881/2006 (December 19, 2006), (EU) No 835/2011 (August 19, 2011), (EU) No 1327/2014
(December 12, 2014), (EU) 2015/1125 (July 10, 2015) and (EU) 2015/1933 (October 27, 2015).
c
China: According to National Food Safety Standards GB 2762–2017 (March 17, 2017).
d
Canada: According to Health Canada's maximum levels for chemical contaminants in foods (January 25, 2018).
e
Brazil: According to National Health Surveillance Agency Resolution n° 281 (October 6, 2003).

Olive oil. Most PAHs are highly lipophilic. This leads to widespread and home cooking (such as baking, drying, roasting, grilling, frying,
PAH presence in various vegetable oils. Among PAH-contaminated barbecuing, and smoking). The production of PAHs during food pro-
edible oils, olive oil arouses great concern due to the high PAH level in cessing and cooking depends on processing temperature and time, the
olive pomace oil. Controlling the concentration of PAHs in olive oil is a fuel used, the distance from the heat source, and the compositions of
prerequisite for its healthy value. Olive oil can be divided into different the material, such as lipid, proteins and pro-oxygens. In addition,
grades according to their quality, from high-quality extra virgin olive higher pH was reported to increase PAH concentration in fried chicken
oil to low-quality olive pomace oil. Extra virgin olive oil is produced in (Wongmaneepratip & Vangnai, 2017). Furthermore, PAHs can form
specific regions and extracted from olive fruits only by mechanical and during edible oil storage (Zhao, Gong, & Wu, 2018). It is worth noting
physical methods without any further high-temperature roasting and that there have been several mechanisms on the formation of PAHs in
refining. Normally, extra virgin olive oil contains very low amounts of fuel combustion. The most popular of these is the hydrogen-abstraction-
PAHs, which only originate from the tree. In comparison, olive pomace acetylene-addition (HACA) mechanism. It involves extracting H from
oil is produced by drying the olive pomace through burning smoke and the PAH by another H atom to create a free radical site. This is followed
hot air, followed by solvent extraction. These processes result in a high by C2H2 addition to the radical site and ring closure (Sinha & Raj,
PAH concentration in olive pomace oil. Therefore, olive oil fraud or 2016). In a high temperature environment, resonantly stabilized radi-
adulteration is commonly found in PAH investigations and includes the cals such as propargyl, cyclopentadienyl and benzyl groups can form 2-
incorporation of extra virgin olive oil with olive pomace oil. In the past ring and 3-ring PAHs, and can further form PAHs of four or more rings
20 years, many publications have focused on PAH determination in by aromatization of steroids (Gong et al., 2018). However, the forma-
olive oil. Microwave heating instead of high-temperature drying was tion mechanism of PAHs in food during processing and storage remains
recently reported to minimize the concentration of PAHs in olive po- unclear. The mainstream view is that the radicals generated by the
mace oil (Kiralan, Erdogdu, & Tekin, 2017). Nevertheless, refined olive pyrolysis of organic matter at high temperatures can form stable
pomace oil containing PAH levels that are under the legal limitation or polynuclear aromatics by recombination and form PAHs through the
similar to those in extra virgin olive oil should not be mislabeled. Diels-Alder reaction (Chen & Chen, 2001). PAHs may be formed by
PAH formation. As a group of persistent organic pollutants, PAHs are Maillard reaction (Britt, Buchanan, Owens Jr., & Skeen, 2004) and li-
mainly formed by the condensation and cyclization of smaller organic pids oxidation (Guillen & Goicoechea, 2008). In 2011, a research in-
compounds in industrial productions and human activities dicated that cholesterol and androsterone are prone to produce a higher
(Arditsoglou, Petaloti, Terzi, Sofoniou, & Samara, 2004). PAHs pro- proportion of PAHs at 300–500 °C (Christy, Lian, & Francis, 2011). In
duced in the environment can be introduced into the food chain 2016, the formation mechanism of benz[a]anthracene and chrysene
through the enrichment and uptake of plants and animals, including was attributed to cyclopentadienyl, indenyl, and benz[f]indenyl radi-
from contaminated air, soil and water to organisms. In addition, PAHs cals (Oz & Yuzer, 2016). Recently, Min, Patra, and Shin (2018) used
in food can also derive from packaging materials, industrial processing electron spin resonance to study the role of lipid precursors in the

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formation of PAHs in meat model systems. They indicated that the resolution of heavy PAHs (Bansal et al., 2017; Zhou, Jiang, Mao, Zhao,
formation of PAHs increased with increasing lipid precursor unsatura- & Lu, 2016). Single quadrupole analyzers with a single ion monitoring
tion. mode are common, while ion trap and triple quadrupole are less often
PAH content. The PAHs presently detected in foods are mostly in used (Russo, Avino, & Notardonato, 2017; Varlet, Serot, Monteau, Le
concentrations of μg/kg (such as in edible oils) or ng/mL (such as in Bizec, & Prost, 2007). Some high-resolution mass spectrometers (such
beverages). These units are widely used in different food categories. So as time-of-flight) have a high degree of selectivity and very low de-
far, edible oils, cereals, smoked foods, seafoods, teas, baked goods and tection limits (Quesada-García et al., 2013). At the present, the detec-
fried foods have been reported to contain relatively high concentrations tion limits of PAHs in food are at (sub-)ppb levels in most studies. In
of PAHs. Most of these foods have been subjected to high temperatures, other words, the development of GC-MS has played a positive role in
exposure to open flames, or enrichment with PAHs at high levels in the improving the analysis of PAHs.
food chain or have a higher oil content that can easily absorb and GC-MS for PAH determination has been validated as standard
produce PAHs. method in many countries (Purcaro, Barp, & Moret, 2016). It is worth
The PAH concentration in food has always been a hot topic. On one mentioning that HPLC coupled to a fluorescence detector (FLD) has
hand, many countries are constantly lowering their limitation standards been widely used for PAHs determination in foods. This method was
for PAHs. Among them, the latest limitation standards of PAHs in also validated by Association of Official Analytical Chemists (AOAC),
European Union, China, Canada and Brazil are summarized in Table 4 European Food Safety Authority (EFSA), International Standardization
(Singh & Agarwal, 2018; Zelinkova & Wenzl, 2015). Except for Eur- Organization (ISO) and US EPA (Purcaro, Moret, & Conte, 2013). To
opean Union, other countries surveyed only restricted the concentration combine both advantages of GC and LC, online hyphenated techniques
of benzo[a]pyrene and focused on vegetable oils, grilled or smoked (LC-GC or LC-LC-GC) might be potential for reducing the amount of
foods and cereals. What's more, German food regulatory agencies have solvent and detection time (Moret & Conte, 2000). More dedicated PAH
recently lowered the maximum allowed concentration of benzo[a] analytical columns and databases are expected to make the analysis
pyrene to 0.01 μg/L in drinking water. On the other hand, PAHs are process more accurate and effective.
constantly detected in other foods in high concentrations due to in- Alkylated derivatives. Alkylated PAHs, which were the mainly con-
creased environmental PAH emission or contamination. cerned compounds in mineral oils, come from crude oil and the oil
Smoked meat food; Commercial liquid smoke flavoring. Smoking is one production process and migrate from the environment to food. In the
of the oldest methods used to preserve and season food, and its main oceans, alkylated PAHs in petroleum from drilling platforms and leaky
applications are meat, fish and cheese. However, the smoke generated ships are enriched in marine organisms, such as fish and scallops. This
by the combustion of wood contains many carcinogenic substances, not only causes illnesses in the marine organisms but also humans who
such as PAHs, which can migrate to the smoked food (Akpambang ingest them through the food chain (Lin et al., 2015; Uno et al., 2017).
et al., 2009; Stołyhwo & Sikorski, 2005). Studies have shown that the In addition, alkylated PAHs have also been found in smoked fish and
content of lignin in wood for combustion, the fat content in food, the vegetable oils (Stołyhwo & Sikorski, 2005). Notably, studies have
processing time and temperature are positively correlated with the shown that alkylated PAHs account for more than half of total PAHs in
concentration of PAHs (Essumang, Dodoo, & Adjei, 2013; Ledesma vegetable oils (Guillén & Sopelana, 2004). However, due to the lack of
et al., 2014). Although the concentration of PAHs in smoked food is data regarding accumulation, tolerable daily intakes of alkylated PAHs
high, these compounds are mainly distributed on the surface of the still remain to be established. As for the analysis of alkylated PAHs, LC
foodstuffs, and the removal of food epidermis when consuming can and GC followed by suitable pre-separation are the most common
significantly reduce the intake of PAHs (Fasano et al., 2016). The use of methods. A method for accurately quantifying alkylated PAHs in pet-
activated carbon to filter smog is also effective in reducing PAHs roleum based on relative response factors and GC-MS has been reported
(Essumang, Dodoo, & Adjei, 2014). To avoid the shortcomings of wood and is expected to be applied to foods (Yang, Zhang, Wang, Yang,
smoking, commercial liquid smoke flavorings have gradually become Hollebone, Landriault, et al., 2014). Moreover, comprehensive two-di-
an additive to produce smoked products. They are steam condensates mensional GC is demanding implement for alkylated PAHs analysis in
produced by wood retorting and have the advantages of cleanliness, foods (Purcaro et al., 2016). More studies have shown the potential
convenience and continuous production. Numerous studies have shown risks of alkylated PAHs to human health and should be given more
that PAHs in smoked food produced by liquid smoke flavorings are attention by researchers (Baird, Bailey, & Vorhees, 2007; Kang, Lee, &
significantly lower than those in food smoked by traditional wood Kwon, 2016).
(Zachara, Galkowska, & Juszczak, 2017; Šimko, 2005). In addition, Various organic environmental pollutants; Environmental analysis. As
highly carcinogenic benzo[a]pyrene was not detected in smoked food PAH is an organic environmental pollutant, the current research on
produced by sugar instead of wood, which is also a good alternative PAHs mainly focuses on the field of environment. In addition, many of
(Chen, Kao, Chen, Huang, & Chen, 2013). How to balance the unique the methods used to detect PAHs in foods originate from environmental
flavor and safety of smoked foods will continue to receive attention. analyses. Two excellent recent reviews on PAHs in the environment can
Gas chromatography (GC). Accurate quantitative analysis of PAHs in be found in the reference section (Cheruyiot, Lee, Mwangi, Wang, Lin,
food is a complicated and arduous task. GC combined with mass Lin, et al., 2015; Kuppusamy et al., 2017).
spectrometry (MS) get great attention due to its higher resolution and Tea infusion. Tea is the most widely consumed beverage in the world
PAHs detection with low (naphthalene and acenaphthene) or no (ace- after water. It is also a natural drink that has nutritional values and
naphthylene) fluorescence effects (Plaza-Bolaños, Frenich, & Vidal, health benefits for the human body. However, due to environmental
2010). In addition, the use of isotope-labeled internal standards factors (atmospheric deposition and soil uptake) and human factors
(deuterated PAHs) enables more accurate quantitative analysis and (fertilizers, processing and sewage irrigation), numerous contaminants,
structural elucidation (Li, Wu, Zeng, Wang, & Yu, 2016). For efficient including PAHs, remain in the tea leaves (Girelli, Apriceno, Tarola, &
separation of multiple PAHs, GC-MS analysis typically requires longer Tortora, 2017). In particular, the large surface area of the tea leaves
separation times (30–90 min) and columns (> 30 m). Based on the enables the accumulation of PAHs from the atmosphere, and the use of
traditional method, more novel devices have been applied in recent open flames for the smoke drying of tea leaves produces a high con-
years. In the field of chromatography, two-dimensional GC (GC × GC) centration of PAHs (Duedahl-Olesen, Navaratnam, Jewula, & Jensen,
can significantly improve resolution, but the raw data and chromato- 2015; Lin, Zhu, He, & Tu, 2006). Studies have shown that the con-
grams are complex and require powerful software tools for analysis centrations of benzo[a]anthracene and chrysene in smoked tea are
(Drabova et al., 2013). In the field of mass spectrometry, tandem MS higher than in non-smoked tea (Pincemaille, Schummer, Heinen, &
(MS-MS) eliminates the signal interference of lipids and improves the Moris, 2014). Due to the low solubility of PAHs in water, tea infusion

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can significantly reduce the uptake of PAHs. Only 3.03–7.69% of the fish and indirectly absorbed by the body. Studies of the pelagic fish
total PAHs contained in black tea is released into the tea infusion (Lin, species in the Atlantic indicate that the concentration of PAHs in chub
Tu, & Zhu, 2005). The mobilization rates for PAHs in green tea range mackerel is higher than that in horse mackerel and sardine, reaching
from 4.6 to 7.2%, and the concentration of PAHs in the first brewed tea 1.80–19.90 μg/kg wet weight (Ramalhosa et al., 2012). The con-
infusion is higher than that in the second (Gao, Chen, Liu, Hao, Ma, centration of PAHs in Salmo salar from Norway or the Irish Sea reached
Chai, et al., 2017). In addition, increasing the brewing time and 141.21–303.56 μg/kg dry weight (Visciano, Perugini, Amorena, &
opening the lid during brewing can also reduce the concentration of Ianieri, 2006). Due to the lipophilic character of most PAHs, the con-
PAHs in the tea infusion (Lin et al., 2006). To control the concentration centration of PAHs in fish is proportional to the fat content. Ad-
of PAHs in tea, it is necessary to reduce the local pollution level in the ditionally, the PAH level in fish is related to the seasons (Ramalhosa
production areas and improve the traditional high-temperature pro- et al., 2012). Moreover, the PAH concentration in processed fish foods
cessing methods. High tea polyphenol levels in the tea leaves may re- may be further aggravated on account of processing contamination,
duce PAH concentration in tea products, according to our latest studies such as grilling, smoking and repeated frying.
on inhibitory effects of natural antioxidants on PAHs in edible oils Meat product. In addition to the smoked meat products mentioned
(Gong et al., 2018). above, non-smoked meat products have also been found to contain
Sample treatment. A number of standards and review papers have appreciable levels of PAHs, including cured, preserved, grilled, fried
well described the efficient sample preparation methods. Normally, due and fermented meat products. One of the most important causes of PAH
to the high lipophilicity of PAHs, lipids are first extracted from foods production during roasting is attributed to the smoke created by the
and removed using suitable cleaning methods (Purcaro et al., 2013; incomplete combustion of fat dripping on the charcoal (Lee et al., 2016;
Zelinkova & Wenzl, 2015). Rey-Salgueiro, García-Falcón, Martínez-Carballo, & Simal-Gándara,
In most cases, PAHs exist in trace amounts in food. Due to the di- 2008). PAHs can be significantly reduced in the barbecue by the proper
versity and complexity of the ingredients in foods, food samples need removal of fat from meat and avoidance of direct contact between
proper pretreatment methods, including extraction, concentration and roasted smoke and food. Notably, the addition of onions and garlic in
purification, to improve the selectivity and sensitivity of detection. the grilling process can also reduce PAH concentration in the finished
Soxhlet extraction (Hilber, Blum, Leifeld, Schmidt, & Bucheli, 2012), products (Janoszka, 2011). PAHs in fried meat products are closely
ultrasonic extraction (Guatemala-Morales et al., 2016), microwave-as- related to the type of frying oil and the concentration of PAHs in the
sisted extraction (Purcaro, Moret, & Conte, 2009) and accelerated sol- background. Previous research has indicated that prolonged frying and
vent extraction (Kacmaz, Zelinkova, & Wenzl, 2016) are commonly repeated use of the same frying oil should be avoided (Hao, Li, & Yao,
used for solid foods during the extraction stage for PAH determination. 2016; Li et al., 2016). Compared with the above processing methods,
Compared to Soxhlet extraction, the latter two methods can reduce the boiling of meat results in lower PAH concentrations (Olatunji, Fatoki,
amount of the solvent used and the extraction time. This can improve Opeolu, & Ximba, 2014). This means that mild or simply processed
the efficiency and selectivity of extraction. Traditional liquid-liquid meat products can not only protect their nutritional value but also re-
extraction is usually used for liquid foods, but it is complicated, time- duce the production of harmful pollutants.
consuming, and labor-intensive. In this method, the light PAHs are li- Food contaminant. The contaminants in food can be divided into two
able to escape when the solvent evaporates in the concentration stage. categories. One is the environmental pollutants transferred from the
To achieve the highest yield and minimal loss of target substances, a environment to the food chain. The other is the process pollutants
quick, easy, cheap, effective, rugged, and safe (QuEChERS) extraction is generated by chemical reactions in the process of food cooking, pro-
currently used in the detection of PAHs in cereals (Deng & Chan, 2017), cessing and storage (Silano & Silano, 2017). Pollutants may naturally
meat (Han, Sapozhnikova, & Lehotay, 2016), chocolate (Sadowska- exist in the environment and may be either generated due to human
Rociek, Cieślik, & Sieja, 2015), and fish (Nácher-Mestre et al., 2014). activities or produced by fungi, plants, algae and other organisms
This procedure is based on acetonitrile extraction and the removal of (Domingo, 2017). Process pollutants mainly include acrylamide,
most of the disruptors by dispersive solid phase extraction. The purified chloropropanol, nitrosamines, heterocyclic amines, and PAHs. PAHs are
extract can be directly analyzed with high recovery and low detection both environmental pollutants and process pollutants. In many studies,
limits (Anastassiades, Lehotay, Štajnbaher, & Schenck, 2003). PAHs are often detected simultaneously with other food contaminants.
Clean-up methods for PAH analysis include column chromato- For example, the concentrations of acrylamide and PAHs in cocoa beans
graphy (Janoszka, 2011), gel permeation chromatography (Rojo are affected by the temperature, relative air humidity and time of the
Camargo & Toledo, 2003), solid phase extraction (Silva, Sampaio, & baking process (Żyżelewicz, Oracz, Krysiak, Budryn, & Nebesny, 2017).
Torres, 2017), and matrix solid phase dispersion extraction (Pensado, The concentration of PAHs and heterocyclic aromatic amines in steaks
Casais, Mejuto, & Cela, 2005). At present, simpler and more solvent- roasted with wire roasting is higher than that in steaks roasted with
friendly pretreatment methods are used, including solid-phase micro- stone (Oz & Yuzer, 2016). During processing, PAH concentrations are
extraction (García-Falcón, Pérez-Lamela, & Simal-Gándara, 2004), stir also associated with other food contaminants. One study indicates that
bar sorptive extraction (Lacroix et al., 2014), and dispersive liquid there is a strong positive correlation between the total amount of polar
phase microextraction (Mohammadi, Ghasemzadeh-Mohammadi, compounds and PAH concentration during the frying of edible oil (An,
Haratian, Khaksar, & Chaichi, 2013). In addition, a method named in- Liu, & Liu, 2017). The mechanism of interaction or transformation
pipe solid-phase microextraction is available for extraction and analysis between PAHs and other food contaminants still needs further study.
online (Sun, Feng, Bu, & Luo, 2015). Toxicological issue. Numerous studies have shown that PAHs have
Pelagic fish species; Salmo salar. PAHs in the oceans mainly come mutagenicity, genotoxicity and strong carcinogenicity. In the Ames test
from the accidental leakage of oil tankers or the leakage of fuel from for bacterial mutagenicity, most PAHs, especially those heavy PAHs,
vessels in navigation. In addition, some hydrophilic PAHs may also be gave positive results (Tamakawa, 2008). Among the many side effects
generated from dust particles and suspended particulate matter in the of PAHs, carcinogenicity receives the most attention. PAHs can cause a
atmosphere, rainwater runoff and discharge of rivers (Pelletier, Sargian, variety of cancers including digestive tract cancer, lung cancer and liver
Payet, & Demers, 2006). High concentrations of PAHs pose a significant cancer (Diggs, Huderson, Harris, Myers, Banks, Rekhadevi, et al., 2011;
threat to fish survival. It has been pointed out that PAHs released from Wang & Xue, 2015). There are four mechanisms for carcinogenesis of
the Deepwater Horizon oil spill in the northern Gulf of Mexico in 2010 PAHs, including the diol epoxide mechanism, the radical-cation me-
had a devastating effect on the pelagic fish in the area of the incident chanism, the quinone mechanism, and the benzylic oxidation me-
and was strongly cardiotoxic (Incardona, Gardner, Linbo, Brown, chanism (Ramesh et al., 2004). According to the SCF 2002 report,
Esbaugh, Mager, et al., 2014). PAHs are also abundant and enriched in benzo[a]pyrene (BaP) can be used as an indicator of total carcinogenic

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PAHs (Li et al., 2016). The potential health effects of PAHs can be through photochemical reactions and reactions with hydroxyl radicals,
quantitatively analyzed by using the toxicity equivalent factor (TEF) nitrate radicals and ozone. Likewise, oxygenated PAHs can also be
calculated from the toxicity of BaP (Hu et al., 2007; Zachara et al., produced or transferred during food processing (Chen, Shen, Su, Shen,
2017). According to the carcinogen list of the International Agency for Huang, Li, et al., 2014; Li et al., 2016). PAH derivatives are endocrine
Research on Cancer (IARC), benzo[a]pyrene is classified as Category 1, disruptors and produce reactive oxygen species, and some have a higher
benz[a]anthracene and dibenz[a,h]anthracene are classified as Cate- cytotoxicity than their parent PAHs (Walgraeve, Demeestere, Dewulf,
gory 2A carcinogens, and most other PAHs also potentially have car- Zimmermann, & Van Langenhove, 2010). Halogenated PAHs, mainly
cinogenicity (Manoli et al., 2016). Based on many studies, EFSA re- including chlorinated and brominated PAHs, originate from automobile
commended the sum of eight heavy PAHs (PAH8), or the sum of four exhaust emissions, waste incineration and a large amount of electronic
PAHs (PAH4), as an indicator of carcinogenicity in its 2008 report. In waste. Their toxicity increases with the number of substituent groups
2011, EFSA introduced a maximum standard for BaP and PAH4 in foods on the lower-molecular weight PAHs (three-ring and fluoranthene de-
(Moret, Purcaro, & Conte, 2010; Zhao et al., 2017). An analysis of the rivatives) (Sun, Zeng, & Ni, 2013). For these PAH derivatives, more
risk assessment studies in various countries showed that PAHs in the research is needed to evaluate their bioaccumulation or biomagnifica-
food are mainly derived from cereals, vegetables and oils. The EFSA tion through the food chain and their environmental transport. In ad-
2008 report also pointed out that cereal products, vegetables and meat dition, the details of potential hazards and human exposure to PAH
are the main contributors to the dietary intake of BaP in European derivatives through various pathways remain unclear. The relevant
consumers (Alexander, Benford, Cockburn, Cravedi, Dogliotti, Di detection technology for PAH derivatives in food also needs to be es-
Domenico et al., 2008). The concentration of PAHs in baked and tablished. Moreover, the greater scope of application and the corre-
smoked foods is relatively high, but their contribution to the total sponding maximum limit should also be reflected in the standards for
amount is not high due to their low daily consumption (Yebra-Pimentel, PAHs in foods.
Fernandez-Gonzalez, Martinez-Carballo, & Simal-Gandara, 2015). Third, methods to reduce or remove PAHs in food need to be de-
veloped, considering their serious pollution and consequent human
6. Emerging trends health risks. Commonly used methods in the past include decoloration
and deodorization in oil refining, the use of lower temperatures and the
Based on the analysis of the studies on PAHs during the past two avoidance of direct contact with the flame during grilling, as well as
decades, three key issues demand prompt solution. First, the determi- photodegradation under UV light. Recently, the addition or existence of
nation of PAHs still needs improvement. Previous efforts, including antioxidants in oils and marinades have been reported to reduce the
those related to equipment and pretreatment, have made great progress concentration of PAHs during storage, frying and grilling (Gong et al.,
in PAH analysis both in PAH types and LOD. Recently, QuEChERS 2018). These studies indicated that the formation of PAHs might be
consisting of dispersive solid phase extraction was reported to have related to free radicals. However, the detailed mechanism needs further
good recovery and precision (Petrarca & Godoy, 2018). Additionally, study. Moreover, biodegradation methods for PAHs are gradually
the detection range and applicability were reported to be further ex- emerging in view of sustainable solutions. Biodegradation, an efficient
tended compared to extraction conditions, such as solvents, buffer salts and environmentally friendly cleaning technology, attempts to use
and adsorbents, by using the QuEChERS method (Socas-Rodríguez, specific types of microbes (including bacteria, fungi, and microalgae) to
González-Sálamo, Herrera-Herrera, Hernández-Borges, & Rodríguez- degrade PAHs into harmless products (Alegbeleye, Opeolu, & Jackson,
Delgado, 2017). 2017; Ghosal, Ghosh, Dutta, & Ahn, 2016). In soil, the main fungal
Moreover, the development trends of future detection methods are group that causes PAH degradation is white rot fungi. They contain a
mainly reflected in the miniaturization of instruments and equipment, range of enzymes including lignin peroxidase and manganese perox-
the simplification of pretreatment processes, and the miniaturization of idase, which convert PAHs into a less harmful and simpler form. Many
test samples. Recently, the direct use of a programmed temperature algae species have the property of bioconverting contaminants into less
vaporizer and a quadrupole mass spectrometer without the need for harmful species (Haritash & Kaushik, 2009). However, many micro-
chromatography to detect PAHs in liquids was reported (Santos, organisms currently only have the ability to degrade a range of low
Sanchez, Pavon, & Cordero, 2018). In addition, the use of commercial molecular weight PAHs such as naphthalene, anthracene and phenan-
immunoassay methods and molded immunosensors also has prospects, threne. Their ability to degrade PAHs for five or more fused benzene
as reported in a latest review (Bansal et al., 2017). Nanotechnology is rings like BaP is rather limited (Juhasz & Naidu, 2000). Research on
also an efficient, convenient and fast emerging detection technology. bioaugmentation and bacterial-fungal co-cultures needs to be further
For example, polystyrene-coated magnetic nanoparticles (PSt/MNPs) deepened to enhance the ability to degrade PAHs. It is worth noting
have been reported for the detection of pyrethroid pesticides in vege- that biodegraded products of PAHs should also be isolated, identified
tables, fruits and vegetable oils with high precision and reproducibility and submitted for safety evaluation.
(Yu, Ang, Yang, Zheng, & Zhang, 2017; Yu, Li, Ng, Yang, & Wang, 2018;
Yu & Yang, 2017). g-C3N4/Fe3O4 nanocomposites have been reported 7. Conclusion
as new adsorbents for the detection of PAHs in water samples (Wang,
Cui, Yang, & Bi, 2015). A new core-shell nanostructure magnetic In total, 1110 research papers on PAHs in food published in the past
covalent organic framework hybrid microsphere (Fe3O4@COF-(TpBD)) 20 years were analyzed. Their citation and cited data were used for
can adsorb 99.95% of PAHs in food within 12 min, and the limit of bibliometrics and scientific knowledge mapping studies. A rising trend
quantification has reached 2.76–39.0 ng/L (Li, Wu, Hu, Fan, Li, Sun, can be clearly seen based on the overall output. The co-citation analysis
et al., 2018). The physicochemical properties of these nanomaterials obtained by CiteSpace obtained 16 hot research fields, mainly on the
deserve further improvement to increase their matrix adaptability and distribution, formation mechanism, pretreatment and detection tech-
binding specificity. niques, toxicological analysis and derivatives of PAHs in foods. In this
Second, PAH derivatives, such as oxygenated, nitro-, and haloge- study, to meet the requirements of data analysis, the literature source
nated PAHs, found in the atmosphere are also detected in foods covers the WoS Core Collection. To obtain more comprehensive and
(Table 5). These derivatives are detected mainly by GC-MS. The con- useful comments, other well-known databases, such as Scopus,
centrations of both oxygenated PAHs and halogenated PAHs are sig- SciFinder, and PubMed, may be combined with a large number of high-
nificantly higher in meat products compared with plant-based foods. So value documents in different languages other than English.
far, little data are available on the distribution of these compounds in Furthermore, upgrading the calculation methods in cluster analysis and
foods. Oxygenated and nitro-PAHs can be formed in the atmosphere using a powerful software might lead to a more comprehensive review

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Table 5
Distribution and analysis of PAH derivatives in foods.
Type of PAHs Sample Sample pretreatment technique Detection technique Concentration (μg/kg) References

a b c
Oxygenated PAHs (5 kinds) Youtiao (a popular Chinese fried LLE + SPE GC-MS 3.46–6.10 Gong et al. (2018)
bread)
Oxygenated PAHs (5 kinds) Soybean oil and rapeseed oil LLE + SPE GC-MS 0.93–6.56 Zhao et al. (2018)
Oxygenated PAHs (4 kinds) Smoked meat Microwave-accelerated reaction system + column chromatography GC-MS 9.26–20.50 Chen et al. (2014)
Oxygenated PAHs (15 kinds)i Fish ASEd + SPE GC-MS 28.00–1534.00 Bandowe et al. (2014)
Nitrated PAHs (2 kinds) Rice QuEChERSe HPLC-FLDf 0.86–4.19 Deng and Chan (2017)
Nitrated PAHs (12 kinds)j Smoked meat Microwave-accelerated reaction system + column chromatography GC-MS 4.29–7.32 Chen et al. (2014)
Nitrated PAHs (3 kinds) Meat product LLE + SPE UPLC-FLDg 2.00–249.30 Deng, Wong, Wang, Leung, and Chan
(2015)
Halogenated PAHs (5 Br-PAHs and 3 Cl- Rice LLE + column chromatography GC-MS 0.63–9.90(Br-PAHs) Ding, Ni, and Zeng (2012)
PAHs) 0.38–2.25(Cl-PAHs)
Halogenated PAHs (6 Br-PAHsk and 3 Cl- Pork LLE + column chromatography GC-MS 1.77–30.70 Ding, Ni, and Zeng (2013)
PAHs)
Halogenated PAHs (6 Br-PAHs and 5 Cl- Vegetables QuEChERS GC-MS/MS 0.36–0.87 Wang et al. (2018)
PAHsl)
h
Halogenated PAHs (6 Br-PAHs and 3 Cl- Seafood Soxhlet extraction + GPC + column chromatography GC-MS 0.79–6.73 Ni and Guo (2013)

95
PAHs)

a
LLE: Liquid-liquid extraction.
b
SPE: Solid phase extraction.
c
GC-MS: Gas chromatography-mass spectrometry.
d
ASE: Accelerated solvent extraction.
e
QuEChERS: Quick, easy, cheap, effective, rugged, safe.
f
HPLC-FLD: High-performance liquid chromatography-fluorescence detection.
g
UPLC: Ultra performance liquid chromatography.
h
GPC: Gel permeation chromatography.
i
Oxygenated PAHs (15 kinds): 1-indanone (1-INDA), 1,4-naphthoquinone (1,4-NQ), 1-naphthaldehyde (1-NLD), 2-biphenylcarboxaldehyde (2-BPCD), 9-fluorenone (9-FLO), 1,2-acenaphthenequinone (1,2-ACQ), 9,10-
anthraquinone (9,10-ANQ), 1,8-naphthalic anhydride (1,8-NAA), 4H-cyclopenta[d, e, f]phenanthrenone (4-CYPHENON), 2-methyl-9,10-anthraquinone (2-M-9,10-ANQ), benzo[a]fluorenone (B(a)FLONE), 7H-benzo[d,e]
anthracene-7-one (B(de)ANTHONE), benzo[a]anthracene-7,12-dione (B(a)ANTDIONE), naphthene-5,12-dione (5,12-NAA) and 6H-benzo[c, d]pyren-6-one (B(cd)PYRONE).
j
Nitrated PAHs (12 kinds): 1-nitronaphthalene (1N-NAP), 2-nitronaphthalene (2N-NAP), 5-nitroacenaohthene (5N-ACE), 2-nitrofluorene (2N-FLO), 9-nitroanthracene (9N-ANT), 9-nitro-phenanthrene (9N-PHE), 3-
nitro-phenanthrene (3N-PHE), 3-nitrofluoranthene (3N-FLA), 1-nitropyrene (1N-PYR), 7-nitrobenzo[a]anthracene (7N-BaA), 6-nitrochrysene (6N-CHR), 6-nitrobenzo[a]pyrene (6NeBaP).
k
Br-PAHs (6 kinds): 2-Bromofluorene (2-BrFle), 9-Bromophenanthrene (9-BrPhe), 9-Bromoanthracene (9-BrAnt), 9,10-Dibromoanthracene (9,10-Br2Ant), 1-Bromopyrene (1-BrPyr), 7-Bromobenz(a)anthracene (7-
BrBaA).
l
Cl-PAHs (5 kinds): 9-Chlorofluorene (9-ClFle), 9-Chlorophenanthrene (9-ClPhe), 2-Chloroanthracene (2-ClAnt), 9-Chloroanthracene (9-ClAnt), 9,10-Dichloroanthracene (9,10-Cl2Ant).
Trends in Food Science & Technology 83 (2019) 86–98
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