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Antifouling paints have a very harmful efect not only on marine organisms but also, through the food chain, on humans. Although the ban on tributyltin (TBT) has resulted in significant changes in the paint industry, its adverse effects are still present. This paper investigates the degree of pollution by antifouling paints. Previous studies confirmed contamination by organic compounds as a result of their long-term use in antifouling paints. Given that there has been no continuous monitoring of harmful antifouling systems at the national level, the authors point to the necessity of its implementation. Keywords - Antifouling; Pollution; Organotin tributyltin Introduction Croatia has about has total 1244 islands, islets, cliffs and reefs scattered all along its coastline, which is the main reason why it has been attracting a large number of leisure boats. Boat owners have problems with fouling organisms attached to underwater parts of boat hulls. Marine biofouling can be defined as a natural process of undesirable attachment and accumulation of microorganisms, plants and animals on underwater surfaces. Attaching organisms create friction that decrease the boat’s speed, manoeuvrability, and also increase fuel consumption. Antifouling coatings are used in maritime transport to control the growth of organisms such as algae and barnacles on underwater parts of boat hulls. Generally, antifouling paints can be divided into traditional and alternative antifouling coatings. Traditional antifouling coatings slowly release toxic elements from the paint applied on the underwater hull. While such coatings are very effective as they discourage the growth of fouling organisms, the toxic elements also slowly leak in the surrounding water and eventually fall to the sediment. Such marine biofouling can be reduced or eliminated, but unfortunately the release of hazardous substances also causes serious problems to the environment. Alternative antifouling coatings can generally be classified as biocide antifouling coatings and non-biocide antifouling coatings. Biocide antifouling coatings slowly release toxic substances such as zinc, fluorine, chlorine and various organic biocides. Non-biocide coatings contain silicon or have ceramic or epoxy basis, which may produce a slick surface thus making it difficult for organisms to attach [1]. One of the most effective antifouling paints was developed in the 1960s, with the organotin tributyltin (TBT) as main toxic component. It has been proven to cause serious problems to the environment. Copper-based antifouling paint is currently dominated on the market and its ions at low concentration may have influence on the health of animals and plants through the enrichment effect of food chain, causing damage to the ecological balance [1]. The toxicity of antifouling paints decades and attention has generally focused on the active substances. The toxicity of antifouling coatings has been debated during the last 30 years [2]. Focused studies have shown that toxic elements from antifouling coatings remain in the water and bottom sediment, killing sea-life, harming the environment and entering the food chain. A study conducted in the UK estimated that commercial vessel and pleasure boats are the single largest source of metals like copper and zinc in coastal areas, and also significant concentrations of irgarol and dichlofluanid have been detected in waters and sediments in marinas and mooring areas. Conducted research has shown that oysters located in the vicinity of marinas and mooring areas had significant copper content. Focused studies in Sweden have shown that especially at the time of launching pleasure boats (May–June), high concentrations of copper and irgarol have been measured in the archipelago of Stockholm [3]. Organotin tributyltin (TBT) has been globally banned for all sizes of ships by the International Convention on the Control of Harmful Anti-fouling Systems on Ships (AFS) Convention of the International Maritime Organization (IMO), but TBT and its degradation products, dibutyltin (DBT) and monobutyltin (MBT), are still observed in high concentrations in sediments at marinas, harbours and estuaries [4]. Being a significant tourist destination in the Mediterranean, especially during the summer season, Croatia has been attracting a large number of pleasure boats. These boats, together with boats owned by the local residents and merchant (passengers and cargo) ships, have been leaching significant concentrations of toxic elements from antifouling paints which have accumulated in the sea and the sediment. The main objective of this paper is to present the amounts of contaminants accumulated in some areas and to point to establish continuous monitoring of harmful antifouling systems. Marine biofouling, term Marine biofouling, settlement and growth of sedentary and semi-sedentary organisms at artificially sunken structures in the water, is a grave technical and economic problem [5]. It is a very dynamic process which can be affected by sea currents, mechanical damage, sea salinity, the amount of light, temperature, pollution and the availability of nutrients. Marine biofouling communities which can be found on immersed hulls are a special problem as they reduce the smoothness of the hull, thus increasing its resistance to passage through water. Fouled ships use more fuel to achieve necessary speed, which creates additional pollution of the atmosphere. The protective method used to prevent marine biofouling on vessels is applying antifouling paint. The application of antifouling paint must satisfy two basic criteria: Rejection of colonisation by micro- and macro-organisms Keeping the surface as smooth as possible Other desirable characteristics of antifouling paints include their low persistency, low toxicity for sea organisms, poor water-solubility, a broad spectrum of impact, acceptable price, easy application and low bioaccumulation. Vessels are normally coated once a year and in contact with water, the coating gradually dissolves and its active components infiltrate in the marine environment. The rate of dissolution varies from paint to paint, depending on the method of using the active components, pH, temperature, sea salinity, current velocity and the speed of the vessel. Released biocides are venomous for the marine environment and for people. Biocide coatings which contain stannyne are the most harmful. The toxic effects of tributyltin (TBT) can be seen already at concentrations of one nanogram per litre. The European Water Framework Directive lists TBT among the major pollutants and its application is forbidden in the EU countries. Among the coatings that started being used after the ban on the use of TBT, those containing copper oxide and zinc oxide prevail, although Directive 67/548/EEC categorized them as dangerous for the environment. Toxic components that are soluble in water may spread their toxic effect into the surrounding environment [6]. The biggest problem of contamination by antifouling paints lies in the fact that it is the ecosystems of enclosed and shallow seas that are the most exposed to it. Antifouling paints enter the water tower and remain there for some time. Sea tides, wind, local currents, adsorption of suspended particles and gravitational sedimentation are the most powerful mechanisms of their removal from the water column [7]. However, in seas like the Adriatic Sea, the exchange of water with the open sea is poor, which favours marine sediment deposition. The problem is only amplified with nautical tourism, which is one of the most profitable selective forms of tourist offer and which, considering the market, can be expected to lead to an increase in vessel mooring. Although the vessels individually do not represent a threat to the environment, the cumulative effect of a larger number of vessels found in confined waters represents a major source of contamination and other forms of degradation of the marine environment [8]. Legislation Marine environment protection imposes the necessity of legal regulation of activities related to the sea. Due to the threat that antifouling paints present to the environment and human health, their application in Croatia must comply with the following regulations: International Convention on the Control of Harmful Antifouling Systems on Ships - AFS Convention, 2001. The Convention was adopted with a view to prohibiting and/or restricting the use of harmful antifouling systems on ships, which comprise coatings, paints, surface treatments or agents. Moreover, the Convention establishes a mechanism for preventing the potential future use of other harmful substances in antifouling systems. Appendix 1 of the Convention lists systems whose use has been prohibited or whose application has been limited. At present, these are systems containing organic tin compounds, usually tributyltin – TBT, whose harmful effects on marine organisms have been proven. However, the list is not exhaustive and will be supplemented as needed. The Convention entered into force on 17th September 2008. The AFS Convention has been implemented in the EU which prohibits using harmful organotins, thus tributyltin and other harmful components, in antifouling paints on ships. Based on the adopted Convention and EC Regulations, and due to the harmful effects of some antifouling systems, special measures were introduced to control and prohibit entry into the Croatian ports to ships using harmful substances in antifouling paint and, moreover, the use of these systems is prohibited on ships of Croatian nationality [9]. Restriction of application of harmful substances in antifouling coatings in the EU is regulated by: Regulation (EC) No. 782/2003 adopted by the European Parliament and the Council on 14 April 2003, banning the use of TBT and other harmful components in antifouling coatings Since January 2008, EU member states have been required to prohibit and/or restrict the use of harmful antifouling systems on ships flying EU countries flag, as well as ships not entitled to fly their flag but which operate under their authority, and all ships that enter in EU ports, shipyards or offshore terminals. Ships of less than 24 metres in length are not required to have special examination or declaration. These ships include mainly recreational craft and fishing vessels, and are adequately covered by the provisions of Directive 76/769/EEC relating to restrictions on the marketing and use of certain substances and preparations in antifouling paints. The Croatian government, within the Mediterranean strategy, has adopted Mediterranean Strategy for Sustainable Development: A Framework for Environmental Sustainability and Shared Prosperity (UNEP(DEC/MED IG. 16/7)) An integral part of the Mediterranean Strategy for Sustainable Development is the requirement to improve the quality of coastal waters. The issue of toxicity of antifouling paints has been addressed in: Sustainable Development Strategy of the Republic of Croatia This Strategy comprises a plan to solve the problem of toxicity of antifouling paints [10]. Prevention of possible transfer of harmful marine aquatic organisms and pathogens through marine fouling has been regulated by: The Maritime Code Maritime objects are required to take measures to prevent the transmission of harmful marine aquatic organisms and pathogens through fouling [11]. The maintenance of freeboard and underwater parts of ship hulls is regulated by: Port's Rules and Regulations and rules and regulations on other parts of internal waters and the territorial sea of the Republic of Croatia Cleaning, scraping and painting of freeboard and underwater parts of ship hulls have been prohibited in port and at anchorage. Such activities may be carried out in the shipyards, while in ports they should be approved by the relevant port authority [12]. The concentration of TBT substances in the water has been regulated by: Regulation on Hazardous Substances in Water This Regulation prescribes the maximum allowable concentration (MAC) of tributyltin compounds in the waters [13]. To date, no continuous monitoring of harmful elements in antifouling paints has been carried out on national level. This is due to: discrepancies in the mode and location of sampling, ill-defined tasks for workers who will perform sampling, and insufficient number of specialists who will perform the analysis and interpret the results, which has led to an improper assessment of the sea condition. The new Environment Protection Act recognised the National List of Indicators (NLI) as a key document for drafting reports on the state of the environment at the national level. Control of harmful elements in antifouling systems is expected to become a reality shortly. The data will be provided by the Ministry of the Sea, Transport and Infrastructure and also by the Oceanographic and Fisheries Institute, each within their respective jurisdiction. Overview of previous studies of overload with antifouling paints in the Croatian part of the Adriatic In spite of its few areas with increased contamination (Gulf of Rijeka, Gulf of Bakar, the zone of Zadar, ٹibenik, Split with the Gulf of Kaڑtela, embouchure of the Neretva), the Adriatic Sea along the coast of Croatia is not a highly contaminated sea. In the past few years, several studies were carried out to establish the degree of its contamination. The Adriatic project was designed for the purpose of protection and preservation of the quality of the sea, and for creating conditions for safe economic development in accordance with the requirements of environmental protection, and the preservation and improvement of the achieved level of this protection. The results of analysis are shown in Table I. Concentrations of Organotin Compounds in Mussels Location2010. (µg Sn/kg)2013. (µg Sn/kg)Sveti IvanMBT=42.5©BuT=82MBT=11.4©BuT=31.9DBT=5DBT=0TBT=34.5TBT=20.5Plo eMBT=.9 ©BuT=203.8MBT=25.4©BuT=57.8DBT=63.2 DBT=3.6TBT=103.7TBT=28.8VranjicMBT=130.3©BuT=330.4MBT=58©BuT=185.4DBT=102.2DBT=15.4TBT=97.9TBT=112MartinskaMBT=137.9©BuT=234.9MBT=24.7©BuT=68.9DBT=49.2DBT=11.5TBT=47.8 TBT=32.7BakarMBT=124.3©BuT=354.8MBT=25.1©BuT=85DBT=106.6DBT=13TBT=123.9TBT=46.9RijekaMBT=96.3©BuT=276.2MBT=35.1©BuT=79.7DBT=94.1DBT=8.2TBT=85.8TBT=36.4Lim bayMBT=230.9©BuT=383.7MBT=21.4©BuT=55.2DBT=86.5DBT=0TBT=66.3TBT=33.8 In 2010, research conducted at 15 locations along the Adriatic coast investigated the concentrations of TBT and its degradation products DBT and MBT found in mussels. Table 1 shows the results of measurements at the seven locations where this was carried out also in 2013. The total concentration of butyltin compounds ("BuT = TBT + DBT + MBT) indicates the amount of TBT that has been released into the environment [14]. In 2010, the respective concentrations of organotin compounds found at the locations shown in the table were as follows: TBT: 34.5-123.9; DBT: 5-106.6; MBT: 36.9-230.9. The total butyltin compounds concentration (£BuT) range was 82-383.7 µg Sn/kg, average 233.22 µg Sn/kg. In 2013, the concentrations of organotin compounds were: TBT: 20.5-112; DBT: 3.6-15.4; MBT: 11.4-35.1. The total butyltin compounds concentration (£BuT) range was 31.9-185.4 mg Sn/kg, average 80.55 µg Sn/kg. In 2013, a new location, Marina Rovinj, was included and it showed the greatest overload of all locations investigated in 2013. The concentrations of organotin compounds found amounted to 119.2 for TBT; 83.7 for DBT and 150.9 for MBT, the total concentration of butyltin compounds (£BuT) being 353.8 µg Sn/kg. The results of analysis in sea sediment samples from marinas are shown in Fig. 1. Concentration of butyltin products at surface sediment in marinas, 2009. These concentrations were the highest in marinas, a little lower in ports, and the lowest in farms. This proves that pollution by organotin compounds is widespread along the Adriatic coast. Sea sediments, which are the final repository of heavy metals but also a source of contamination of water and wildlife, represent an issue apart. Many countries have introduced Cu regulations. Sweden has limited emissions on copper-bearing coatings in the Baltic to 200 µg/cm²/14-day, while the Netherlands bans cleaning or scrubbing copper-bearing antifouling coatings altogether. That the Cu problem is big is best illustrated by data from the USA. The estimates for total annual copper loadings from all discharges within a contiguous zone (<12 nm) is 121 675 kg/year; vessels hull coating leachate is responsible for 78% (93 929 kg/year) [15]. The results of the studies assessing the concentration of toxic elements in sediments near areas where ships are serviced along the Gulf of Kvarner and its islands were presented at the 2nd Scientific Symposium of Natural History Research in the Region of Rijeka in 2006. Concentrations of copper, zinc and lead, found in high levels in antifouling paints, were measured in Punat Bay. The results, expressed in ppm, were as follows: sediment depth 0-2 cm: Cu-46.4; Zn-167.1; Pb-43.4 sediment depth 2-4 cm: Cu-32.9; Zn-143.91; Pb-99.4 sediment depth 4-6 cm: Cu-25.1; Zn-61.7; Pb-25.5 sediment depth 6-8 cm: Cu-23.3; Zn-54.9; Pb-25.1 sediment depth 8-10 cm: Cu-24.3; Zn-55.91; Pb-14.3 The highest concentrations were present in the first two layers, the concentrations in the top layer being twice the value of the 8-10 cm layer. Given that heavy metals are not degradable, their concentration increases over time [16]. The increasing number of vessels in transit and at berth may lead to additional overload of sediment with heavy metals from antifouling paints in seaports and marinas, primarily due to increased concentrations of copper, zinc and lead. Another point worth mentioning is the problems caused by sport ports, especially during the preparation of boats for the season. The fact that sports ports present a significant source of pollution is due to relaxed understanding and lax application of regulations, and tolerance on the part of those responsible for enforcement of relevant regulations in them. Conclusion Vessel protection is based on continuous release of particles that prevent marine biofouling. Application of antifouling paint has an adverse effect on the sea environment, but this harmful effect spreads through the food chain from sea organisms also to humans. Once heavy metals like copper, arsenic, cadmium, chrome, nickel, lead and mercury get into the sea environment, they settle on the existing sediments. This is especially manifest in confined areas like gulfs and harbours. However, although use of TBT has been prohibited, its presence has been proven at 15 locations along the Adriatic coast. Changes in the sea environment due to contamination by vessels can permanently endanger the quality of the sea. For this reason, the above-mentioned causes of pollution must be monitored, controlled and sanctioned in accordance with positive regulations of the Republic of Croatia. In order to achieve comprehensive protection, systematic planning of human activities that must be in harmony with the environment is required. The state of the environment in Croatia is also important for the broader European and global context, so indicators of environmental pollution by antifouling paints could serve as the basis for international reporting to, for instance, the European Commission, the European Environment Agency or the United Nations. Given that that the damage caused by pollution cannot be removed completely, it is necessary to put in place preventive measures to obstruct its occurrence in the first place. Raising the ecological awareness of all the participants in nautical tourism and also of the society as a whole could positively affect the protection of the ocean ecosystem, which is the basis of sustainable development, particularly important in this century. 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