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Short-chain chlorinated paraffins (SCCPs) are persistent organic pollutants. In Japan, SCCPs are widely detected in the environment although the production and use of SCCPs have been banned. It is essential to estimate the amount and sources of SCCPs to implement countermeasures for SCCP emission. In this study, we estimated the emission and environmental concentrations of SCCP homologues in Japan from 1950 to 2050. Initially, the material flow of total SCCPs was estimated considering the material recycling process. The emission from each process during the entire life cycle of products containing SCCPs was estimated for each homologue. Volatilization factors of long-term-use products were specifically estimated from release factors and surface area, weight, and SCCP concentration of products containing SCCPs. The environmental concentrations were then estimated using the environmental fate model. In the material flow and emission estimation, parameter uncertainties, such as emission factors and SCCP application distribution, were considered, assuming each parameter follows a uniform distribution. The results of emission estimation suggested a decreasing trend of SCCP emission in recent years and continuation of this trend in the future. However, some emissions from long-term-use products may persist. In the future, products that have a long lifetime with closed-loop recycling, such as polyvinyl chloride wire-coating materials, are expected to significantly contribute to atmospheric emission. Moreover, recycled products may contain SCCPs. Based on the estimated concentration, the estimated water and sediment concentrations were within the range of the observed concentrations. Conversely, we could reduce the gap between the estimated and observed atmospheric SCCP concentrations compared with those in previous studies that did not consider the volatilization factor for each SCCP-containing product and material recycling process. However, a difference between the estimated and observed concentrations suggests that some unconsidered emission sources may exist that emit SCCPs into the atmosphere, such as SCCPs as impurities in medium-chain chlorinated paraffins, imported products containing SCCPs, and atmospheric advection from other countries. Hence, it is essential to calculate emissions from sources other than products that intentionally contain SCCPs produced in the past.

Different countries produce varying amounts of polychlorinated biphenyls (PCBs), have distinct patterns of use, and regulations for treatment and disposal. Therefore, long-term countermeasures require an understanding of historical and future emission trends at the national scale. In this study, we estimate historical PCB emissions from products containing PCBs, unintentional production related thermal processes, and disposal processes for products containing PCBs from 1950 to 2030 in Japan. In addition, in order to validate the results, we estimated PCB concentrations in environmental media using an environmental fate model and a sensitivity analysis was conducted. Our results show that total PCB emissions were approximately 2.6 tons in 2017, which was a dramatic decrease from peak emissions of 68.9 tons in 1970. We suggest that PCB emissions may continue to decrease, reaching 0.707 tons in 2030. This trend might be due to a change in the emission source; it was estimated that the main emission source in past and recent years was volatilization from large products containing PCBs. However, it is predicted that the main emission sources in the future will be unintentional PCB production from thermal processes and volatilization from small untreated products containing PCBs, although the estimation of environmental PCB levels suggested that there might be unknown emission sources. Additionally, the sensitivity analysis indicated that some parameters greatly influenced the estimation of recent and future emissions. In particular, there was no detailed information concerning the applications for PCBs, which potentially had a large influence on the estimation of future emissions.

Numerous reports have elucidated different statistical approaches to identify temporal trends in atmospheric persistent organic pollutant (POP) time series. However, the correlation of industrial activity with concentrations of atmospheric POPs in Japan has not yet been determined. Herein, a panel data analysis of a 16-year monitoring program (2003–2018) conducted by the Japanese Ministry of Environment was used to investigate a range of POPs in the atmosphere above Japan. This work focuses on polychlorinated biphenyls (PCBs), polychlorinated naphthalenes (PCNs), polybrominated diphenyl ethers (PBDEs), hexachlorobenzene (HCB), and pentachlorobenzene (PeCBz) collected each year at 53 sites across Japan. The panel analysis revealed that PCB, PCN, and PBDE concentrations were influenced by a combination of factors including year, industrial activity (municipal and industrial waste incinerators, cement kilns, steel industry, and secondary zinc production), population, temperature, and atmospheric boundary layer. However, HCB and PeCBz were not significantly affected by these factors. Industrial activity showed stronger positive correlations with all homologues of PCBs, PCNs, and PBDEs as compared to those demonstrated by population. Significant decreasing trends were identified for the atmospheric ∑ P B D E s (half-life t1/2 = 9.4 years), ∑ P C N s (t1/2 = 8.9 years), and ∑ P C B s (t1/2 = 13.5 years) concentrations, while HCB and PeCBz showed slightly increasing or steady levels. As a statistical tool, panel data analysis can contribute to the assessment of spatial and temporal trends of POPs at a national scale, while elucidating different behavioral responses to numerous environmental variables.