Formaldehyde in China: Production, consumption, exposure levels, and health effects

Formaldehyde, an economically important chemical, is classified as a human carcinogen that causes nasopharyngeal cancer and probably leukemia. As China is the largest producer and consumer of formaldehyde in the world, the Chinese population is potentially at increased risk for cancer and other associated health effects. In this paper we review formaldehyde production, consumption, exposure, and health effects in China. We collected and analyzed over 200 Chinese and English documents from scientific journals, selected newspapers, government publications, and websites pertaining to formaldehyde and its subsequent health effects.Over the last 20 years, China's formaldehyde industry has experienced unprecedented growth, and now produces and consumes one-third of the world's formaldehyde. More than 65% of the Chinese formaldehyde output is used to produce resins mainly found in wood products — the major source of indoor pollution in China. Although the Chinese government has issued a series of standards to regulate formaldehyde exposure, concentrations in homes, office buildings, workshops, public places, and food often exceed the national standards. In addition, there have been numerous reports of formaldehyde-induced health problems, including poisoning and cancer. The lack of quality epidemiological studies and basic data on exposed populations emphasizes the need for more extensive studies on formaldehyde and its related health effects in China.     

"Healthy" eye in office-like environments

Eye irritation symptoms, e.g. dry eyes, are common and abundant symptoms reported in office-like environments, e.g. aircraft cabins. To improve the understanding of indoor related eye symptomatology, relevant knowledge from the ophthalmological and indoor environmental science literature has been merged. A number of environmental (relative humidity, temperature, draft), occupational (e.g. visual display unit work), and individual (e.g. gender, use of cosmetics, and medication) risk factors have been identified, which are associated with alteration of the precorneal tear film (PTF); these factors may subsequently exacerbate development of eye irritation symptoms by desiccation. Low relative humidity including reduced atmospheric pressure further increases the water evaporation from an altered PTF; in addition, work with visual display units may destabilize the PTF by lower eye blink frequency and larger ocular surface. Results from epidemiological and clinical studies support that relative humidity >40% is beneficial for the PTF. Only few pollutants reach high enough indoor concentrations to cause sensory irritation of the eyes, while an altered PTF may exacerbate their sensory effect. Sustained low relative humidity causes impairment of the PTF, while its stability, including work performance, is retained by low gaze and intermittent breaks.     

Pollutant exposures and health symptoms in aircrew and office workers: Is there a link?

Sensory effects in eyes and airways are common symptoms reported by aircraft crew and office workers. Neurological symptoms, such as headache, have also been reported. To assess the commonality and differences in exposures and health symptoms, a literature search of aircraft cabin and office air concentrations of non-reactive volatile organic compounds (VOCs) and ozone-initiated terpene reaction products were compiled and assessed. Data for tricresyl phosphates, in particular tri-ortho-cresyl phosphate (ToCP), were also compiled, as well as information on other risk factors such as low relative humidity.A conservative health risk assessment for eye, airway and neurological effects was undertaken based on a “worst-case scenario” which assumed a simultaneous constant exposure for 8 h to identified maximum concentrations in aircraft and offices. This used guidelines and reference values for sensory irritation for eyes and upper airways and airflow limitation; a tolerable daily intake value was used for ToCP. The assessment involved the use of hazard quotients or indexes, defined as the summed ratio(s) (%) of compound concentration(s) divided by their guideline value(s).The concentration data suggest that, under the assumption of a conservative “worst-case scenario”, aircraft air and office concentrations of the compounds in question are not likely to be associated with sensory symptoms in eyes and airways. This is supported by the fact that maximum concentrations are, in general, associated with infrequent incidents and brief exposures. Sensory symptoms, in particular in eyes, appear to be exacerbated by environmental and occupational conditions that differ in aircraft and offices, e.g., ozone incidents, low relative humidity, low cabin pressure, and visual display unit work. The data do not support airflow limitation effects. For ToCP, in view of the conservative approach adopted here and the rareness of reported incidents, the health risk of exposure to this compound in aircraft is considered negligible.     

The dichotomy of relative humidity on indoor air quality

Dry and irritated mucous membranes of the eyes and airways are common symptoms reported in office-like environments. Earlier studies suggested that indoor pollutants were responsible. We have re-evaluated, by review of the literature, how low relative humidity (RH) may influence the immediately perceived indoor air quality (IAQ), including odour, and cause irritation symptoms (i.e. longer-term perceived IAQ). "Relative humidity" were searched in major databases, and combined with: air quality, cabin air, dry eyes, formaldehyde, inflammation, mucous membranes, offices, ozone, pungency, sensory irritation, particles, precorneal tear film, sick building syndrome, stuffy air, and VOCs. The impact of RH on the immediately and longer-term perceived IAQ by VOCs, ozone, and particles is complex, because both the thermodynamic condition and the emission characteristics of building materials are influenced. Epidemiological, clinical, and human exposure studies indicate that low RH plays a role in the increase of reporting eye irritation symptoms and alteration of the precorneal tear film. These effects may be exacerbated during visual display unit work. The recommendation that IAQ should be "dry and cool" may be useful for evaluation of the immediately perceived IAQ in material emission testing, but should be considered cautiously about the development of irritation symptoms in eyes and upper airways during a workday. Studies indicate that RH about 40% is better for the eyes and upper airways than levels below 30%. The optimal RH may differ for the eyes and the airways regarding desiccation of the mucous membranes.     

Chemical and biological evaluation of a reaction mixture of R-(+)-limonene/ozone: formation of strong airway irritants

The airway irritation of a reaction mixture of R-(+)-limonene and ozone was evaluated by a mouse bioassay in which sensory irritation, bronchoconstriction and pulmonary irritation were measured. Significant sensory irritation (33% reduction of mean respiratory rate) was observed by dynamic exposure of the mice, during 30 min, to a ca. 16 s old reaction mixture of ozone and limonene. The initial concentrations were nominally 4 ppm O3 and 48 ppm limonene. After reaction, the residual O3 was <0.03 ppm. Conventional analytical chemical methods were used to measure the formation of readily identified and stable products. Besides the expected products, 1-methyl-4-acetylcyclohexene (AMCH), 3-isopropenyl-6-oxoheptanal (IPOH), formaldehyde and formic acid, autooxidation products of limonene and a series of compounds including acetone, acrolein and acetic acid, which may or may not be artefacts, were identified. Addition of the sensory irritation effects of the residual reactants and all the identified compounds could not explain the observed sensory irritation effect. This suggests that one or more strong airway irritants were formed. Since limonene is common in the indoor air, and ozone is infiltrated from outdoors and/or produced indoors (e.g., by photocopiers), such oxidation reactions may be relevant for indoor air quality.     

Chemical and biological evaluation of a reaction mixture of R-(+)-limonene/ozone: Formation of strong airway irritants

The airway irritation of a reaction mixture of R-(+)-limonene and ozone was evaluated by a mouse bioassay in which sensory irritation, bronchoconstriction and pulmonary irritation were measured. Significant sensory irritation (33% reduction of mean respiratory rate) was observed by dynamic exposure of the mice, during 30 min, to a ca. 16 s old reaction mixture of ozone and limonene. The initial concentrations were nominally 4 ppm O₃ and 48 ppm limonene. After reaction, the residual O₃ was <0.03 ppm. Conventional analytical chemical methods were used to measure the formation of readily identified and stable products. Besides the expected products, 1-methyl-4-acetylcyclohexene (AMCH), 3-isopropenyl-6-oxoheptanal (IPOH), formaldehyde and formic acid, autooxidation products of limonene and a series of compounds (i.e., acetone, acrolein and acetic acid), which may or may not be artefacts, were identified. Addition of the sensory irritation effects of the residual reactants and all the identified compounds could not explain the observed sensory irritation effect. This suggests that one or more strong airway irritants were formed. Since limonene is common in the indoor air, and ozone is infiltrated from outdoors and/or produced indoors (e.g., by photocopiers), such oxidation reactions may be relevant for indoor air quality.     

Health effects of oxidants

Oxidants of significance to human health include ozone, nitrogen dioxide, and peroxyacetylnitrate. All of these compounds are involved in complex photochemical reactions which makes quantification and prediction of their individual health effects difficult. Ozone causes trauma to lung tissues and interferes with enzyme systems in the lungs and other tissues causing a broad range of symptoms. Measurable health impacts can occur at concentrations as low as 390 μg/m³. Acute effects of ozone exposure are reversible at normal urban concentrations (80–120 μg/m³). A special problem of concern, however, is increased susceptibility to infectious diseases contracted through the lungs. Nitrogen dioxide also causes trauma to lung tissues and interferes with enzyme systems. Measurable impacts can occur at concentrations as low as 100 μg/m³, but recovery is rapid and it is not known whether repeated exposures at this level have cumulative effects or predispose the lungs to permanent damage. Chronic exposure of laboratory animals to higher nitrogen dioxide levels can cause emphysema-like conditions and reduction in resistance to respiratory infection. Epidemiological studies of children in houses with gas stoves confirm the finding of reduced resistance to respiratory infection. The U.S. EPA estimates that health effects may occur in young children exposed to concentrations in excess of 280 to 560 μg/m³ one-hour average. These concentrations occur routinely in houses having gas stoves. Peroxyacetylnitrate is a powerful eye irritant in photochemical smog. Other health effects are similar to those of ozone, but less important because of the relatively low concentrations of this pollutant compared to other oxidants.     

A passive sampling device for determining formaldehyde in indoor air

A passive sampling device based on the principle of diffusion has been developed for the determination of formaldehyde in ambient air. The sampler consists of a capped glass tube (with approximate dimensions of 2.4 × 9 cm) containing a glass-fiber filter treated with NaHSO₃. In the field, the device collects a sample by being uncapped for a specified sampling time. After being recapped and returned to the laboratory, the filter is analyzed by the chromotropic acid (CTA) method. Laboratory validation studies were conducted by exposing the sampling devices for 1 week to dry formaldehyde gas generated by passing trioxane vapor over an acid catalyst bed. In these tests, formaldehyde concentrations ranged from 0.05 to 0.80 mL/m³. Reproducibility was excellent, with relative standard deviations averaging 5.4% for five constant concentrations. The lower detection limit was determined to be 3.6 mL/m³ h. In an occupational environment an 8-h sample would be sufficient to detect compliance with the OSHA permissible exposure limit of 3 mL/m³; in a residential environment a 1-week sample would allow detection of 0.025 mL/m³ for indoor air quality audits.     

Respiratory irritation due to carpet shampoo: Two outbreaks

Dried detergent residue left in carpets after they were shampooed with underdiluted carpet shampoo caused respiratory irritation among most employees in an office building and among all staff members and most children in a day-care center. Symptoms included cough, dry throat, difficulty in breathing, nasal congestion, and headache. Eye irritation was also noted by day-care center staff members. Symptoms persisted for many weeks until the carpets were wet extracted. The major ingredient of the three shampoo products implicated in these two outbreaks and in a third similar report in sodium dodecyl sulfate, a respiratory irritant in mice. Unpublished occupational investigations suggest that soap dust exposure may be associated pulmonary function abnormalities in some exposed workers. Detergent dust is a newly recognized example of indoor air pollution and should be considered when patients or employees complain of building-specific respiratory or eye irritation.     

Formaldehyde monitoring in urea-formaldehyde foam-insulated houses in St. John's,Newfoundland, Canada: Correlative field evaluation of a real-time infrared spectrophotometric method

Formaldehyde air levels in a group of houses containing urea-formaldehyde foam insulation (UFFI) in St. John's, Newfoundland, Canada, were measured on at least four separate occasions. The NIOSH method and a portable, commercially available single-beam infrared spectrophotometer was used. No correlation was found to exist between the two methods. The formaldehyde air levels were found to be significantly higher in the group of UFFI-insulated houses than in the control group which did not contain UFFI. Large daily variations in the ambient formaldehyde levels could be observed in some selected UFFI houses, attributable to changes in both exterior and, to a lesser extent, interior conditions. In particular, the effect of direct sunlight on UFFI-containing walls is described.     

Changes in serum levels of perfluoroalkyl substances during a 10-year follow-up period in a large population-based cohort

Poly- and perfluoroalkyl substances (PFASs) are a group of man-made fluorinated chemicals which have, at background levels, been associated with negative health effects in humans. Thus far, most human biomonitoring studies have evaluated the general change in PFAS concentration over time by continuously testing various individuals. This is one of the few studies to report the longitudinal trend of a range of PFAS concentrations in humans. In addition, this is the first known longitudinal study to include a large background level exposed cohort of both men and women with the same age and location who were repeatedly sampled from 2001 to 2014.The longitudinal change in concentration of eight PFASs detected in serum collected from the Prospective Investigation of the Vasculature in Uppsala Seniors (PIVUS) cohort were determined and compared to results from general population studies. The sex-dependent changes in PFAS concentrations over time were also assessed.Serum was sampled from the same individuals at ages 70 (collection period 2001–2004), 75 (2006–2009) and 80 (2011–2014,). Eight (C_6–11) of fourteen (C_4–13) analyzed PFASs were usually detected in over 75% of individuals and assessed using a random effects (mixed) model.In the 579 individuals attending all three examinations, PFOSA and PFOS concentrations significantly decreased, while the remaining six PFASs significantly increased between ages 70 and 75. However, between ages 75 and 80 all PFAS concentrations significantly decreased. Overall from age 70 to 80, concentrations of PFHxS, PFUnDA, PFNA, and PFDA showed a significant increase (7% to 34%), whereas concentrations of PFOSA, PFHpA, PFOS, and PFOA (− 75% to − 27%) significantly decreased. Over time PFHxS concentrations increased more among women, while PFHpA concentrations showed a greater decrease among men.From age 70 to age 80, spanning from 2001‐2004 to 2011–2014, the PIVUS cohort showed decreases in circulating levels of some PFASs phased out of production with the exception of PFHxS and C_>8 PFASs. Contrary to other studies, PFHxS concentrations showed the greatest overall increase, which is likely attributed to a local drinking water contamination incident.     

Interactions between diesel emissions and gaseous copollutants in photochemical air pollution: Some health implications

A complete assessment of the health effects of diesel emissions must take into account the possible chemical transformations (and associated biological impacts) of particulate organic matter (POM) due to reactions with the many gaseous copollutants which have now been unambiguously demonstrated to be present in atmospheres burdened by photochemical air pollution. These copollutants include the “trace” species, nitric (HNO₃) and nitrous (HONO) acids, the nitrate radical (NO₃), formaldehyde (H₂CO) and formic acid (HCOOH), as well as the criteria pollutants, ozone (O₃) and nitrogen dioxide (NO₂). Techniques for establishing the atmospheric concentrations of the trace pollutants (and their spatial and temporal variations) are briefly described, and we present results of investigations into the reactions of polycyclic aromatic hydrocarbons (PAH) coated on filters and exposed to ambient concentrations of O₃ and NO₂. Environmental health implications of these results are discussed and include the potential for sampling “artifacts” and their possible effects on the correlation (or lack thereof) between ambient PAH levels and urban lung cancer rates, as well as the problems associated with understanding the appropriate POM “dose” to be employed in animal testing and assessments of impacts on human health.     

Risk assessment of sensory irritants in indoor air--a case study in a French school

Exposure to airborne pollutants can result in adverse health effects. Acute symptoms can for instance comprise of irritation of the eyes or of the respiratory tract (called sensory irritation). In a recent case, health problems were reported in a French school and supposedly attributed to the presence of airborne irritant pollutants. Based on measured concentrations, the risk of developing the described health effects was assessed.Numerous airborne sensory irritants (aldehydes, organic acids, volatile organic compounds (VOCs), SO(2), NH(3)) were identified and quantified in the indoor air by using active and passive sampling and online monitoring techniques. Reference values based on toxicological properties of compounds (sensory irritants) were taken from the literature. If not available, tentative values were specially developed for this purpose. Concentrations of all sensory irritants remain below their corresponding guideline values and are comparable to literature data. It was concluded that the risk of developing sensory irritation due to the presence of the studied compounds is negligible. This holds both for individual compounds and for the mixture of studied compounds. Limitations of the employed sampling strategy, and of existing sampling and analytical techniques, which do not allow for analysing more reactive compounds-which are strong sensory irritants-may play a role. New sampling techniques need to be developed. Psychosocial factors (group behaviour, increased attention to sensory irritation) should also be taken into account when dealing with health complaints on sensory irritation.     

Human bones obtained from routine joint replacement surgery as a tool for studies of plutonium, americium and ⁹⁰Sr body-burden in general public

The paper presents a new sampling method for studying in-body radioactive contamination by bone-seeking radionuclides such as ⁹⁰Sr, ^239+240Pu, ²³⁸Pu, ²⁴¹Am and selected gamma-emitters, in human bones. The presented results were obtained for samples retrieved from routine surgeries, namely knee or hip joints replacements with implants, performed on individuals from Southern Poland. This allowed to collect representative sets of general public samples. The applied analytical radiochemical procedure for bone matrix is described in details. Due to low concentrations of ²³⁸Pu the ratio of Pu isotopes which might be used for Pu source identification is obtained only as upper limits other then global fallout (for example Chernobyl) origin of Pu. Calculated concentrations of radioisotopes are comparable to the existing data from post-mortem studies on human bones retrieved from autopsy or exhumations. Human bones removed during knee or hip joint surgery provide a simple and ethical way for obtaining samples for plutonium, americium and ⁹⁰Sr in-body contamination studies in general public.     

Pollutant emission rates from indoor combustion appliances and sidestream cigarette smoke

Particulate and gaseous emissions from indoor combustion appliances and smoking can elevate the indoor concentrations of various pollutants. Indoor pollutant concentrations resulting from operating one of several combustion appliances, or from sidestream tobacco smoke, were measured in a 27-m³ environmental chamber under varying ventilation rates. The combustion appliances investigated were gas-fired cooking stoves, unvented kerosene-fired space heaters, and unvented natural-gas-fired space heaters. Results showed elevated levels of carbon dioxide, carbon monoxide, nitric oxide, nitrogen dioxide, formaldehyde, and suspended particles from one or more of the pollutant sources investigated. Our findings suggest that, of the sources examined in this study, nitrogen dioxide from combustion appliances and particles from sidestream cigarette smoke are the most serious contaminants of indoor air, if we use existing standards and guidelines as the criteria. An emission rate model was used to quantify the strengths of the pollutant sources, which are reported in terms of the mass of pollutant emitted per energy unit of fuel consumed (in the case of gas and kerosene appliances) and per mass of tobacco combusted (in the case of smoking).     

A study of radium uptake by the water-lily Nymphaea violacea (Lehm) from contaminated sediment

The rate and extent of radium-226 accumulation from sediment by the water-lily Nymphaea violacea (Lehm) were assessed. The plants were collected from Magela Creek, Northern Territory, Australia and grown in ²²⁶RaCl₂-labelled laboratory sediment over a period of 570 days. The nominal sediment activity of 5 Bq g⁻¹ dry weight was 100 times that of the naturally occurring concentration.In the roots and rhizomes, ²²⁶Ra accumulated on plant surfaces. This result was confirmed by autoradiographic studies which showed the presence of an iron-containing plaque on the surface of these tissues with which the radium was closely associated. Little radium reached the pith of the rhizomes and acropetal translocation was not detected. The average concentration ratio for growing rhizomes was 0·22. Assuming first order accumulation kinetics and likely incremental environmental concentrations, this Aboriginal dietary tissue could become dose-limiting within 50 years.The foliar accumulation of radium originating from the sediment was predominately due to contamination via the sediment-water-plant pathway. Differences in foliar radium concentrations in plants of different ages were due to differential biomass turnover rates. Plants with faster biomass turnover had higher average radium concentrations.     

Determinants of urinary bisphenol A concentrations in Mexican/Mexican–American pregnant women

Prenatal exposure to bisphenol A (BPA) may be associated with adverse health effects in the developing fetus; however, little is known about predictors of BPA exposure during pregnancy. We examined BPA exposure in 491 pregnant women from the Center for the Health Assessment of Mothers and Children of Salinas (CHAMACOS) cohort and explored the role of living in the United States on significant dietary predictors of BPA exposure. Women provided urine samples up to two times during pregnancy (n = 866 total samples). We computed the intraclass correlation coefficient (ICC) to evaluate variability in concentrations between collections and used generalized estimating equation (GEE) models to assess predictors of exposure. Geometric mean (GSD) BPA concentrations were 0.9 (2.8) μg/L and 1.0 (2.6) μg/L at the first and second prenatal visits, respectively. We observed greater within- than between-woman variability in urinary BPA concentrations (ICC = 0.22). GEE models suggest that women who lived in the United States their entire life had 38% (CI: − 0.1, 89.3) higher urinary BPA concentrations compared with other immigrant women. Additionally, women who consumed ≥ 3 sodas per day or hamburgers three times a week or more had 58% (CI: 18.0, 112.1) and 20% (CI: − 0.2, 45.2) higher urinary BPA concentrations, respectively, compared with women who consumed no sodas or hamburgers. A higher percentage of women who lived their entire life in the United States reported increased consumption of sodas and hamburgers compared with other immigrant women. Independent of other factors, BPA urinary concentrations were slightly higher when the sample was collected later in the day. As in previous studies, high within-woman variability in urinary BPA concentrations confirms that several samples are needed to properly characterize exposure during pregnancy. Results also suggest that some factors could be modified to minimize exposures during pregnancy in our study participants (e.g., reducing soda and hamburger intake) and that factors associated with acculturation might increase BPA concentrations.     

Regional geology and radon variability in buildings

Radon concentrations in dwellings vary by more than two orders of magnitude. Predicting where and when concentrations are likely to be high requires studying the variability of the contributors to radon in buildings. Among common sources, geological factors (water supply and substrate) are the most variable, whereas building materials are much less variable. Ventillation variation among houses is generally responsible for radon variations comparable to those introduced by building materials, but it is more significant at lower ventilation rates. In some regions with relatively high proportions of houses with elevated radon concentrations, mappable geological factors are associated with most cases of high radon concentrations. However, a priori identification of rock types likely to be implicated is likely to be successful in only a few cases.     

Metal uptake, transport and release by wetland plants: implications for phytoremediation and restoration

Marshes have been proposed as sites for phytoremediation of metals. The fate of metals within plant tissues is a critical issue for effectiveness of this process. In this paper we review studies that investigate the effects of plants on metals in wetlands. While most of these marsh plant species are similar in metal uptake patterns and in concentrating metals primarily in roots, some species retain more of their metal burden in below ground structures than other species, which redistribute a greater proportion of metals into above ground tissues, especially leaves. Storage in roots is most beneficial for phytostabilization of the metal contaminants, which are least available when concentrated below ground. Plants may alter the speciation of metals and may also suffer toxic effects as a result of accumulating them. Metals in leaves may be excreted through salt glands and thereby returned to the marsh environment. Metal concentrations of leaf and stem litter may become enriched in metals over time, due in part to cation adsorption or to incorporation of fine particles with adsorbed metals. Several studies suggest that metals in litter are available to deposit feeders and, thus, can enter estuarine food webs. Marshes, therefore, can be sources and well as sinks for metal contaminants. Phragmites australis, an invasive species in the northeast U.S. sequesters more metals below ground than the native Spartina alterniflora, which also releases more via leaf excretion. This information is important for the siting and use of wetlands for phytoremediation as well as for marsh restoration efforts.     

Australian firefighters' exposure to air toxics during bushfire burns of autumn 2005 and 2006

Bushfire fighting is a hazardous occupation and control strategies are generally in place to minimize the hazards. However, little is known regarding firefighters' exposure to bushfire smoke, which is a complex mixture of toxic gases and particles. In Australia, during the prescribed burning season, firefighters are likely to be exposed on a regular basis to bushfire smoke, but whether these exposures affect health has yet to be determined. There are a number of factors that govern whether exposure to smoke will result in short-term and/or long-term health problems, including the concentrations of air pollutants within the breathing zone of the firefighter, the exposure duration, and health susceptibility of the individual, especially for pre-existing lung or heart disease. This paper presents measurements of firefighters' personal exposure to bushfire smoke, the first step within a risk management framework. It provides crucial information on the magnitude, extent and frequency of personal exposure to bushfire smoke for a range of typical scenarios. It is found that the primary air toxics of concern are carbon monoxide (CO), respirable particles and formaldehyde. Also, work activity is a major factor influencing exposure with exposure standards (both average and short-term limits) likely to be exceeded for activities such as suppression of spot fires, holding the fireline, and patrolling at the edge of a burn area in the urban-rural interface.