Different "nongrain" activities affect the accumulation of heavy metals and their source-oriented health risks on cultivated lands.

"Nongrain" production on cultivated land is one of the primary environmental issues in China. Different "nongrain" activities may introduce different pollution sources to the local environment, leading to variations in heavy metal contents in soil, which can profoundly impact national food security. In this study, three typical "nongrain" regions (Nanxun (NX), Xiaoshan (XS) and Lin'an (LA)) with intensive aquaculture, tea planting and flower (seedling) growth on cultivated land around the Hangzhou metropolitan area were selected to address the spatial heterogeneity of accumulation levels, sources and source-oriented health risks of heavy metals in soil. The results showed that Hg was the main pollutant in NX and XS, while Cd and As were the major contaminants in LA. Aquiculture and sericultural industries (37.43%), natural sources (23.59%) and industrial activities (38.99%) were the major sources in NX; atmospheric deposition (37.73%), flower and seedling planting (23.49%) and metal-related industries (35.16%) were the major sources in XS; and atmospheric deposition (28.06%), excessive application of fertilizers and pesticides during tea planting (43.47%) and natural sources (28.47%) were the major sources in LA. The major risk population, area, exposure route and hazardous elements were children, LA, ingestion and As and Cr, respectively. From the perspective of source-based health risk assessment, in addition to natural sources that are difficult to intervene in, industrial activities, especially leather and wood process industries, metal-related industries and excessive fertilizer and pesticide application during tea planting contributed the most to the total health risk, which explained 67%, 41% and 42%, respectively, of the total risk in NX, XS and LA. High health risks are present in sources with heavy loadings of hazardous heavy metals (As and Cr); thus, to protect human health, the corresponding high-risk anthropogenic pollution sources in different "nongrain" areas need to be controlled.

Quantitative heterogeneous source apportionment of toxic metals through a hybrid method in spatial random fields.

Toxic metals in soils pose hazards to food security and human health. Accurate source apportionment provides foundation for pollution prevention. In this study, a novel hybrid method that combines positive matrix factorization, Bayesian maximum entropy and integrative predictability criterion is proposed to provide a new perspective for exploring the heterogeneity of pollution sources in spatial random fields. The results suggest that Cd, As and Cu are the predominant pollutants, with exceedance rates of 27%, 12% and 11%, respectively. The new method demonstrates superiority in predicting toxic metals when combined major and all sources as auxiliary information., with the improvements of 44% and 46%, respectively, Although the major sources identified with the hybrid method are the primary contributors to the accumulation of toxic metals (e.g. coal combustion for Hg, traffic emission for Pb and Zn, industrial activities for As, agricultural activities for Cd and Cu and natural sources for Cr and Ni), the impact of nonmajor sources on toxic metal sin specific regions should not be ignored (e.g. industrial activities on Ni, Pb and Zn in the north and natural sources on Cd, Cu, As, Pb and Zn in the south). For better pollution control, specific local sources should be considered.

Processing toxic metal source proxies appropriately for better spatial heterogeneity source apportionment.

Soil toxic metals have strong spatial heterogeneity, and their sources vary among regions. Thus, this study integrated the Catreg and geographically weighted regression (GWR) models to quantitatively extract the main source proxies (numerical and categorical variables were analyzed simultaneously) for different toxic metals and analyze the spatial heterogeneity of the distributions of these sources. Pb, Cd and Hg were the predominant toxic metals in soil. Of the samples with Pb, Cd and Hg, 84.12 %, 68.03 % and 41.57 % exceeded the background values, and 5.36 %, 6.42 % and 5.43 % were moderately contaminated according to the geoaccmulation index, respectively. Industrial activities, with relative importance values of 17.82 %, 31.54 % and 26.51 % for Cd, Hg and Pb, respectively, were the predominant source of these metals especially, in their high-content cluster areas (central urban areas). Soil available phosphorus was another important factor (relative importance values of 13.03 %, 13.41 % and 25.55 % for Cd, Hg and Pb, respectively), and agricultural activities (especially the overuse of phosphoric fertilizers) were identified as an anthropogenic source of these toxic metals. Soil parent material had the greatest influence on As and Cr, with relative importance values of 19.88 % and 19.09 %, respectively, especially in their high-content accumulation area (the eastern coastal area), indicating that these toxic metals mainly come from natural sources. Slope had important impacts on toxic metal accumulation (relative importance values of 17.48 %, 21.22 %, 12.40 % and 16.13 % for Cd, Hg, Cr and As, respectively) by influencing industrial distribution and pollutant migration. By changing the soil adsorption capacity, soil organic matter (explaining 13.01 % of Pb) and soil pH (explaining 14.58 % of As and 12.40 % of Cr) strongly influenced toxic metal accumulation. This study highlights the benefits of the integrated Catreg-GWR model for analyzing multiple spatially heterogeneous environmental data types (numerical and categorical variables), providing a potential foundation for local pollution prevention.

Pollution threshold assessment and risk area delineation of heavy metals in soils through the finite mixture distribution model and Bayesian maximum entropy theory.

Pollution threshold and high-risk area determination for heavy metals is important for effectively developing pollution control strategies. Based on heavy metal contents in 3627 dense samples, an integrated framework combining the finite mixture distribution model and Bayesian maximum entropy (BME) theory was proposed to assess pollution thresholds, contamination levels and risk areas in an uncertain environment for soil heavy metals. The results showed that the average heavy metal contents were in the order Zn > Cr > Pb > Cu > Ni > As > Cd > Hg, with strong/moderate variation, and the corresponding pollution thresholds were 158.39, 84.29, 47.84, 49.75, 28.95, 18.01, 0.49 and 0.16 mg/kg, respectively. The thresholds were consistently greater than the Zhejiang Province backgrounds but lower than the national risk screening values, except for Cd. Approximately 27.9% of the samples were classified as contaminated at various levels, and they were distributed in the northern, northwestern and eastern regions of the study area. Additionally, 3.73%, 5.34% and 8.22% of the total area were classified as at-risk areas under confidence levels of 95%, 90% and 75%, respectively, through BME theory. The findings provide a reasonable classification system and suggestions for heavy metal pollution management and control.

Predicting isoscapes based on an environmental similarity model for the geographical origin of Chinese rice.

The authentication of geographical origin of food is important using stable isotope analysis. However, the isotopic databank is still short of comprehensive. The isoscapes model based on environmental similarity is used for the first time to predict the geospatial distribution of δ13C, δ2H and δ18O in Chinese rice in 2017 and 2018. 794 rice samples in 2017 were used to build isoscapes model. Independent verification shows that the predicted isotope distribution from this new approach is of high accuracy, with a root mean square error (RMSE) of 0.51 ‰, 7.09 ‰ and 2.06 ‰ for δ13C, δ2H and δ18O values for 2017, respectively. Our results indicate that it is possible to predict the spatial distribution of stable isotopes in rice using an isoscapes model based on environmental similarity. This novel strategy can enrich and complement a stable isotope reference database for rice origin identification at regional scale.

Contamination assessment and source apportionment of heavy metals in agricultural soil through the synthesis of PMF and GeogDetector models.

Heavy metal pollution in soils has attracted great attention worldwide in recent decades. Selecting Hangzhou as a case study location, this research proposed the synthesis application of positive matrix factorization (PMF) and GeogDetector models for quantitative analysis of pollution sources, which is the basis for subsequent soil pollution prevention and remediation. In total, 2150 surface soil samples were collected across the study area. Although the mean concentrations of As, Cd, Cr, Hg, and Pb in the soils were lower than the National Environmental Quality Standards for Soils in China, the mean contents of As and Cd were higher than their corresponding local background values by approximately 1.31 and 1.59 times, respectively, indicating that heavy metals have been enriched in topsoil. Agricultural activities, industrial activities, and soil parent materials were the main sources of heavy metal pollution in the soils, accounting for 63.4%, 19.8%, and 16.8% of the total heavy metal accumulation, respectively. Cr was derived mainly from soil parent materials (80.72%). Cd was closely associated with agricultural activities (73.68%), such as sewage irrigation and application of fertilizer. Mercury was mainly attributed to industrial activities (92.38%), such as coal mining and smelting. As was related to agricultural (57.83%) and natural (35.56%) sources, and Pb was associated with industrial (42.42%) and natural (41.83%) sources. The new synthesis models are useful for estimating the source apportionment of heavy metals in soils.

Improved heavy metal mapping and pollution source apportionment in Shanghai City soils using auxiliary information.

Soil heavy metal pollution can be a serious threat to human health and the environment. The accurate mapping of the spatial distribution of soil heavy metal pollutant concentrations enables the detection of high pollution areas and facilitates pollution source apportionment and control. To make full use of auxiliary soil properties information and show that they can improve mapping, a synthesis of the Bayesian Maximum Entropy (BME) theory and the Geographically Weighted Regression (GWR) model is proposed and implemented in the study of the Shanghai City soils (China). The results showed that, compared to traditional techniques, the proposed BME-GWR synthesis has certain important advantages: (a) it integrates heavy metal measurements and auxiliary information on a sound theoretical basis, and (b) it performs better in terms of both prediction accuracy and implementation flexibility (including the assimilation of multiple data sources). Based on the heavy metal concentration maps generated by BME-GWR, we found that the As, Cr and Pb concentration levels are high in the eastern part of Shanghai, whereas high Cd concentration levels were observed in the northwestern part of the city. Organic carbon and pH were significantly correlated with most of the heavy metals in Shanghai soils. We concluded that Cd pollution is mainly the result of agricultural activities, and that the Cr pollution is attributed to natural sources, whereas Pb and As have compound pollution sources. Future studies should investigate the implementation of BME-GWR in the case of space-time heavy metal mapping and its ability to integrate human activity information and soil category variables.

The association between heavy metal soil pollution and stomach cancer: a case study in Hangzhou City, China.

Stomach cancer (SC) is a severe health burden, with nearly half of the world's cases found in China. Noticeably, the emissions of heavy metals into the environment have increased alongside rapid urbanization and industrialization in China. However, as regards carcinogenic associations, the relationship between heavy metals and SC is yet unclear. Based on 9378 newly diagnosed SC cases in Hangzhou City from 2009 to 2012, this work is concerned with the quantitative characterization of the spatial distribution pattern of SC incidence and its geographical association with soil heavy metals by means of a novel geographical model. The results show that (a) Cd is one of the severe soil pollutants in Hangzhou; (b) higher SC incidence clusters are in central Hangzhou, whereas lower clusters are found in the northeast and southwest with a male to female incidence ratio about 2.2:1; (c) although when considered separately, the heavy metals in this work do not have a considerable impact on the distribution of SC incidence in Hangzhou City, nevertheless, the joint effects of multiple heavy metals have significant impacts on SC risk. The present work calls for a rigorous quantitative assessment of the integrated heavy metal soil pollution and its effects on SC incidence.

Soil organic carbon of an intensively reclaimed region in China: Current status and carbon sequestration potential.

Land reclamation has been highly intensive in China, resulting in a large amount of soil organic carbon (SOC) loss to the atmosphere. Evaluating the factors which drive SOC dynamics and carbon sequestration potential in reclaimed land is critical for improving soil fertility and mitigating global warming. This study aims to determine the current status and factors important to the SOC density in a typical reclaimed land located in Eastern China, where land reclamation has been undergoing for centuries. A total of 4746 topsoil samples were collected from 2007 to 2010. The SOC density of the reclaimed land (3.18±0.05kgCm(-2); mean±standard error) is significantly lower than that of the adjacent non-reclaimed land (5.71±0.04kgCm(-2)) (p<0.05). A Random Forest model is developed and it captures the relationships between the SOC density and the environmental/anthropogenic factors (R(2)=0.59). The soil pH, land use, and elevation are the most important factors for determining SOC dynamics. In contrast, the effect of the reclamation age on the SOC density is negligible, where SOC content in the land reclaimed during years 1047-1724 is as low as that reclaimed during years 1945-2004. The scenario analysis results indicate that the carbon sequestration potential of the reclaimed lands may achieve a maximum of 5.80±1.81kgCO2m(-2) (mean±SD) when dryland is converted to flooded land with vegetable-rice cropping system and soil pH of ~5.9. Note that in some scenarios the methane emission substantially offsets the carbon sequestration potential, especially for continuous rice cropping system. With the optimal setting for carbon sequestration, it is estimated that the dryland reclaimed in the last 50years in China is able to sequester 0.12milliontons CO2 equivalent per year.