Policies on the management of paddy fields are usually made at a broad scale and from a long-term perspective, while predicting the spatial extent of cadmium (Cd) contamination in paddy soils remains challenging. In this study, we developed a process-driven spatial model to quantify the transport of Cd in paddy soils and validated it against observed data from a 10-year regional investigation in southern China. Using a geographic information system and Monte Carlo simulation, the model was then applied to evaluate the effectiveness of different remediation strategies for contaminated paddy fields at field-to-regional scales in a 100-year period. In the last decade, atmospheric emissions have accounted for 43.5 % of the total Cd input in local paddy soils. However, the local clean air act failed to mitigate Cd contamination in 99.8 % of study area over the period of 2020-2120 because straw return became the dominant contributor to Cd inputs. Improving aerosol emission reductions by 3 % per year, stopping straw return to soil, and cleaning irrigation channels would take approximately 30 years (2020-2050) to protect 95 % of local rice production from causing an excessive human Cd kidney burden, especially in the paddy fields located in mining-affected areas.

Cadmium (Cd) exposure risks to consumers of locally grown rice are often estimated without considering the sources and bioavailability of Cd. Here, we present the first comprehensive and quantitative analysis on the sources and transport of Cd in paddy ecosystems by combining a regional investigation in southern China, a positive matrix factorization algorithm, and a classification and regression tree approach. Results showed that local atmospheric emission regulations failed to mitigate Cd contamination as the Cd inputs from industrial effluent irrigation were largely overlooked. Leaching loss of soil Mn is an invisible threat to grain safety as Mn can exhibit a significant facilitation effect on rice Cd uptake under acidic pH. A probability-based toxicokinetic model is proposed to optimize the strategies for minimizing the Cd body burden through the source-soil-rice -human pathway. Urinary Cd exceeded its safety threshold in 61.7 % of local female adults (6.14 +/- 4.42 mu g g(-1) creatinine) who consumed less rice grain but with a low Zn bioavailability. To protect 85 % of local rice production from causing excessive Cd exposure risk, irrigation channel needs to be effectively cleaned up, and the pH and amorphous Mn content of rice soils need to be raised to 5.50 and 179 mg kg(-1), respectively.

High concentrations of potentially toxic elements (PTEs) in tobacco leaves are possible from the soil contamination and would have adverse health risks on residents. A large-scale survey of 306 tobacco fields in southern China was conducted to investigate the accumulation of PTEs in tobacco leaves through the soil-tobacco-human pathway and the associated health risks for local smokers and passive smokers. Significant enrichment of As, Cd, Hg, and Pb was observed in the investigated tobacco fields, with industrial emissions and applied fertilizers as the major potential sources. Dynamic interactions between factors in the soil acidic labile pool showed site-specific effects on the uptake of PTEs by tobacco plants. It was 99.6% and 91.8% probable that exposure of local adult men smokers to Cd and As exceeded the permitted safety limits, respectively. The population of men smokers had a 20-fold higher Cd exposure risk than did passive smokers. A probability-based transfer model was developed to demonstrate that interactions between soil factors could affect the Cd exposure risk of men smokers of locally harvested tobacco. Optimizing the pH (>6.0) and organic matter content (>40 g kg-1) of tobacco-growing soils, and setting a safe tobacco consumption rate of 2.80 g dry weight per day would help protect 90.4% of men smokers from excessive risks of exposure to Cd.

When rice soils are contaminated by cadmium (Cd), the sources and timing of such contaminations need to be identified. In this study, we aimed to quantify the sources, history, and fate of Cd in the rice soils of southern China, by combining a near 10-year regional investigation, by developing a normalized positive matrix factorization algorithm, a Cd mass balance model, and probabilistic simulation. We simulated the historical contamination process of Cd in rice soils from 1991 to 2019 and the future changes from 2019 to 2069 under varying input parameters, as affected by different environmental management measures. Over the period of 1991-2019, the input flux of Cd through atmospheric deposition was estimated at 421 g ha-1, which contributed 52.1% of the total increments in soil Cd concentration. Over the next decade, a 25.6% probability is predicted that the Cd concentration of local rice soils would increase from the baseline to the upper level of soil threshold, despite the efforts of environmental regulators. Removing the rice straw from production fields, cleaning up the irrigation channels, and strengthening environmental regulations would take approximately 50 years (2019-2069) to ensure that 90% of soils were safe for rice cultivation.

The present study evaluates the sustainability of tobacco-rice rotation by reducing the phytoavailability of cadmium (Cd) to rice by combining large-scale field sampling and regional investigations in southern China. The rotation involves frequent tillage and liberal application of nitrogen and phosphorus fertilizers, which increases yields but lowers soil pH. As a result, manganese is lost from soil and, at the same time, more soil Cd is taken up by rice and tobacco. The tendency to overcompensate for the Mn loss is influenced by soil properties, crop type, and economics of cultivation. Based on the scenario analysis, this tendency and the Cd uptake risks were estimated. Dietary intake of 83.3% of rice grain produced on the rotation fields would have adverse health effects on local male nonsmokers. Besides the rice, Cd in local tobacco leaf may lead to an increase in the kidney Cd levels of local male smokers (21.5 cigarettes per day) by 16.2-fold at age 50. Field trials and model estimations indicated that for a Cd concentration below 0.2 mg dry weight kg(-1) in rice grain, the critical pH value in rice soils was similar to 6.0, and that for amorphous Mn oxide at pH 4.5-6.0 was 120 mg kg(-1).

小麦富镉(Cd)问题受到广泛关注,铁氧化物具备降镉潜力.通过盆栽小麦幼苗实验,分析了三氧化二铁(Fe2O3)、氢氧化铁[Fe(OH)3[及拜耳法赤泥(B-RM)3种铁氧化物的降镉能力.结果显示3种铁氧化物中,Fe(OH)3可显著降低小麦幼苗茎叶Cd含量,与对照相比降幅为16.3％～27.7％,投加量为0.5％时降Cd效果最优.Fe(OH)3能够显著降低小麦幼苗根部向茎叶的Cd转运,投加量为10％时富集系数及转运系数最低.小麦幼苗根际土壤Fe/Cd、Cu/Cd及Zn/Cd是影响小麦幼苗茎叶Cd积累的关键因子,当Fe/Cd＞25000、Cu/Cd＞50或Zn/Cd＞100时,根际土壤元素比与茎叶镉含量呈显著负相关.该比值的确定对于大田应用中钝化剂材料投加量的确定具有指导意义.

The simulation analysis of the migration path and soil accumulation trend of Cd in paddy soil systems could contribute to improved scientific and reasonable risk decision-making. In this study, based on a regional survey of environmental media in Youxian County, Hunan Province, a pollutant accumulation model (PAM) was built to predict the cumulative trend of Cd in paddy soils. Combined with Monte Carlo simulation, the PAM model was used to evaluate the effectiveness and sustainability of various remediation measures. Results showed that the probability of Cd accumulation in paddy soils in Youxian County exceeded that of the national soil environmental quality standard by 2-fold and was up to 82.1%, and the average accumulation rate reached 4.28 μg·(kg·a)-1 after 50 years of cultivation under current input pattern. Sensitivity analysis results showed that atmospheric deposition and rice uptake were the key processes affecting Cd accumulation in paddy soils. Results of a multi-scenario simulation showed that the comprehensive measures, such as reducing the straw returning, optimizing the layout of industrial and mining enterprises that reduce the atmospheric deposition of Cd, and cleaning irrigation water, could reduce the Cd accumulation in paddy soils by 43.7% and reduce the probability of light Cd pollution by 80.6% after 50 years, which would be an effective long-term measure to prevent and control Cd pollution risk in paddy soils.

A reliable and accurate soil threshold helps prevent excessive dietary Pb intake risks to consumers of locally grown wheat and rice crops. Based on a three-year investigation of 206 wheat fields and 358 rice fields throughout China, this study aimed to improve the soil protection guidelines by investigating Pb accumulation in soil-wheat and soil-rice systems and by assessing Pb exposure risks through the soil-grain-human pathway. A site-specific bioconcentration factor (BCF, ratio of Pb concentration in plant to that in soil) was calculated and used to assess grain Pb intake risks instead of a generic BCF value to reduce data uncertainty. In addition to soil pH, cation-exchange capacity exerted a major influence on the Pb BCF variations in wheat, whereas the organic carbon dynamics affected the BCF variations in rice. Once normalized BCF against those soil variables, the distributions of BCF were log-normal in nature. Optimizing the pH and cation-exchange capacity of wheat soils would help protect 49.8% of local adults from excessive Pb dietary intake. The scenario soil thresholds linked to soil variables and grain Pb intake risks were then derived and validated by independent data from field surveys and published articles. Poor production practices in the wheat fields under study included using soils with low fertility.

Sources of cadmium (Cd) contamination of farmlands and the potential risk to human health via dietary intake of wheat Cd are of great concern to consumers. A source-specific risk assessment (SSRA) model, which combined a positive matrix factorization receptor model and spatial analysis with a health risk assessment model, was developed based on a wheat field investigation in northern China. It was used to estimate the daily intake risk from different sources of ingesting Cd from wheat. The mixed source of wastewater and residues from industrial activities and atmospheric deposition were identified as the dominant sources of Cd contamination. Wheat Cd uptake could be predicted reliably from the pH and total Cd concentration of field soil. Based on the predictive model of Cd transfer from soil to wheat, the SSRA model then linked sources to the Cd intake risk from wheat grain. Results showed that the mixed source and the atmospheric deposition source accounted for 52.8% and 29.3%, respectively, of the wheat Cd intake risk. In combination with the spatial analysis, the potential risk of Cd contamination in western and central eastern areas was mainly attributed to the mixed source of wastewater and industrial residues, whereas the risk in the northwestern area was associated mainly with atmospheric deposition. Regionalized risk management strategies, focusing on different sources, were proposed to minimize the Cd input to field cropping system and to mitigate health risk for local residents.

我国北方地区小麦镉(Cd)污染形势严峻.土壤锌(Zn)与Cd存在显著的交互作用,但两者关系尚不明确.本研究通过区域调查及大田实验,探究了北方碱性小麦土壤锌镉比(Zn/Cd)与小麦籽粒Cd含量的相关关系.结果 表明,土壤Zn/Cd与小麦籽粒Cd含量显著负相关.施加硫酸锌(增Zn)及深翻耕措施(降Zn)均能显著提高土壤Zn/Cd,并降低小麦籽粒Cd含量.其中,增施100 mg· kg-1的Zn2+,可将土壤Zn/Cd增加61.2％,并使小麦籽粒Cd含量降低9.28％;将土壤0～ 30 cm及30～60 cm土层互换的深翻耕措施,可将土壤Zn/Cd增加45.8％,并使小麦籽粒Cd含量降低13.5％.综合区域调查及大田实验数据,发现当土壤Zn/Cd小于50时,小麦籽粒Cd含量全部超标且有98.4％的样品超标1倍以上;而当土壤Zn/Cd大于100时,小麦籽粒Cd含量超标风险显著降低至11.9％.该阈值的确定对于小麦Cd污染防治具有指导意义.

Limestone shows great potential to reduce the production of cadmium (Cd)-contaminated rice in acidic paddy soils, but has generated uncertainty effects. We conducted batch sorption and greenhouse experiments to investigate optimal conditions of pH and amorphous manganese content (M-nox) in limestone treated-soil for suppressing the Cd uptake by rice plants. The adsorption/desorption behavior of Cd in a soil/limestone mixture was dominated by the composition and density of sorption sites, followed by sorption conditions, which were mainly influenced by soil pH and exchangeable Ca2+. Interactions among soil factors were influenced both by the limestone effects and plant responses. The Cd uptake of rice plants did not matched to the doses of limestone applied. The increase in pH and decrease in M-nox following higher dosages of limestone treatment might produce contradictory effects on rice Cd uptake. We proposed a trade-off model to demonstrate how did the interactions of soil pH and M-nox affect the rice Cd uptake. To minimize the accumulation of Cd in rice grain harvested from acidic paddy soils, limestone was applied at 0.25 % to achieve an optimal pH of 6.5 and a Mnox of 95 mg kg(-1).

Characterizing the interactions between Cd and Zn with respect to the soil soluble Cd and crop Cd uptake allows the development of risk-based approaches to the performance of grain crops. By means of a three-year survey of 358 rice fields and 206 wheat fields across China, this study investigated the effect of Cd-Zn interactions on the phytoavailability of Cd to rice and wheat. The interactive nature between the Cd:Zn ratio and pH of soil affected crop Cd uptake, and the resulting grain Cd intake risk, were examined by the Free-Ion Activity-based model and probability analysis. In highly acidic rice soils (pH < 5.9), soil Zn had no effect on rice Cd uptake, whereas, under near-neutral conditions (pH > 5.9), a site-specific influence of soil Zn on grain Cd concentration was found. Soil Zn could inhibit Cd uptake and translocation by the plant in soil-wheat system when the soil Cd:Zn ratio decreased to 0.0083 and lower. Rice grain poses a significant health risk to local consumers due to its high Cd accumulation and its low Zn accumulation. In order to reduce the health risks from dietary Cd to local consumers, approximately 63.9% of the rice fields and 30.5% of the wheat fields require strategies ameliorating soil acidity in rice soils and increasing Zn concentrations in wheat soils.