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相对湿度对铁锰氧化物表面甲基对硫磷降解行为的影响OA

Effect of relative humidity on the degradation behavior of methyl parathion on the surface of iron-manganese oxides

中文摘要英文摘要

土壤中有机磷农药的污染问题引起了广泛的关注,探索有机磷农药在土壤铁锰氧化物表面的环境行为对厘清该类污染物在环境中的归宿至关重要.研究了水分有限条件下7种不同晶型铁、锰氧化物对甲基对硫磷的降解行为.结果表明,甲基对硫磷在铁氧化物和铁锰氧化物表面主要发生水解反应,锰氧化物表面同时发生水解和氧化反应.相对湿度在 33%~76%时,铁氧化物对甲基对硫磷的水解速率最高(1.37×10-2 h-1);锰氧化物对甲基对硫磷降解的速率(Kobs)与相对湿度之间呈现明显的负相关,相对湿度从5%升至100%时,Kobs 值从0.66 h-1 下降至0.31 h-1.此外,α-MnO2 对甲基对硫磷降解的速率(0.276 h-1·m-2)比针铁矿(0.010 6 h-1·m-2)和铁锰氧化物(0.004 03 h-1·m-2)高2~3个数量级.铁氧化物和锰氧化物表面羟基和 Lewis 酸位点共同控制甲基对硫磷的水解行为;然而,铁锰氧化物对甲基对硫磷的水解仅受表面Lewis酸位点影响.本研究的结果强调水分有限条件下铁、锰氧化物对有机磷农药降解行为的影响,也揭示了该类污染物在土壤环境中可能被长期忽略的非生物转化行为.

The pollution of soil by organophosphorus pesticides(OPPs)has attracted widespread attention from researchers.Exploring the environmental behaviors of OPPs on the surface of soil iron-manganese oxides is crucial for clarifying the environmental fate of such pollutants.The degradation behaviors of methyl parathion(MP)by seven iron and manganese oxides with different crystal forms were investigated under limited moisture conditions.Results showed that MP mainly underwent hydrolysis on the surface of iron oxides and iron-manganese oxides,while both hydrolysis and oxidation reactions occurred simultaneously on the surface of manganese oxides.When the relative humidity(RH)was in the range of 33%-76%,the hydrolysis rate of MP by iron oxides reached the maximum(1.37×10-2 h-1).For manganese oxides,there was a significant negative correlation between the observed degradation rate(Kobs)of MP and RH.As RH increased from 5%to 100%,the Kobs value decreased from 0.66 h-1 to 0.31 h-1.In addition,the degradation rate of MP by α-MnO2(0.276 h-1·m-2)was 2~3 orders of magnitude higher than that of goethite(0.010 6 h-1·m-2)and iron-manganese oxides(0.004 03 h-1·m-2).The hydrolysis of MP by iron oxides and manganese oxides was jointly controlled by surface hydroxyl groups and Lewis acid sites,while the hydrolysis by the iron-manganese oxide was governed exclusively by the surface Lewis acid sites.The findings of this study underscore the impact of limited moisture conditions on the catalytic transformation of OPPs by iron and manganese oxides,and also reveal the likely long-overlooked abiotic transformation behavior of such pollutants in the soil environment.

彭美淋;雷蒙;郑菲;胡立嵩;董万强;廖小平

武汉工程大学化学与环境工程学院,湖北 武汉 430205武汉工程大学化学与环境工程学院,湖北 武汉 430205武汉工程大学化学与环境工程学院,湖北 武汉 430205武汉工程大学化学与环境工程学院,湖北 武汉 430205武汉工程大学化学与环境工程学院,湖北 武汉 430205||磷矿及其共伴生资源绿色高效开发利用全国重点实验室,湖北 武汉 430205武汉工程大学化学与环境工程学院,湖北 武汉 430205

资源环境

铁锰氧化物甲基对硫磷相对湿度降解行为

iron manganese oxidemethyl parathionrelative humiditydegradation behavior

《武汉工程大学学报》 2026 (3)

253-260,8

国家自然科学基金(41702267)武汉工程大学科学基金(K201935)武汉工程大学研究生教育创新基金(CX2022423)

10.19843/j.cnki.CN42-1779/TQ.202510005

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