光照条件下施加生物质炭的水土界面中活性氧形成行为及影响因素
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1.浙江科技大学环境与资源学院;2.浙江环科环境研究院有限公司

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国家自然科学基金项目(42577019)和浙江省重点研发计划项目(2025C02097)资助


The Behaviors and Influencing Factors of Reactive Oxygen Species Generation at the Soil-Water Interface Containing Biochar Under Simulated Solar Illumination Conditions
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Affiliation:

1.School of Environment and Resources, Zhejiang University of Science and Technology;2.Zhejiang Environmental Science Research Institute Co Ltd

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Supported by the National Natural Science Foundation of China (No. 42577019) and the Key Research and Development Program of Zhejiang Province, China (No. 2025C02097)

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    摘要:

    为探索施用生物质炭的水土界面中活性氧(Reactive oxygen species, ROS)形成规律,在模拟太阳光照条件下,利用化学探针法定量分析了含10 gkg-1生物质炭的水土界面中羟基自由基(?OH)、过氧化氢(H2O2)和超氧阴离子自由基(O2??)三种典型ROS的生成动力学过程及机制,并考察了生物质炭制备温度(300℃、500℃和700℃)、生物质炭溶解性碳(DBC)、黏土矿物(高岭石)和可溶性有机质(富里酸)对水土界面中ROS形成的影响。结果表明:光照条件下,施加生物质炭的水土界面中产生了大量的?OH和H2O2,其浓度范围分别是0.43~0.83 μmolL-1和21.12~30.93 μmolL-1,分别是不含生物质炭水土界面(对照组)的1.39倍~2.65倍和1.31倍~1.91倍;但O2??浓度则较低(< 0.2 μmolL-1),低于对照组。DBC对水土界面中ROS形成具有重要作用,去除DBC之后,含生物质炭的水土界面中H2O2生成受到显著抑制,但?OH的生成不受影响。高岭石能显著抑制光照下生物质炭介导固液界面生成ROS的能力(高温生物质炭除外),并抑制H2O2向?OH的转化效率。富里酸能显著增加光照下含生物质炭水土界面中H2O2的生成能力,但降低了?OH的浓度。光照对含生物质炭水土界面介导ROS形成具有重要作用,它促进含生物质炭水土界面中H2O2的生成与转化,有助于O2??的转化及?OH的生成,但生物质炭介导的水土界面ROS生成不完全依赖于光照。生物质炭表面的持久性自由基、含氧官能团以及水土界面中溶解性有机碳和Fe2+含量共同决定了光照下施加生物质炭水土界面中ROS的形成。本研究结果对认识生物质炭施用土壤中ROS的形成和分布具有重要参考价值。

    Abstract:

    【Objective】Reactive oxygen species (ROS) at the soil-water interface play a crucial role in carbon/nitrogen cycling and pollutant transformation. However, it is still unclear how biochar influences the formation of ROS at the soil-water interface. Thus, this study aims to explore the formation behaviors and factors influencing ROS generation at the soil-water interface containing biochar. 【Method】Under simulated solar illumination conditions, the probe capture method was used to quantitatively analyze the generation kinetics and mechanisms of three typical ROS (hydroxyl radical ?OH, hydrogen peroxide H2O2, and superoxide radical (O2??) at the 10 gkg-1 biochar-amended soil-water interface. The effects of biochar pyrolysis temperature, dissolved biochar carbon (DBC), clay minerals (kaolinite), and dissolved organic matter (fulvic acid) on ROS formation were also examined at such interfaces. 【Result】The results showed that under light, substantial ?OH and H2O2 were generated at the biochar-containing soil-water interface, with concentration ranges of 0.43-0.83 μmolL-1 and 21.12-30.93 μmolL-1, respectively, which were 1.39-2.65 times and 1.31-1.91 times higher than those at the biochar-free interface (control group). In contrast, O2?? concentration was low (< 0.2 μmolL-1), significantly lower than that in the control. DBC played an important role in the formation of ROS, and after removing DBC, the generation of H2O2 in the water-soil interface containing biochar was significantly inhibited, but the generation of ?OH was not affected. Also, kaolinite significantly inhibited the capacity of biochar to mediate ROS generation at the soil-water interface under light (except for high-temperature biochar) and reduced the conversion efficiency of H2O2 to ?OH. Fulvic acid significantly enhanced H2O2 generation at the light-irradiated, biochar-containing soil-water interface but decreased ?OH concentration.【Conclusion】Light plays a critical role in mediating ROS formation at the biochar-amended interface: it not only promotes H2O2 generation and transformation, but also facilitates ?OH production and O2?? conversion. However, biochar-mediated ROS generation at the interface is not entirely dependent on light. The generation of ROS at the light-irradiated, biochar-amended soil-water interface is collectively determined by biochar surface persistent free radicals, oxygen-containing functional groups, as well as dissolved organic carbon and Fe2+ contents at the interface. These findings provide an important reference for understanding the formation and distribution of ROS in biochar-amended soils.

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王浩伟,侯雨橙,姚嘉一,黎梦薇,方婧,单胜道.光照条件下施加生物质炭的水土界面中活性氧形成行为及影响因素[J].土壤学报,DOI:10.11766/trxb202506200296,[待发表]
WANG Haowei, HOU Yucheng, YAO Jiayi, LI Mengwei, FANG Jing, SHAN Shengdao. The Behaviors and Influencing Factors of Reactive Oxygen Species Generation at the Soil-Water Interface Containing Biochar Under Simulated Solar Illumination Conditions[J]. Acta Pedologica Sinica, DOI:10.11766/trxb202506200296,[In Press]

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  • 收稿日期:2025-06-20
  • 最后修改日期:2025-10-09
  • 录用日期:2025-11-04
  • 在线发布日期: 2025-11-10
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