生物炭对稻田土壤镉生物有效性的影响研究
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摘要
在我国有效耕地面积日益缩小,重金属污染土壤面积却逐年扩大的严峻形势下,为明确生物炭治理镉污染土壤的应用价值,以生物炭理化性质分析与镉吸附-解吸动力学行为研究为基础,通过在镉污染稻田土壤上开展秸秆直接粉碎和炭化两种还田方式的比较研究,探讨了生物炭施入后对土壤镉赋存形态的影响及其相互关系,系统分析了生物炭结合土壤因子对镉胁迫条件下水稻生理、生化性状及镉吸收、分配、转运和积累的影响,以及不同还田方式与水稻品质及糙米镉含量的相互关系,以期为改良与修复重金属镉污染稻区土壤,消减农产品中可食用部位镉残留,并有效防止污染面继续扩散提供理论依据,研究结果表明：
1.不同最高热解温度(HTT)生物炭理化性质分析结果表明,随着HTT升高,生物炭产率从60%降低到34%,灰分含量从12%升高到33%,挥发分下降到原材料稻壳的四分之一,在HTT400℃之前pH值急剧增大,上升至9以后开始放缓。HTT达到500℃时,生物炭的阳离子交换量、比表面积显著提高,较原材料增幅分别达到41%和85%。微观外表面结构逐渐清晰、规则,疏松多孔的结构增多,以上变化有助于提高生物炭的吸附能力。
2.根据不同HTT生物炭对镉的吸附-解吸动力学行为特征差异及平衡时最大吸附、固持量与生物炭理化性质的关联分析,初步构建了适于生物炭的动力学拟合模型。结果表明：(1)稻壳和3种不同HTT条件下制成的生物炭的吸附量均随着初始镉离子浓度的升高而增加,HTT500℃在0.5mg/L镉溶液浓度的吸附效果最好,达到99.55%,并且随着HTT的升高,生物炭在增加了吸附量同时也相对缩短了吸附进程；(2)解吸过程中,吸附态镉离子的解吸量随振荡时间的延长而不断增加,高热解温度制备的生物炭最快到达解吸平衡,与Elovich方程拟合度最好；(3)能谱分析证实了生物炭对重金属镉离子存在吸附、固持作用,同时随HTT的升高,生物炭对镉离子的固持量增大,相对原子数量百分比值较原材料增幅达到3.4%；(4)通过相关分析表明生物炭酸碱度、阳离子交换量和比表面积对其固持镉离子能力有显著的正向作用。
3.对生物炭施入土壤后镉赋存形态的分析结果表明,随着施炭量的增加金属可交换态镉所占土壤总镉含量比例出现减少趋势,各处理分别较CK降低3%、8%和11%。其它四种形态镉都不同程度的增加,其中毒性最小的残渣晶格结合态镉含量较对照提高了4到5个百分点。对土壤理化性质与有效态镉进行线性回归分析,pH值、电导率和阳离子交换量与有效态镉含量均呈显著负相关趋势,表明生物炭施入土壤带来的一系列的变化对降低土壤中有效态镉具有积极作用。
4.随着镉胁迫的增大,水稻剑叶的游离脯氨酸、丙二醛含量呈现增加趋势。在土壤最大镉胁迫浓度下,添加生物炭的C1、C2处理与CK相比游离脯氨酸含量降幅达到24.7%和39.3%；同时丙二醛含量显著低于不施炭对照处理。但超氧化物歧化酶和过氧化氢酶活性呈现先降低后升高趋势,说明如果施炭量过大,保护酶活性继续增强,可能造成了水稻的另一种逆境胁迫,从而使酶活性出现了升高反复。
5.生物炭的施入明显影响镉在水稻不同器官的积累,施炭量最大处理消减镉积累量最大,各器官(叶、茎,鞘、糙米)分别较CK降低21%、19%、26%和19%,均达到显著水平。通过水稻糙米镉积累量与产量性状指标的逐步回归分析得出生物炭的施入可以影响水稻库容量进而降低糙米内镉浓度水平。
6.秸秆炭化还田与直接粉碎还田两种方式对比上年镉污染水稻处理糙米中镉含量都有大幅的降低,秸秆炭化还田降幅为56-60%,而秸秆直接粉碎还田降幅为52-57%,炭化还田消减糙米镉含量效果较优于秸秆直接粉碎还田。
综上所述,生物炭施用于土壤后,不但可以通过抑制镉的运输量来消减水稻镉库器官糙米对镉的积累,还可以通过相对增加水稻籽粒镉库的容量进而使籽粒中镉含量下降。因此,秸秆炭化还田是一项兼顾碳封存与土壤重金属污染治理的双赢技术措施。
The contaminated area of heavy metal has expanded each year in China. In order to define the value of biochar for controlling contaminated soil of cadmium, physical, chemical properties and cadmium adsorption-desorption kinetics behavior of biochar were researched for base, difference of rice straw direct crushing and charring into paddy soil of cadmium were compared, influence of cadmium combined forms and their relationship of biochar combined with soil were investigated, effect of physiological, biochemical traits and cadmium absorption, distribution, transport and accumulation of rice under cadmium stress with different biochar application were analysed, and variation of different returning to field measures on the quality of rice and cadmium content of brown rice were also studied. Be hope to provide a theoretical basis for cutting the cadmium residues in agricultural products, repairing paddy soil with heavy metal cadmium contaminated, preventing the spread of polluted area. The main results are as follow:
1. The chemical properties analysis of different HTT biochar showed that the production rate of biochar was reduced from60%to34%, ash content was increased from12%to33%, volatile down to a quarter of rice husk, pH value was increased rapidly before HTT reaching400℃. When the HTT reached500℃, the CEC and BET surface area were increased significantly; amplification of T-500compared with the raw materials reached41%and85%. Biochar's micro surface structure appeared clearly, ruly and porous structure was increased. Influence of physical and chemical properties in biochar was contributed to increase its adsorption properties.
2. The kinetic fitting model suitable for biochar was built according maximum adsorption, solid retention capacity on balance and correlation analysis between physical and chemical properties of biochar. The main types are as follow:
(1) Desorption of rice husk and biochars at three different pyrolysis temperatures were increased with the rising of initial Cd2+concentration. The adsorption effect of HTT500℃was the most, could reached99.55%in0.5mg/L Cd2+solution, and adsorption also shortened by biochar.(2) Cd2+desorption amount increased with the extension of the oscillation time, desorption of biochar at high pyrolysis temperature reached balance the fastest and was fitted with Elovich equations the best.(3) The energy spectrum analysis of biochar showed that they all had cadmium on the surface after desorbing. At the same time, the cadmium ions fixation of biochar increased with HTT.(4) Correlation analysis also showed that pH, CEC and BET surface area had a positive effect on adsorption-desorption ability of biochar.
3. Analysis of cadmium combined forms in soils with different biochar treatments showed that the amount of exchangeable cadmium reduced3%,8%and11%respectively, although the other forms increased variedly. A significant negative correlation trend was showed on the linear regression analysis of physical and chemical properties with available cadmium in soil. It was found that the biochar application had a positive effect on reducing available cadmium in soil.
4. Free proline and MDA content of rice flag leaf showed varying degrees of increase with the soil cadmium concentration rising. In biochar treatments, free proline content of C1and C2lower than that of CK relatively, and this effect was amplified by biochar application rate. Contents of SOD and POD down first and then increased, indicated that high biochar application ratio might cause another kind of stress and suppress the positive function on cadmium amelioration.
5. The effect of cadmium accumulation was significantly in different organs of rice by biochar application. The cadmium accumulation of various organs (leaves, stems, sheath, brown rice) in different biochar application decreased by21%,19%,26%and19%compared with CK. Stepwise regression analysis of yield traits indicators and cadmium accumulation in brown rice showed that the biochar could affect the storage of the rice grain for reducing cadmium accumulation of brown rice.
6. Cadmium content of brown rice with two ways of returning,(rice straw charring and crushing directly to field) had reduced significantly. The reductions were56-60%or52-57%for rice straw charring and crushing directly to field. The reduction of cadmium content in brown rice by straw charring to field was better than straw crushing directly to field.
In summary, biochar could not only reduce the cadmium accumulation of brown rice by controlling the transport of cadmium, but also decreased cadmium content by increasing the storage of the rice grain. Therefore, it is a win-win measure to managing the heavy metal pollution of soil management and carbon sequestration.
1.不同最高热解温度(HTT)生物炭理化性质分析结果表明,随着HTT升高,生物炭产率从60%降低到34%,灰分含量从12%升高到33%,挥发分下降到原材料稻壳的四分之一,在HTT400℃之前pH值急剧增大,上升至9以后开始放缓。HTT达到500℃时,生物炭的阳离子交换量、比表面积显著提高,较原材料增幅分别达到41%和85%。微观外表面结构逐渐清晰、规则,疏松多孔的结构增多,以上变化有助于提高生物炭的吸附能力。
2.根据不同HTT生物炭对镉的吸附-解吸动力学行为特征差异及平衡时最大吸附、固持量与生物炭理化性质的关联分析,初步构建了适于生物炭的动力学拟合模型。结果表明：(1)稻壳和3种不同HTT条件下制成的生物炭的吸附量均随着初始镉离子浓度的升高而增加,HTT500℃在0.5mg/L镉溶液浓度的吸附效果最好,达到99.55%,并且随着HTT的升高,生物炭在增加了吸附量同时也相对缩短了吸附进程；(2)解吸过程中,吸附态镉离子的解吸量随振荡时间的延长而不断增加,高热解温度制备的生物炭最快到达解吸平衡,与Elovich方程拟合度最好；(3)能谱分析证实了生物炭对重金属镉离子存在吸附、固持作用,同时随HTT的升高,生物炭对镉离子的固持量增大,相对原子数量百分比值较原材料增幅达到3.4%；(4)通过相关分析表明生物炭酸碱度、阳离子交换量和比表面积对其固持镉离子能力有显著的正向作用。
3.对生物炭施入土壤后镉赋存形态的分析结果表明,随着施炭量的增加金属可交换态镉所占土壤总镉含量比例出现减少趋势,各处理分别较CK降低3%、8%和11%。其它四种形态镉都不同程度的增加,其中毒性最小的残渣晶格结合态镉含量较对照提高了4到5个百分点。对土壤理化性质与有效态镉进行线性回归分析,pH值、电导率和阳离子交换量与有效态镉含量均呈显著负相关趋势,表明生物炭施入土壤带来的一系列的变化对降低土壤中有效态镉具有积极作用。
4.随着镉胁迫的增大,水稻剑叶的游离脯氨酸、丙二醛含量呈现增加趋势。在土壤最大镉胁迫浓度下,添加生物炭的C1、C2处理与CK相比游离脯氨酸含量降幅达到24.7%和39.3%；同时丙二醛含量显著低于不施炭对照处理。但超氧化物歧化酶和过氧化氢酶活性呈现先降低后升高趋势,说明如果施炭量过大,保护酶活性继续增强,可能造成了水稻的另一种逆境胁迫,从而使酶活性出现了升高反复。
5.生物炭的施入明显影响镉在水稻不同器官的积累,施炭量最大处理消减镉积累量最大,各器官(叶、茎,鞘、糙米)分别较CK降低21%、19%、26%和19%,均达到显著水平。通过水稻糙米镉积累量与产量性状指标的逐步回归分析得出生物炭的施入可以影响水稻库容量进而降低糙米内镉浓度水平。
6.秸秆炭化还田与直接粉碎还田两种方式对比上年镉污染水稻处理糙米中镉含量都有大幅的降低,秸秆炭化还田降幅为56-60%,而秸秆直接粉碎还田降幅为52-57%,炭化还田消减糙米镉含量效果较优于秸秆直接粉碎还田。
综上所述,生物炭施用于土壤后,不但可以通过抑制镉的运输量来消减水稻镉库器官糙米对镉的积累,还可以通过相对增加水稻籽粒镉库的容量进而使籽粒中镉含量下降。因此,秸秆炭化还田是一项兼顾碳封存与土壤重金属污染治理的双赢技术措施。
The contaminated area of heavy metal has expanded each year in China. In order to define the value of biochar for controlling contaminated soil of cadmium, physical, chemical properties and cadmium adsorption-desorption kinetics behavior of biochar were researched for base, difference of rice straw direct crushing and charring into paddy soil of cadmium were compared, influence of cadmium combined forms and their relationship of biochar combined with soil were investigated, effect of physiological, biochemical traits and cadmium absorption, distribution, transport and accumulation of rice under cadmium stress with different biochar application were analysed, and variation of different returning to field measures on the quality of rice and cadmium content of brown rice were also studied. Be hope to provide a theoretical basis for cutting the cadmium residues in agricultural products, repairing paddy soil with heavy metal cadmium contaminated, preventing the spread of polluted area. The main results are as follow:
1. The chemical properties analysis of different HTT biochar showed that the production rate of biochar was reduced from60%to34%, ash content was increased from12%to33%, volatile down to a quarter of rice husk, pH value was increased rapidly before HTT reaching400℃. When the HTT reached500℃, the CEC and BET surface area were increased significantly; amplification of T-500compared with the raw materials reached41%and85%. Biochar's micro surface structure appeared clearly, ruly and porous structure was increased. Influence of physical and chemical properties in biochar was contributed to increase its adsorption properties.
2. The kinetic fitting model suitable for biochar was built according maximum adsorption, solid retention capacity on balance and correlation analysis between physical and chemical properties of biochar. The main types are as follow:
(1) Desorption of rice husk and biochars at three different pyrolysis temperatures were increased with the rising of initial Cd2+concentration. The adsorption effect of HTT500℃was the most, could reached99.55%in0.5mg/L Cd2+solution, and adsorption also shortened by biochar.(2) Cd2+desorption amount increased with the extension of the oscillation time, desorption of biochar at high pyrolysis temperature reached balance the fastest and was fitted with Elovich equations the best.(3) The energy spectrum analysis of biochar showed that they all had cadmium on the surface after desorbing. At the same time, the cadmium ions fixation of biochar increased with HTT.(4) Correlation analysis also showed that pH, CEC and BET surface area had a positive effect on adsorption-desorption ability of biochar.
3. Analysis of cadmium combined forms in soils with different biochar treatments showed that the amount of exchangeable cadmium reduced3%,8%and11%respectively, although the other forms increased variedly. A significant negative correlation trend was showed on the linear regression analysis of physical and chemical properties with available cadmium in soil. It was found that the biochar application had a positive effect on reducing available cadmium in soil.
4. Free proline and MDA content of rice flag leaf showed varying degrees of increase with the soil cadmium concentration rising. In biochar treatments, free proline content of C1and C2lower than that of CK relatively, and this effect was amplified by biochar application rate. Contents of SOD and POD down first and then increased, indicated that high biochar application ratio might cause another kind of stress and suppress the positive function on cadmium amelioration.
5. The effect of cadmium accumulation was significantly in different organs of rice by biochar application. The cadmium accumulation of various organs (leaves, stems, sheath, brown rice) in different biochar application decreased by21%,19%,26%and19%compared with CK. Stepwise regression analysis of yield traits indicators and cadmium accumulation in brown rice showed that the biochar could affect the storage of the rice grain for reducing cadmium accumulation of brown rice.
6. Cadmium content of brown rice with two ways of returning,(rice straw charring and crushing directly to field) had reduced significantly. The reductions were56-60%or52-57%for rice straw charring and crushing directly to field. The reduction of cadmium content in brown rice by straw charring to field was better than straw crushing directly to field.
In summary, biochar could not only reduce the cadmium accumulation of brown rice by controlling the transport of cadmium, but also decreased cadmium content by increasing the storage of the rice grain. Therefore, it is a win-win measure to managing the heavy metal pollution of soil management and carbon sequestration.
引文
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