环境科学  2018, Vol. 39 Issue (4): 1926-1933   PDF    
引用本文
赵军超, 王权, 任秀娜, 李荣华, Mukesh Kumar Awasthi, Altaf Hussain Lahori, 张增强. 钙基膨润土辅助对堆肥及土壤Cu、Zn形态转化和白菜吸收的影响[J]. 环境科学, 2018, 39(4): 1926-1933.
ZHAO Jun-chao, WANG Quan, REN Xiu-na, LI Rong-hua, Mukesh Kumar Awasthi, Altaf Hussain Lahori, ZHANG Zeng-qiang. Effect of Ca-bentonite on Cu and Zn Forms in Compost and Soil, and Their Absorption by Chinese Cabbage[J]. Environmental Science, 2018, 39(4): 1926-1933.
钙基膨润土辅助对堆肥及土壤Cu、Zn形态转化和白菜吸收的影响
赵军超, 王权, 任秀娜, 李荣华, Mukesh Kumar Awasthi, Altaf Hussain Lahori, 张增强     
西北农林科技大学资源环境学院, 杨凌 712100
收稿日期: 2017-06-08; 修订日期: 2017-09-22
基金项目: 杨凌示范区产学研用协同创新重大项目（2016CXY-12）
作者简介: 赵军超(1993~), 男, 硕士研究生, 主要研究方向为固体废物资源化处理, E-mail:zjc2011yly@163.com
通信作者: 张增强, E-mail:zhangzq58@126.com
摘要: 通过好氧堆肥和盆栽试验，探究不同比例（0%、2.5%、5%、7.5%和10%）钙基膨润土（CB）辅助猪粪堆肥过程及盆栽土壤中Cu、Zn形态的变化，并分析CB对白菜生物量及吸收Cu、Zn的影响.结果表明，在所有处理的堆肥过程中，可交换态Cu、Zn的分布比例逐渐下降，而可氧化态和残渣态逐渐升高，与0% CB相比，2.5%~10% CB可使堆肥结束时生物可利用态（可交换态和可还原态）Cu、Zn的分布比例分别降低19.84%~48.90%和4.94%~16.39%，并以10% CB的效果最为显著.进而开展的盆栽试验显示，施用堆肥后，土壤有机质和EC显著升高，而pH有所下降；CB辅助堆肥能够促使土壤EC的降低及pH的升高，稳定土壤有机质.与纯土处理相比，施用堆肥可显著提升白菜的生物量，且10% CB处理中的生物量最大（6.51 g·盆-1±0.34 g·盆-1）.施用CB辅助堆肥后，种后土壤中生物可利用态Cu含量增加；但各处理中可交换态Zn含量分别降低38.91%、43.69%、46.02%、45.12%和54.65%.白菜在施用堆肥后Cu、Zn的吸收量显著降低，并且随着CB辅助比例的增加Zn的吸收量随之减少，而Cu的吸收量呈增加趋势.本研究表明，钙基膨润土能够降低堆肥过程中Cu、Zn活性，在堆肥施入土壤后仍对Zn有持续的固定作用，同时CB辅助堆肥可以提高白菜的生物量，减少重金属Zn在白菜中的累积，并以10% CB的效果最为显著.
关键词: 钙基膨润土      堆肥      土壤      铜      锌      形态     
Effect of Ca-bentonite on Cu and Zn Forms in Compost and Soil, and Their Absorption by Chinese Cabbage
ZHAO Jun-chao , WANG Quan , REN Xiu-na , LI Rong-hua , Mukesh Kumar Awasthi , Altaf Hussain Lahori , ZHANG Zeng-qiang     
College of Natural Resources and Environment, Northwest A & F University, Yangling 712100, China
Abstract: Aerobic composting was conducted to evaluate the effects of the different ratios (0%, 2.5%, 5%, 7.5%, and 10%) of Ca-bentonite (CB) on the speciation of Cu and Zn during pig manure composting, while pot experiment was performed to investigate the role of CB-added compost on the bio-availability of Cu and Zn to Chinese cabbage and its biomass. The results showed that the exchangeable fractions of Cu and Zn decreased, while their oxidized and residual fractions gradually increased during composting; CB addition reduced the distribution ratios of bio-available Cu and Zn in mature compost by approximately 19.84%-48.90% and 4.94%-16.39%, compared to those in the 0% CB-added treatment, and the best result was found in the 10% CB-added treatment.. Meanwhile, the pot experiment confirmed that the addition of compost considerably increased soil organic matter (OM) and electrical conductivity (EC) but decreased soil pH value. On the contrary, the application of CB effectively decreased EC and increased soil pH but inhibited OM mineralization in soil as compared to non-amended treatment. While addition of compost significantly increased plant dry biomass as compared to that with soil alone, maximum biomass was obtained[(6.51±0.34) g·pot-1] in 10% CB-added compost. After the application of CB-added compost, the contents of the bio-available factions of Cu in the harvested soil increased, while the contents of the exchangeable fractions of Zn decreased by 38.91%, 43.69%, 46.02%, 45.12%, and 54.65%, respectively. The absorption of Cu and Zn by Chinese cabbage was considerably reduced after the application of compost, while the uptake of Zn in the plant declined as the CB rates increased, and the absorption of Cu increased. The study indicated that 10% CB addition could significantly reduce the bioavailability of Cu and Zn in compost, and also showed a continuous effect on restricting the bioavailability of Zn after land utilization. Meanwhile CB amendment enhanced Chinese cabbage biomass and reduced the uptake of Zn.
Key words: Ca-bentonite      composting      soil      copper      zinc      forms     

随着我国集约化养殖业的快速发展, 每年都会产生大量的猪粪.猪粪的养分含量较高, 是一种良好的潜在肥源[1].然而, 在养殖过程中饲料添加剂的过度使用, 导致猪粪中重金属含量普遍较高, 尤其以Cu、Zn含量最为显著[2].猪粪的直接农田施用不仅会危害作物的生长, 也有造成环境污染的风险[3].因此猪粪农用之前一般需经过堆肥处理, 促使其转化为稳定、安全、无害的有机肥料[4].然而传统的堆肥工艺存在重金属钝化效率不高及产品品质低下等问题, 限制了堆肥产业的发展和有机固体废物的快速消纳[5, 6].为了改进这些缺点, 现代堆肥工艺立足于高效高品质有机肥的生产, 注重堆肥过程和施用风险的控制.其中, 在堆肥过程中引入廉价易得的矿物添加剂就是现代堆肥工艺中的一种有效工程措施[7~9].例如, Wang等[6]指出麦饭石辅助猪粪堆肥对Cu、Zn的钝化作用显著, 添加比例为10%时能使堆肥过程中NH3和N2O的排放量分别减少48.76%和85.26%. Li等[1]发现添加钠基膨润土能有效降低猪粪堆肥中重金属(Cu、Zn)活性, 促进有机质的矿化分解, 且添加比例不宜超过2.5%. Chen等[10]的研究表明添加生物炭可以提高堆肥过程中重金属(Cu、Zn、Cd、Cr)的钝化效率, 缩短堆体升温时间.

综上所述, 加入一定比例的矿物添加剂可以有效钝化重金属, 改善堆肥进程[11].然而, 堆肥作为有机肥料, 土壤是其最终的归宿.猪粪堆肥中Cu、Zn总量仍然较高, 长期施用容易导致农田Cu、Zn污染, 加重作物中重金属元素的累积[12, 13].同时重金属的生物有效性与其化学形态密切相关[14~16], 在土壤中重金属形态易受到pH、氧化还原电位、有机质和阳离子交换量等因素的变化而重新分布[17].添加矿物质能够有效钝化堆肥中的重金属, 而在土壤施用矿物添加剂辅助堆肥后, 其对土壤中Cu、Zn生物有效性及作物吸收Cu、Zn的影响, 目前尚不明确.由此可知, 深入探究矿物添加剂对堆肥过程及土地利用中重金属形态变化的影响, 对促进畜禽粪便堆肥的安全农用具有重要意义.

钙基膨润土在我国矿产丰富, 价廉易得, 有着良好的吸附和离子交换能力[2].前期研究[2, 18]表明添加钙基膨润土能有效降低堆肥初期氮素损失, 促进有机质的降解及腐熟度的提升.在此基础上, 本研究以钙基膨润土为堆肥辅助剂, 结合盆栽试验来探究钙基膨润土对堆肥过程以及土壤施用堆肥后Cu、Zn形态分布的影响, 同时评价其在改善作物吸收重金属方面的应用潜力, 以期能探明钙基膨润土固定堆肥重金属的实际功效, 同时为矿物添加剂辅助堆肥工艺的应用推广提供理论依据.

1 材料与方法 1.1 堆肥试验

本研究供试材料为杨凌规模化养殖场的新鲜猪粪, 调理剂木屑出自杨凌周边家具厂, 钙基膨润土购置于山东潍坊华潍有限公司.堆肥原料基本理化性质见表 1, 堆制方法详见文献[2].试验中, 将猪粪和木屑按干基2:1比例混合, 然后添加干基质量0%、2.5%、5%、7.5%和10%的钙基膨润土, 共设置5个处理, 分别记为0% CB、2.5% CB、5% CB、7.5% CB和10% CB, 调节含水率60%左右, 混匀后转移入自制半自动搅拌式好氧堆肥反应器[1]进行为期60 d好氧堆肥, 于1、3、7、14、21、30、45和60 d采集样品.堆肥结束后, 自然风干腐熟堆肥, 开展盆栽试验.

表 1 堆肥原料基本理化性质 Table 1 Physicochemical properties of composting materials

1.2 盆栽试验

盆栽土取自西北农林科技大学试验站农田表层土, 土壤类型为黄褐土：pH 8.04、电导率0.40 mS·cm-1、有机质1.04%、Cu 20.61 mg·kg-1、Zn 64.52 mg·kg-1.土壤和堆肥粉碎过2 mm筛.盆栽装置为上口直径28 cm、下口直径16 cm、高18 cm的塑料盆, 填装总质量为3 kg, 肥土比为2.5% (湿基质量), 每个处理3个重复, 加去离子水至田间持水量的70%, 放置两周使各组分稳定化.供试植物为常见蔬菜白菜, 每盆均匀播种20粒, 放置于西北农林科技大学温室大棚, 待植株萌发4个叶片后进行间苗, 均匀保留5株幼苗, 40 d后收获白菜地上部分.

1.3 测定方法

堆肥和白菜采用HNO3-HClO4消解, 土样采用HNO3-HCl-HClO4消解, 日立Z-3000型原子吸收分光光度计测定Cu、Zn总量; 重金属形态采用改进BCR连续提取法测定[19], 操作要点见表 2; 白菜收获后经过杀青、烘干至恒重后记录干重; pH和电导率EC采用电极法测定(水土质量比5:1)[18]; 有机质及原材料总凯氏氮和总磷测定方法见文献[20].

表 2 改进BCR连续提取法操作要点 Table 2 Scheme of modified BCR sequential extraction

重金属形态分级为可交换态(X-EXC)、可还原态(X-RED)、可氧化态(X-OXI)、残渣态(X-RES), X代表Cu、Zn.因为堆肥过程中重金属含量变化较大, 为了更好地进行比较, 堆肥样品采用各形态占总量的质量分数进行表示.试验中土壤和堆肥重金属总量测定采用标准物质GBW08502, 植物样品用GBW10014分别进行分析质量控制.堆肥和土壤重金属形态分析试验回收率为91.86%~105.28%.

1.4 数据处理

采用Origin 8.5软件进行图表绘图, SPSS 19.0进行数据显著性检验以及相关性分析.

2 结果与讨论 2.1 堆肥过程中Cu、Zn总量的变化

堆肥过程中各处理Cu、Zn总量变化如图 1所示, 随着CB辅助比例的增加, 各处理初始物料中重金属含量逐渐降低, 这是由于CB中Cu、Zn含量低于猪粪, 对堆体有一定的稀释作用[6, 14].随着堆肥的进行, 0%~10% CB的处理中Cu、Zn含量逐渐上升, 这是因为有机质的降解及水分散失会导致堆体浓缩[1].堆肥结束时各处理Cu、Zn总量的增幅分别为14.92%~35.41%、12.71%~25.73%, 与毛晖等[21]报道的Cu (28.8%~32.9%)和Zn (12.3%~17.3%)结果相似, 但与郭靖等[22]报道的鸡粪堆肥中Cu、Zn增幅分别为1.68%~4.71%和4.03%~11.46%的结果存在一定差异.这是由于堆肥中重金属总量变化受堆肥原料和外部条件(如堆肥方式、天数等)的影响较大[14, 21], 不同堆肥原料的有机质降解速率及CO2释放速率不同, 因而导致了不同研究结果之间Cu、Zn的相对浓缩效应有所差异[14].

图 1 堆肥过程中Cu、Zn总量变化 Fig. 1 Changes in the total contents of Cu and Zn during composting of pig manure

2.2 堆肥过程中Cu、Zn形态变化

与重金属总量相比, 重金属的化学形态能更精确的反映其在环境中的生物有效性[23], 并且可交换态和可还原态的生物活性较高, 常将其统称为生物可利用态(X-BF; X为Cu、Zn)[14, 15].堆肥过程中不同处理Cu形态变化如图 2所示.随着堆肥的进行, 各处理中Cu-EXC和Cu-RED质量分数逐渐降低, 而Cu-OXI逐渐升高, Cu-RES略有增加.堆肥结束后, Cu形态分布以可氧化态为主, 占其总量的61.85%~73.56%, 与Meng等[16]的研究结果相印证.这是由于随着堆肥的进行, 大量增加的腐殖质会通过羧基及酚基等有机官能团对Cu(Ⅱ)产生较强的络合能力, 促使Cu-EXC和Cu-RED向Cu-OXI转化[24].堆肥结束后与对照相比, 2.5%~10% CB可使Cu-BF的分布比例降低19.84%~48.90%, 促进Cu的化学形态向生物有效性低的方向转化, 并且10% CB处理效果最显著.

图 2 添加钙基膨润土堆肥过程中Cu形态变化 Fig. 2 Changes in the Cu fractions during composting of pig manure amended with Ca-bentonite

堆肥过程中Zn的各形态分布与Cu有所不同(图 3).随着堆肥的进行, 各处理中Zn-EXC逐渐降低, Zn-RED逐渐升高, Zn-OXI和Zn-RES略有增加, 这与侯月卿等[25]的研究结果具有一定的相似性.堆肥结束后, Zn以可还原态为主, (占60.85%~69.24%), 而此时Cu主要以可氧化态存在.造成这一差异的原因可能是由于Zn与腐殖物质的结合能力弱于Cu, 而与铁锰氧化物的结合能力较强, 在堆肥过程中有利于Zn-RED的转化[26].堆肥结束后与0% CB相比, 2.5% CB、5% CB、7.5% CB和10% CB处理中Zn-BF分布比例分别下降了8.25%、4.94%、12.28%和16.39%.结果与Cu类似, CB辅助有利于降低堆肥处理中Zn的生物有效性, 并以10% CB处理的效果最明显.其原因可能是多方面的：第一, CB的添加提高了堆体孔隙度, 微生物大量繁殖的同时使得腐殖物质含量增加, Cu的形态向较为稳定的可氧化态转化[14, 26], 生物有效性降低; 第二, CB本身为多孔矿物质, 具有较强的物理吸附和离子交换能力, 且其表面能形成呈电负性的水合氧化物薄膜, 有助于络合吸附重金属, 从而降低重金属的生物有效性[27]; 第三, CB呈碱性(pH 8.4), 对重金属有一定的钝化作用[28].

图 3 添加钙基膨润土堆肥过程中Zn形态变化 Fig. 3 Changes in the Zn fractions during composting of pig manure amended with Ca-bentonite

2.3 钙基膨润土堆肥对土壤pH、EC及有机质变化的影响

与纯土处理相比, 施加堆肥后土壤初始pH有所下降, 而CB辅助堆肥的处理中土壤pH随辅助比例的增加而升高[图 4(a)], 这主要是由于堆肥施用到土壤后有一定的缓冲作用[29].经过40 d的种植过程, 纯土及0%~10% CB处理中土壤pH分别增加了0.42、0.57、0.61、0.51、0.65和0.64, 究其原因可能是有机碳的矿化分解以及随之产生的OH-与土壤中K+、Ca+、Mg2+等进行了离子交换[30].

图 4 盆栽试验前后土壤pH、EC、有机质变化 Fig. 4 Changes in the pH, EC, and organic matter content in soil before and after pot experiment

EC代表土壤水溶性盐分含量, 对作物生长具有重要的作用.施加堆肥显著提高了(P < 0.05)土壤EC值[图 4(b)], 随着种植过程的进行, 纯土及0%~10% CB处理中EC的降幅为26.46%~37.28%, 这与蔡函臻等[20]的研究结果相印证, 可能由于水溶性盐分被植物吸收以及CB的吸附或共沉淀作用导致[18].

种植前后土壤有机质变化见图 4(c).施加堆肥后显著提高了土壤有机质含量, 其中CB辅助处理中有机质含量低于0% CB.盆栽试验结束后, 0%~10% CB处理中有机质含量分别下降了3.51%、3.22%、2.68%、2.71%和2.54%, 由此说明钙基膨润土能够稳定土壤中的有机质. Zhang等[31]通过盆栽试验研究表明, 土壤中微生物对调控有机碳的矿化分解作用显著, 而CB为微生物提供了大量的附着位点, 有利于土壤中微生物的生长繁殖, 因此CB可能通过影响土壤微生物活性间接地稳定土壤有机质.

2.4 盆栽种植前后土壤Cu、Zn形态变化

与纯土相比, 施入堆肥后土壤中不同形态Cu含量显著(P < 0.05)上升[图 5(a)], 各处理Cu的形态分布为Cu-RES>Cu-RED>Cu-OXI>Cu-EXC.经过40 d的盆栽试验, 土壤中Cu-EXC和Cu-RED含量增加, Cu-OXI和Cu-RES含量降低, Cu的生物有效性提高, 这与商和平等[32]的研究结果大致相同.盆栽土壤偏碱性[图 4(a)], 堆肥中的腐殖物质在土壤环境中进一步分解, 促使与有机质结合的Cu向Cu-EXC和Cu-RED方向转化[28].相比0% CB, 2.5%~10% CB处理中土壤Cu-BF含量分别增加了35.72%、23.02%、60.56%和64.36%, 表明CB随堆肥施入土壤后对Cu的生物有效性有一定促进作用, 且2.5%~10% CB处理中白菜的Cu吸收量高于对照, 与此结果相印证.

图 5 盆栽试验前后土壤Cu、Zn形态变化 Fig. 5 Changes in the Cu and Zn fractions in soil before and after pot experiment

盆栽种植前后土壤中Zn形态变化如图 5(b)所示.各处理土壤Zn的形态分布为Zn-RES>Zn-RED>Zn-EXC>Zn-OXI, 盆栽结束后, 0%~10% CB处理中仅Zn-RED含量上升.这是由于Fe、Mn氧化物对Zn具有较强的吸附作用, 同时土壤pH对重金属在土壤中的迁移性和生物有效性具有重要影响[33], pH的上升[图 4(a)]更能促进这一吸附效果[14].改进BCR法提取的4种化学形态中以可交换态的生物有效性最高, 各处理种后土壤中Zn-EXC含量分别降低了38.91%、43.69%、46.02%、45.12%和54.65%, 表明CB辅助堆肥施入土壤后对Zn活性仍有抑制作用, 并且2.5%~10% CB处理中白菜Zn含量显著(P < 0.05)低于0% CB处理[图 6(b)], 与此结果相印证.究其原因可能是CB比表面积巨大, 对重金属有较强的吸附和离子交换作用, 降低了土壤中Zn的生物有效性[2].

不同字母代表数据在 p<0.05下差异显著 图 6 白菜生物量及Cu、Zn吸收量 Fig. 6 Biomass and contents of Cu and Zn in Chinese cabbage

2.5 盆栽试验白菜的生物量及Cu、Zn吸收量

白菜生物量及Cu、Zn含量如图 6所示. 0%~10% CB处理中白菜生物量分别比纯土处理增加了57.06%、80.59%、75.29%、79.71%和91.47%, 施用堆肥显著提高白菜生物量.同时CB辅助堆肥的提升效果要优于对照, 有利于作物生长.

施用堆肥在白菜增产的同时降低了Cu、Zn吸收量, 降幅分别为30.25%~50.97%和21.28%~40.81%, 这是由于施入堆肥后带来的有机物质会吸附土壤中的重金属离子, 对植物的吸收有抑制作用[24]. CB辅助堆肥降低了白菜对Zn的吸收量, 与0% CB处理相比, 10% CB中Zn的吸收量降低了25.94%, 但在2.5%~10% CB处理中Cu的吸收量增加了12.85%~43.94%. CB辅助堆肥抑制了白菜对Zn的吸收, 而对Cu则作用相反, 同时在土地利用过程中对土壤中Zn的活性仍保持抑制作用, 但对Cu则有活化的可能.为了分析这一现象, 进一步对数据进行Pearson相关性分析(表 3).虽然影响土壤Cu、Zn形态变化及白菜吸收的原因是多方面的, 但就本试验而言, 白菜对Cu的吸收量与土壤中Cu-RED含量正相关, 而CB辅助堆肥恰好可以提高Cu-RED的含量, 由此导致白菜对Cu的吸收量增加.对于Zn而言, Zn-EXC、pH及OM均与白菜吸收量负相关, 也暗示了不同元素在土壤中与作物的吸收之间存在较大差异[2].

表 3 不同参数变化量与白菜吸收间的Pearson相关系数1) Table 3 Pearson's correlation coefficient between the changes in parameters and absorption by Chinese cabbage

3 结论

(1) 钙基膨润土辅助堆肥降低了堆肥过程中Cu、Zn的生物有效性, 相比对照, 2.5%~10% CB能使堆肥产品Cu、Zn的生物可利用态分别降低19.84%~48.90%和4.94%~16.39%, 其中10% CB效果最为显著.

(2) 土壤施用堆肥后, 钙基膨润土辅助堆肥能持续抑制土壤中Zn的生物有效性, 促使Cu的活性略有提高.

(3) 钙基膨润土辅助堆肥可以提高白菜生物量, 抑制白菜对Zn的吸收, 而对Cu则表现出一定的促进作用.

(4) 相比而言, 以10%的添加比例进行堆肥, 在降低堆肥土地利用中重金属的环境风险以及改善作物对重金属元素累积方面具有较好的应用潜力.

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