有机电子供体影响下硝酸盐和铁对磷转化的驱动作用

doi:10.16258/j.cnki.1674-5906.2023.07.009

生态环境学报 ›› 2023, Vol. 32 ›› Issue (7): 1263-1274.DOI: 10.16258/j.cnki.1674-5906.2023.07.009

有机电子供体影响下硝酸盐和铁对磷转化的驱动作用

童永杰¹(), 汪毅¹, 华玉妹¹^,^*(), 赵建伟¹, 刘广龙¹, 蒋永参²

1.华中农业大学，湖北武汉 430070
2.中国电建集团勘测设计研究院有限公司，浙江杭州 311122

收稿日期:2023-06-16 出版日期:2023-07-18 发布日期:2023-09-27
通讯作者: * 华玉妹。E-mail: ymhua@mail.hzau.edu.cn
作者简介:童永杰（1999年生），男，硕士研究生，研究方向为水环境污染研究。E-mail: 1114797026@qq.com
基金资助:
国家自然科学基金项目(42177059)

Transformation of Phosphorus in Sediments Driven by Nitrate and Iron in the Presence of Organic Electron Donor

TONG Yongjie¹(), WANG Yi¹, HUA Yumei¹^,^*(), ZHAO Jianwei¹, LIU Guanglong¹, JIANG Yongcan²

1. Huazhong Agricultural University, Wuhan 430070, P. R. China
2. China Electric Power Construction Group Survey and Design Institute Co., Ltd., Hangzhou 311122, P. R. China

Received:2023-06-16 Online:2023-07-18 Published:2023-09-27

摘要/Abstract

摘要：

磷是湖泊的关键生源要素，其转化受多种生物化学反应的驱动。在富营养化后期，藻类在厌氧条件下衰败所产生的乙酸盐可作为反硝化过程的有机电子供体，铁可作为反硝化过程的电子供体和能量来源，它们会通过影响氮的转化而直接或间接对磷转化产生影响。本研究取武汉市墨水湖的样品构建了沉积物-上覆水体系，通过向上覆水中输入硝酸盐、铁和乙酸盐以探明有机电子供体（乙酸盐）影响下铁和氮对磷转化的驱动作用。在不同乙酸盐浓度下，研究上覆水和间隙水中氮、磷与铁质量浓度随时间的变化，确定沉积物中反硝化酶活性与硝酸盐型亚铁氧化菌（NDFOB）丰度，分析沉积物中的磷形态以明晰铁结合态磷的存在形式。结果表明，（1）乙酸盐增加了沉积物中NDFOB丰度和反硝化酶活性，使硝态氮（NO₃^--N）去除效率提高22.6%。（2）总磷（TP）浓度与总铁（TFe）浓度之间显著正相关（P=0.001），易还原铁氧化物（Fe_ox1）和可还原铁氧化物（Fe_ox2）是沉积物中对磷吸附能力最强的铁形态，占沉积物总铁质量的43.8%-54.1%。（3）乙酸盐促进了沉积物中Fe(Ⅲ) 的还原，由于沉积物中Fe_ox1和Fe_ox2还原作用而产生较高质量分数Fe(Ⅱ)，铁结合态磷质量分数明显降低。（4）最终沉积物中易还原铁结合态磷（P-Fe_ox1）质量分数比NO₃^-处理组低0.250 mg·g^-1，同时乙酸盐抑制沉积物中Fe_ox2生成过程，可还原铁结合态磷（P-Fe_ox2）质量分数比NO₃^-处理组低0.010 mg·g^-1，上覆水和间隙水总磷浓度显著高于NO₃^-处理组（P=0.000）。研究结果通过明确不同介导作用下沉积物磷与铁结合形式的转变，有助于加深对湖泊内源污染理论的认识。

关键词: 沉积物, 磷, 硝酸盐, 乙酸盐, 铁结合态磷

Abstract:

Phosphorus is a key biogenic element in lakes, and the transformation is driven by a variety of biochemistry reaction. At the late stage of eutrophication, the acetate produced via alga decaying under anaerobic condition can be used as an organic electron donor in the denitrification process, and iron can be used as an electron donor and energy source in the denitrification process. They can pose direct/indirect effect on the phosphorus transformation by affecting the nitrogen transformation. In this study, a sediment-overlying water system using samples from Lake Moshui of Wuhan was set up, where the driving effect of iron and nitrogen on the phosphorus transformation in the presence of organic electron donors (acetate) was investigated via inputting nitrate, iron and acetate into the overlying water. In the presence of different concentrations of acetate, the changes of nitrogen, phosphorus and iron content in the overlying water and interstitial water with time were firstly investigated, then the denitrification enzyme activity and the abundance of nitrate-dependent Fe(II) oxidation bacteria (NDFOB) in the sediment were determined. Furthermore, the form of phosphorus in sediments was explored to clarify the existence form of iron-bound phosphorus. The results showed: (1) The presence of acetate increased the NDFOB abundance and denitrification enzyme activity in the sediments, increasing the NO₃^--N removal efficiency by 22.6%. (2) There was a significant positive correlation between total phosphorus (TP) concentration and total iron concentration (P=0.001). Easily reducible oxides (Fe_ox1) and reducible oxides (Fe_ox2) were the iron forms with the strongest phosphorus adsorption capacity, accounting for 43.8%-54.1% of the total iron content in sediments. (3) The presence of acetate promoted the reduction of Fe(III) in the sediments. Due to the reduction of Fe_ox1 and Fe_ox2 in the sediments, a relatively high content of Fe(II) was produced, accompanied by a drastic decrease of iron-bound phosphorus content. (4) The content of easily reducible iron-bound phosphorus (P-Fe_ox1) in the final sediments was 0.250 mg·g^-1 lower than that in the NO₃^- treated group. Because the presence of acetate inhibited the formation of Fe_ox2 in the sediments, the content of reducible iron-bound phosphorus (P-Fe_ox2) was 0.010 mg·g^-1 lower than that in the NO₃^- treated group, while the total phosphorus concentrations in overlying water and pore water were significantly higher than those in the NO₃^- treated group (P=0.000). These findings contribute to deepen the understanding of the endogenous pollution theory in lakes by elucidating the transformation of phosphorus-iron binding forms in sediments under different mediation.

Key words: sediments, phosphorus, nitrate, acetate, iron bound phosphorus

中图分类号:

童永杰, 汪毅, 华玉妹, 赵建伟, 刘广龙, 蒋永参. 有机电子供体影响下硝酸盐和铁对磷转化的驱动作用[J]. 生态环境学报, 2023, 32(7): 1263-1274.

TONG Yongjie, WANG Yi, HUA Yumei, ZHAO Jianwei, LIU Guanglong, JIANG Yongcan. Transformation of Phosphorus in Sediments Driven by Nitrate and Iron in the Presence of Organic Electron Donor[J]. Ecology and Environment, 2023, 32(7): 1263-1274.

图/表 13

表1 沉积物铁结合磷同步分级提取过程

Table 1 The iron bound phosphorus simultaneous extraction process of sediments

步骤	提取	提取目标相
Ⅰ	10 mL 1 mol·L^-1Na₂CO₃; pH值4.5, 24 h	碳酸盐铁 (Fe_carb), 碳酸盐铁结合态磷 (P-Fe_carb)
Ⅱ	10 mL 1 mol·L^-1盐酸羟胺 (25%乙酸), 48 h	易还原铁氧化物 (Fe_ox1), 易还原铁氧化物铁结合态磷 (P-Fe_ox1)
Ⅲ	10 mL 50 g·L^-1连二亚硫酸钠 (0.35 mol·L^-1乙酸/0.2 mol·L^-1柠檬酸三钠) 2 h	可还原铁氧化物 (Fe_ox2), 可还原铁结合态磷 (P-Fe_ox2)
Ⅳ	10 mL 0.2 mol·L^-1草酸/0.17 mol·L^-1草酸铵 (pH值3.26 h)	磁铁矿 (Fe_mag), 磁铁矿结合态磷 (P-Fe_mag)
Ⅴ	5 mL 12 mol·L^-1盐酸, 煮沸1 min	片状硅酸盐铁 (Fe_prs), 片状硅酸盐铁结合态磷 (P-Fe_prs)

图1 上覆水（a、c）和间隙水（b、d）中pH和Eh的变化（样本量）n=3，下同

Figure 1 Change of pH and Eh in overlying water (a, c) and pore water (b, d)

图2 上覆水（a、c）和间隙水（b、d）中Fe(Ⅱ)和TFe质量浓度的变化

Figure 2 Change of Fe(Ⅱ) and TFe concentration in overlying water (a, c) and pore water (b, d)

图3 上覆水（a、b、c）和间隙水（d、e、f）NO3-、NO2-和NH4+质量浓度的变化

Figure 3 Change of NO3-, NO2- and NH4+ concentration in overlying water (a, b, c) and pore water (d, e, f)

图4 上覆水TN质量浓度（a）、间隙水TN质量浓度（b）和N2O释放通量（c）的变化

Figure 4 Change of TN concentration in overlying water (a) and pore water (b) and N2O releasing flux(c)

图5 沉积物反硝化酶活性

Figure 5 Change of sediment denitrifying enzyme activity

图6 沉积物中NDFOB数量随时间的变化

Figure 6 Change in the amount of NDFOB in the sediment with time

图7 上覆水和间隙水中TP（a、b）和SRP（c、d）质量浓度的变化

Figure 7 Change of TP and SRP concentration in overlying water (a, b) and pore water (c, d)

图8 上覆水（a）和间隙水（b）可酶解磷质量浓度的变化

Figure 8 Change of enzymatically hydrolysable phosphorus concentration in overlying water (a) and pore water (b)

图9 上覆水（a）和间隙水（b）碱性磷酸酶质量浓度的变化

Figure 9 Change of hydrolysable phosphorus in overlying water and pore water

表2 沉积物TP质量分数的变化

Table 2 Change in sediment TP concentrations mg·g-1

t/d	N组TP质量分数	N-A组TP质量分数
0	2.27±0.03	2.26±0.01
0.5	2.19±0.03	2.13±0.02
1	2.21±0.03	2.14±0.02
2	2.20±0.06	1.99±0.20
6	2.07±0.23	2.02±0.07
10	2.12±0.06	2.01±0.01
15	2.12±0.07	2.00±0.01

图10 沉积物磷形态分级提取

Figure 10 Sequential extraction of phosphorus forms in sediments

图11 沉积物铁与铁结合磷同步分级提取 P-Femag图的缺失是由于其质量分数低于检测限

Figure 11 Synchronous fractional extraction of iron and iron-bound phosphorus insediments

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有机电子供体影响下硝酸盐和铁对磷转化的驱动作用

Transformation of Phosphorus in Sediments Driven by Nitrate and Iron in the Presence of Organic Electron Donor

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