珠江三角洲森林和蔬菜地土壤一氧化氮排放
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摘要
氮氧化物(NO_x=NO+NO_2)在大气光化学烟雾、二次气溶胶和酸雨等重要大气环境与空气质量问题中扮演极其重要角色，在我国人口稠密、工业化程度高的珠江三角洲地区，光化学污染、细粒子污染、灰霾和酸雨正是区内面临的空气污染难题，准确分析NO_x的来源及其排放通量对控制区域大气污染、改善区域空气质量和深入了解氮的地球化学物质循环具有重要意义。迄今为止，除了对珠江三角洲地区石化燃料燃烧过程NO_x排放有过报道之外，对NO_x的其他来源知之甚少。
土壤是大气NO_x的一个重要来源，尤其对于农田耕作强度高、氮肥用量大和大气氮沉降高的地区，土壤源的贡献可能更大。为了初步评价珠江三角洲及广东省土壤NO排放强度，本研究中我们选择本地区典型森林(季风常绿阔叶林和马尾松林)和蔬菜地为对象，比较系统地研究了这两类生态系统土壤NO排放通量及其影响因素，以及土壤排放的NO的氮同位素特征。研究得到的主要结论如下：
1．对于阔叶林，雨季NO平均排放通量为14.9ng N m~(-2) s~(-1)，低于干季平均排放通量(23.8 ng N m~(-2) s~(-1))；对于松林，雨季NO平均排放通量为17.1 ng N m~(-2)s~(-1)，高于干季排放通量(7.9 ng N m~(-2) s~(-1))。两类森林的土壤湿度均与NO排放显著相关(P＜0.001)，土壤湿度变化能很好解释NO排放的季节动态，说明土壤湿度是本地森林土壤NO排放的主要控制因素。由三种不同方法估算出阔叶林全年NO排放为6.1—6.9 kg N ha~(-1) yr~(-1)，马尾松林则为4.0—4.4 kg N ha~(-1) yr~(-1)。
2．外加氮磷实验表明，在阔叶林，硝氮和铵氮处理均大大促进了NO排放，而在松林，铵氮处理对NO排放的促进作用明显高于硝氮。单独氮处理相比同时加氮和磷对NO排放的促进作用更强。我们认为在阔叶林硝化作用和反硝化作用均对NO排放有重要贡献，而对于松林硝化作用在NO排放中起主导作用。根据本研究结果我们推测氮沉降倍增后阔叶林土壤NO排放预计将增加12.2％—21.8％，马尾松林预计将增加12.0％—31.2％。
3．森林干季加水实验的结果表明阔叶林和马尾松林干季期间由Pulses排放的NO总量分别为29.4 mg N m~(-2)和22.2 mg N m~(-2)，分别占全年土壤NO排放总量的4.6％和5.3％。
4．对广州郊区一块典型耕作方式管理下的蔬菜地(种植有菜心)土壤NO排放进行了一个完整生长周期的研究，结果表明施氮肥后NO排放激剧增加，其他涉及到松土的农田管理措施也会引起NO排放增加。在整个生长期(49天)NO平均排放通量为47.5 ng N m~(-2) s~(-1)，基于这一排放通量推算全年NO排放总量约为10.1 kg N ha~(-1) yr~(-1)。施肥引起的NO排放因子为2.4％。根据蔬菜地面积和单位面积NO排放率推算广东省蔬菜地全年向大气排放的NO约为11.7 Gg N yr~(-1)，根据排放因子和土壤NO背景排放率推算广东省蔬菜地NO年排放量为13.3 GgN yr~(-1)。
5．选取南亚热带地区典型菜地土壤，分别施用尿素、碳酸氢铵和硝酸铵。结果表明尿素施用引起的NO排放最大，碳酸氢铵施用引起NH_3排放最大。尿素、碳酸氢铵和硝酸铵施肥引起的NO排放因子分别为2.6％、2.3％和2.2％，引起的NH3排放因子分别为10.9％、15.2％和3.1％。根据本研究结果估算广东省菜地土壤NO排放量约为12.9 Gg N yr~(-1)，如果考虑冠层的截留作用，NO排放量下降为10.2 Gg N yr~(-1)。
6．施尿素和碳酸氢铵后，菜地土壤排放的NO的δ~(15)N值约为-49‰(施肥后第2天)，然后逐渐升高，到施肥后第13天时，NO的δ~(15)N值分别为-28.0‰(尿素处理)和-19.8‰(碳酸氢铵处理)。土壤排放的NH_3的δ~(15)N值也逐渐升高，施尿素的土壤NH_3的δ~(15)N值由-42.69‰(day 1)增加到-17.1‰(day 7)，施碳酸氢铵的土壤NH_3的δ~(15)N值由-39.4‰(day 0)增加到-21.5‰(day 6)。施肥后土壤源NO的δ~(15)N值范围与石化燃料燃烧排放的NO的δ~(15)N值范围相互区分，而施肥后排放的NH_3的δ~(15)N值范围与其他来源的NH_3的δ~(15)N值范围重叠。
Nitrogen oxides (NO_x) play crucial roles in troposphereic photochemical smog, formation of secondary aerosols and acid rain. Ozone, fine particles and acid rain are the right air quality issues facing China's highly industrialized and densely populated Pearl River Delta (PRD). The understanding of NO_x sources and their fluxes is of top priority not only for the control of the regional air pollution and the improvement of the regional air quality, but also for the regional nitrogen biogeochemical cycling. However, the sources of NO_x in PRD have not been well documented except that from fossil fuel combustion.
Soils are an important source for atmospheric NO_x, especially for the China's agricultural lands experiencing extensive management, high nitrogen fertilizer application and high nitrogen deposition. In the present study, soil NO emissions from forests (a broadleaf forest and a pine forest) and vegetable fields were measured and their regulating factors were investigated; the nitrogen isotope signature of soil-derived NO was also characterized as well. The main results were as the following:
1. In the broadleaf forest, mean NO emission in wet season (14.9 ng N m~(-2) s~(-1)) was lower than in dry season (23.8 ng N m~(-2) s~(-1)). In the pine forest, however, mean NO emission in wet season (17.1 ng N m~(-2) s~(-1)) was higher than in dry season (7.9 ng N m~(-1) s~(-1)). Field measurements showed that soil water content was the dominant controlling factor determining the seasonal patterns of NO emissions in both forests. Annual NO emissions in the broadleaf forest and the pine forest were preliminarily estimated to be 6.1-6.9 and 4.0-4.3 kg N ha~(-1) yr~(-1), respectively, by using three upscaling methods.
2. In the broadleaf forest, both NO_3~- and NH_4~+ addition enhanced NO emissions greatly, but in the pine forest, NH_4~+ addition had much greater enhancement than NO_3~-to soil NO emissions. N addition alone caused more N loss as NO than simultaneous addition of N and P did in both forests. In the pine forest, nitrification was the prevailing process responsible for NO production, while in the broadleaf forest both nitrification and denitrification played important roles in soil NO production. NO emissions will likely increase by 12.8%-23.0% in the broadleaf forest and by 12.0%-33.1% in the pine forest after N deposition doubles in the future.
3. Based on the results of the water addition experiment in the dry season, we estimated that total NO emissions from pulses in the broadleaf forest and pine forest were 29.4 mg N m~(-2) and 22.2 mg N m~(-2), respectively, which accounted for 4.6% and 5.3% of the annual emission, respectively.
4. NO fluxes measured in a field of Flowering Chinese cabbage drastically increased after nitrogen fertilizer application, and other practices involving loosening the soil also enhanced NO emission. Mean NO emission flux was 47.5 ng N m~(-1) s~(-1) over a complete growth cycle. Annual NO emission from the vegetable field was about 10.1 kg N ha~(-1) yr~(-1). Fertilizer-induced NO emission factor was estimated to be 2.4%. Total NO emission from vegetable fields in Guangdong province was roughly estimated to be 11.7 Gg N yr~(-1) based on the vegetable field area and annual NO emission rate, and to be 13.3 Gg N yr~(-1) based on fertilizer-induced NO emission factor and background NO emission.
5. We measured NO and NH_3 emissions from a typical vegetable-land soil in south China following the applications of urea, ammonium nitrate and ammonium bicarbonate, respectively. Over a 72-day sampling period, averaged fertilizer-induced NO emission factors from urea, ammonium bicarbonate (ABC) and ammonium nitrate treated soils amounted to 2.6%, 2.3% and 2.2%, respectively. Averaged fertilizer-induced NH3 emission factors were 10.9%, 15.2% and 3.1%, respectively, over a 39-day sampling period. Annual above-soil NO emission from vegetable lands in Guangdong province was estimated to be 12.9 Gg N yr~(-1), but reduced to 10.2 Gg N yr~(-1) when the canopy reduction effect was considered.
6.δ~(15)N values of soil-derived NO after urea and ammonium bicarbonate application were about -49‰(day 2), but increased to -28‰(urea application) and -19.8‰(ammonium bicarbonate application), respectively, after 13 days of fertilization. The case was similar for NH_3.δ~(15)N values of NH_3 volatized from urea treated soil increased from -42.6‰(day 1) to -17.1‰(day 7), and those from the ABC treated soil increased from -39.4‰(day 0) to -21.5‰(day 6). Theδ~(15)N values of NO emitted by fertilized soil could be distinguished from those of NO emitted by fossil fuel combustion, but theδ~(15)N values of NH_3 volatilized from fertilized soil overlapped with those from other sources.
土壤是大气NO_x的一个重要来源，尤其对于农田耕作强度高、氮肥用量大和大气氮沉降高的地区，土壤源的贡献可能更大。为了初步评价珠江三角洲及广东省土壤NO排放强度，本研究中我们选择本地区典型森林(季风常绿阔叶林和马尾松林)和蔬菜地为对象，比较系统地研究了这两类生态系统土壤NO排放通量及其影响因素，以及土壤排放的NO的氮同位素特征。研究得到的主要结论如下：
1．对于阔叶林，雨季NO平均排放通量为14.9ng N m~(-2) s~(-1)，低于干季平均排放通量(23.8 ng N m~(-2) s~(-1))；对于松林，雨季NO平均排放通量为17.1 ng N m~(-2)s~(-1)，高于干季排放通量(7.9 ng N m~(-2) s~(-1))。两类森林的土壤湿度均与NO排放显著相关(P＜0.001)，土壤湿度变化能很好解释NO排放的季节动态，说明土壤湿度是本地森林土壤NO排放的主要控制因素。由三种不同方法估算出阔叶林全年NO排放为6.1—6.9 kg N ha~(-1) yr~(-1)，马尾松林则为4.0—4.4 kg N ha~(-1) yr~(-1)。
2．外加氮磷实验表明，在阔叶林，硝氮和铵氮处理均大大促进了NO排放，而在松林，铵氮处理对NO排放的促进作用明显高于硝氮。单独氮处理相比同时加氮和磷对NO排放的促进作用更强。我们认为在阔叶林硝化作用和反硝化作用均对NO排放有重要贡献，而对于松林硝化作用在NO排放中起主导作用。根据本研究结果我们推测氮沉降倍增后阔叶林土壤NO排放预计将增加12.2％—21.8％，马尾松林预计将增加12.0％—31.2％。
3．森林干季加水实验的结果表明阔叶林和马尾松林干季期间由Pulses排放的NO总量分别为29.4 mg N m~(-2)和22.2 mg N m~(-2)，分别占全年土壤NO排放总量的4.6％和5.3％。
4．对广州郊区一块典型耕作方式管理下的蔬菜地(种植有菜心)土壤NO排放进行了一个完整生长周期的研究，结果表明施氮肥后NO排放激剧增加，其他涉及到松土的农田管理措施也会引起NO排放增加。在整个生长期(49天)NO平均排放通量为47.5 ng N m~(-2) s~(-1)，基于这一排放通量推算全年NO排放总量约为10.1 kg N ha~(-1) yr~(-1)。施肥引起的NO排放因子为2.4％。根据蔬菜地面积和单位面积NO排放率推算广东省蔬菜地全年向大气排放的NO约为11.7 Gg N yr~(-1)，根据排放因子和土壤NO背景排放率推算广东省蔬菜地NO年排放量为13.3 GgN yr~(-1)。
5．选取南亚热带地区典型菜地土壤，分别施用尿素、碳酸氢铵和硝酸铵。结果表明尿素施用引起的NO排放最大，碳酸氢铵施用引起NH_3排放最大。尿素、碳酸氢铵和硝酸铵施肥引起的NO排放因子分别为2.6％、2.3％和2.2％，引起的NH3排放因子分别为10.9％、15.2％和3.1％。根据本研究结果估算广东省菜地土壤NO排放量约为12.9 Gg N yr~(-1)，如果考虑冠层的截留作用，NO排放量下降为10.2 Gg N yr~(-1)。
6．施尿素和碳酸氢铵后，菜地土壤排放的NO的δ~(15)N值约为-49‰(施肥后第2天)，然后逐渐升高，到施肥后第13天时，NO的δ~(15)N值分别为-28.0‰(尿素处理)和-19.8‰(碳酸氢铵处理)。土壤排放的NH_3的δ~(15)N值也逐渐升高，施尿素的土壤NH_3的δ~(15)N值由-42.69‰(day 1)增加到-17.1‰(day 7)，施碳酸氢铵的土壤NH_3的δ~(15)N值由-39.4‰(day 0)增加到-21.5‰(day 6)。施肥后土壤源NO的δ~(15)N值范围与石化燃料燃烧排放的NO的δ~(15)N值范围相互区分，而施肥后排放的NH_3的δ~(15)N值范围与其他来源的NH_3的δ~(15)N值范围重叠。
Nitrogen oxides (NO_x) play crucial roles in troposphereic photochemical smog, formation of secondary aerosols and acid rain. Ozone, fine particles and acid rain are the right air quality issues facing China's highly industrialized and densely populated Pearl River Delta (PRD). The understanding of NO_x sources and their fluxes is of top priority not only for the control of the regional air pollution and the improvement of the regional air quality, but also for the regional nitrogen biogeochemical cycling. However, the sources of NO_x in PRD have not been well documented except that from fossil fuel combustion.
Soils are an important source for atmospheric NO_x, especially for the China's agricultural lands experiencing extensive management, high nitrogen fertilizer application and high nitrogen deposition. In the present study, soil NO emissions from forests (a broadleaf forest and a pine forest) and vegetable fields were measured and their regulating factors were investigated; the nitrogen isotope signature of soil-derived NO was also characterized as well. The main results were as the following:
1. In the broadleaf forest, mean NO emission in wet season (14.9 ng N m~(-2) s~(-1)) was lower than in dry season (23.8 ng N m~(-2) s~(-1)). In the pine forest, however, mean NO emission in wet season (17.1 ng N m~(-2) s~(-1)) was higher than in dry season (7.9 ng N m~(-1) s~(-1)). Field measurements showed that soil water content was the dominant controlling factor determining the seasonal patterns of NO emissions in both forests. Annual NO emissions in the broadleaf forest and the pine forest were preliminarily estimated to be 6.1-6.9 and 4.0-4.3 kg N ha~(-1) yr~(-1), respectively, by using three upscaling methods.
2. In the broadleaf forest, both NO_3~- and NH_4~+ addition enhanced NO emissions greatly, but in the pine forest, NH_4~+ addition had much greater enhancement than NO_3~-to soil NO emissions. N addition alone caused more N loss as NO than simultaneous addition of N and P did in both forests. In the pine forest, nitrification was the prevailing process responsible for NO production, while in the broadleaf forest both nitrification and denitrification played important roles in soil NO production. NO emissions will likely increase by 12.8%-23.0% in the broadleaf forest and by 12.0%-33.1% in the pine forest after N deposition doubles in the future.
3. Based on the results of the water addition experiment in the dry season, we estimated that total NO emissions from pulses in the broadleaf forest and pine forest were 29.4 mg N m~(-2) and 22.2 mg N m~(-2), respectively, which accounted for 4.6% and 5.3% of the annual emission, respectively.
4. NO fluxes measured in a field of Flowering Chinese cabbage drastically increased after nitrogen fertilizer application, and other practices involving loosening the soil also enhanced NO emission. Mean NO emission flux was 47.5 ng N m~(-1) s~(-1) over a complete growth cycle. Annual NO emission from the vegetable field was about 10.1 kg N ha~(-1) yr~(-1). Fertilizer-induced NO emission factor was estimated to be 2.4%. Total NO emission from vegetable fields in Guangdong province was roughly estimated to be 11.7 Gg N yr~(-1) based on the vegetable field area and annual NO emission rate, and to be 13.3 Gg N yr~(-1) based on fertilizer-induced NO emission factor and background NO emission.
5. We measured NO and NH_3 emissions from a typical vegetable-land soil in south China following the applications of urea, ammonium nitrate and ammonium bicarbonate, respectively. Over a 72-day sampling period, averaged fertilizer-induced NO emission factors from urea, ammonium bicarbonate (ABC) and ammonium nitrate treated soils amounted to 2.6%, 2.3% and 2.2%, respectively. Averaged fertilizer-induced NH3 emission factors were 10.9%, 15.2% and 3.1%, respectively, over a 39-day sampling period. Annual above-soil NO emission from vegetable lands in Guangdong province was estimated to be 12.9 Gg N yr~(-1), but reduced to 10.2 Gg N yr~(-1) when the canopy reduction effect was considered.
6.δ~(15)N values of soil-derived NO after urea and ammonium bicarbonate application were about -49‰(day 2), but increased to -28‰(urea application) and -19.8‰(ammonium bicarbonate application), respectively, after 13 days of fertilization. The case was similar for NH_3.δ~(15)N values of NH_3 volatized from urea treated soil increased from -42.6‰(day 1) to -17.1‰(day 7), and those from the ABC treated soil increased from -39.4‰(day 0) to -21.5‰(day 6). Theδ~(15)N values of NO emitted by fertilized soil could be distinguished from those of NO emitted by fossil fuel combustion, but theδ~(15)N values of NH_3 volatilized from fertilized soil overlapped with those from other sources.
引文
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